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CN1648041A - Method and device for preparing super pure silicon from metal silicon - Google Patents

Method and device for preparing super pure silicon from metal silicon Download PDF

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CN1648041A
CN1648041A CN 200410003090 CN200410003090A CN1648041A CN 1648041 A CN1648041 A CN 1648041A CN 200410003090 CN200410003090 CN 200410003090 CN 200410003090 A CN200410003090 A CN 200410003090A CN 1648041 A CN1648041 A CN 1648041A
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silicon
boiler tube
hyperpure
impurity
preparation
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吴尔盛
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Abstract

The present invention is method and apparatus of preparing metal silicon into super pure silicon and the preparation includes three steps of crushing material, impurity compounding and crystallizing purification. Specially, the preparation includes crushing metal silicon into fine grains with increased surface area; introducing oxygen, hydrochloric acid and chlorine to react with impurity in material to produce oxide or chloride; heating to eliminate chloride and intermediate or directional solidification to eliminate other impurity. The present invention eliminates impurities from silicon material and purifies the metal silicon into pure silicon product.

Description

The method and apparatus for preparing hyperpure silicon from Pure Silicon Metal
Technical field
The invention belongs to Pure Silicon Metal refining techniques in the smelting of metallurgical industry light metal, relate to a kind of preparation method and device of hyperpure silicon, especially relating to a kind of is raw material with the Pure Silicon Metal, prepares the production technology of hyperpure silicon by a series of operation operations of removing impurity.
Background technology
The people of silicon industry pay attention to the purity of silicon very much, the same with other high purity substances, usually the purity class of representing silicon with 9 individual numerical value, the silicon of 49 (being called for short 4N) purity is HIGH-PURITY SILICON, the silicon of 69 (being called for short 6N) purity is hyperpure silicon, and the silicon of 99 (being called for short 9N) above purity is the superelevation pure silicon.
The silicone content purity of Pure Silicon Metal is 98--99%, with the silicon oxide is that raw material adopts carbon and hot reducing method to produce in large quantities, the silicon metal purity that this method is made is low, can not directly use, but its turnout is very big, can be supplied to downstream manufacturers as the purify processing operation of impurity elimination series operation of raw material, to produce the silicon product that satisfies particular professional purposes comfortably.
The silicon of the above purity of 9N mainly is to be that the Pure Silicon Metal alkanisation is learned vapor phase process and is called for short the CVD method and produces with well-known Siemens Method.This superelevation pure silicon manufacturing cost height is mainly used in semiconductor manufacturing industry, if through adjusting operation, add the purposes of some element as solar cell silicon, making in this way can be because production cost higher, so that the user can not accept, is unfavorable for that penetration and promotion uses.
The silicon of 9N and following purity mostly is raw material with the Pure Silicon Metal, makes by the method for removing impurity to raw material.Some remove the method for impurity, be the continuity of metallurgical operation in fact, and be in the operation of refining stage, its main method is: earlier the Pure Silicon Metal heating and melting is become melt, add reactant gas when being blown into heat with high-temperature plasma stream again, making impurity in the Pure Silicon Metal become gas evaporation goes out, last using directed solidification technology is further removed impurity, the technology of using serial operation such as above-mentioned grade was arranged in the past, Pure Silicon Metal is removed the patent of invention achievement that impurity is purified to silicon for solar cell openly issue.
Along with the sectionalization that the silicon product is made, the market demand potential of high purity silicon is huge, for example is used as processing semiconductor, processing solar cell, processing high frequency electrical equipment, processes the raw material or the auxiliary agent of purposes such as the high purity material refining is added, production organosilicon.Silicon solar cell particularly, the utilization of sun power has reached the 13--15% efficiency of conversion, so, can the production cost of silicon for solar cell decline to a great extent is to be related to the crux that can silicon solar cell be popularized, because clear along with the exhausted trend of energy growing tension, necessaryly seek multiple energy resource supply to nature energetically.In addition, along with the continuous expansion in many retainings time high purity silicon market, silicon purified technical study trend is with manufacturing process's sectionalization more, becomes more meticulous more so, more inexpensiveization, and this also is the bright and clear direction of technical study.
For example, a kind of method introduced in patent of invention number 96198989.0 " manufacturing method and apparatus of polysilicon " literary composition, this method container of earlier Pure Silicon Metal being packed into, with plasma arc the Pure Silicon Metal heating and melting in the container to 1450-1900 ℃, in the underpressure chamber with 10 -3-10 -5Kept 30-60 minute under the holder vacuum tightness, phosphorus in the sila matter and aluminium gasification finish, this melt is molded into first mold, the control melt is the direction cooled and solidified from top to bottom, impurity element is concentrated in the top of ingot bar, with partly excision of the ingot bar top of the impurity element that concentrates about 30%.Residue is partly changed in the smelting furnace with plasma arc, melt to again more than 1450 ℃, be blown into water vapor H 2O, carbonic acid gas CO 2Deng oxidizing gas, boron in the melt and oxidation of coal are removed, the mixed gas that is blown into argon or argon and hydrogen then is to remove the oxygen in the melt, melt after refining pours in second mold that scribbles releasing agent, repeat above-mentioned directional solidification technique and obtain ingot bar, ingot bar is concentrated after 20% excision on top of impurity element, all the other are partly as the polysilicon goods again.But from the ingot bar Chemical Composition analytical data of this technology, its some impurity elements are by after making the solar cell silicon substrate, just reach specified requirement through the contained impurity element of substrate being carried out subsequent processes again.
Aforesaid method has the following disadvantages:
1, use the plasma arc that utilizes rate variance of heat to carry out the melting solid Pure Silicon Metal, thus uneconomical;
2, plasma jet and oxidizing gas are blown into from the melt top, and evaporation causes damage and operating environment is bad to cause silicon to splash;
3, utilize rare amount of inert gas such as argon gas big, make manufacturing cost higher.
And for example, a kind of method introduced in patent of invention number 98105942.2 " removing the method and apparatus of boron from Pure Silicon Metal " literary composition, this method is the Pure Silicon Metal container that silicon oxide makes of packing into, with non-transfer type plasma body, the transfer type plasma body, combination between the heating unit such as high-frequency induction and resistance, Pure Silicon Metal is melted to more than 1550 ℃, above melt, use hollow plasma torch made of copper, spray into plasma jet at a certain angle, the mixed gas of water vapor and hydrogen or carbon monoxide or paraffinic hydrocarbons, wherein water vapor accounts for the 10-40% volume of above-mentioned three class mixed gas total amounts, and hydrogen accounts for the 5-90% of above-mentioned three class mixed gas total amounts.Also be blown into the mixed gas of water vapor and the combination of rare rare gas element from the bottom porous plug.This technology is for to carry out powerful stirring action to molten silicon, adopts by rotatingfield or induction stirring or by being blown into gas and conventional liquation paddling process such as stirs.This technology thinks that the operation ratio that is blown into mixed gas from the liquation bottom is easier to, and can successfully remove the boron operation.This technology judges that than resistance value the concentration of boron reaches the operation terminal point of silicon for solar cell prescribed value as this method to measure ingot bar, and this on-line analysis operation fast saves time.
This method also has the following disadvantages:
1, it is big to make the amount of plasma fluid with argon, the rare inert gas of helium, and cost is higher;
2, plasma jet and reducing gas are blown into melt liquid level from the melt top, and silicon splashes and causes damage;
3, the heat energy utilization rate is low, and energy consumption is bigger than normal.
Summary of the invention
The object of the present invention is to provide a kind of is raw material with the Pure Silicon Metal, by serial operation combination operation, produces the preparation method and the device of hyperpure silicon a large amount of, inexpensively.
The present invention with chemistry, metallurgical method, has carried out deep research in the hope of obtaining maximum economical effectiveness, thereby has finished the present invention in order to achieve the above object.
The invention provides a kind of preparation method and device of hyperpure silicon, utilize Pure Silicon Metal to prepare hyperpure silicon by following three steps:
The I step is broken for fine particle to Pure Silicon Metal, and the impurity in the silicon increases surface-area because of broken, is beneficial to carry out chemical reaction;
The II step, aerating oxygen or feed chlorine or add hydrochloric acid or aerating oxygen and adding hydrochloric acid or feed a kind of in chlorine and these five kinds of modes of adding hydrochloric acid in silicon grain, make impurity generate oxide compound or muriate, because oxide compound has the eutectoid point lower than silicon fusing point, muriate has the sublimation temperature that is lower than the silicon fusing point;
The III step is implemented crystallization purifying to silicon melt, and solidification technology or directional freeze are coagulated a kind of in these two kinds of modes of technology in the middle of adopting, and utilize characteristics such as segregation and eutectoid point, and the impurity in the silicon is removed from silicon.
That is to say that above-mentioned three steps in the present invention are a sequential steps, are an integral body, are a kind of technical schemes.Each technical scheme in the present invention all is made up of above-mentioned three steps conversely speaking.Also have, because the I step in the sequential steps is a basic steps, the II step can realize this step by any mode in its 5 kinds of modes, and the III step can realize this step by any mode in its 2 kinds of modes, so just can form the multiple technologies scheme.In addition, above-mentioned three steps can also sequentially circulate again and again, and certainly, circulation each time realizes that all the impurity in the silicon reduces significantly, realizes that the purity of silicon increases substantially.
According to above-mentioned three step technique principles, can form following multiple technologies scheme.
A kind of preparation method of hyperpure silicon prepares hyperpure silicon by following operation by Pure Silicon Metal:
A. Pure Silicon Metal is pulverized and be fine particle;
B. silicon grain is packed into the crucible internal heating of high frequency furnace, aerating oxygen makes the impurity in the silicon be oxidized to oxide compound;
C. silicon grain is packed in the glassed steel reaction vessels, add hydrochloric acid and heating, make impurity reaction the becoming muriate in the silicon.Leach reaction solution, feed nitrogen silicon grain moisture content is dried up;
D. silicon grain is packed into the crucible internal heating of high frequency induction furnace feeds chlorine in certain temperature range, make the impurity in the silicon further generate muriate, stops to make the silicon fusion until higher temperature behind the logical chlorine;
E. silicon melt is poured into and to be placed with releasing agent in advance, have in the bucket-shaped mold of senior insulation efficiency, cool off lentamente with in the middle of realizing and solidify, reach impurity is got rid of periphery between crucible inwall and content silicon, after cooling and demolding and the cleaning, acquisition ingot bar goods.
F. silicon melt or silicon grain are packed in the horizontal multi-stage type tube furnace, unlatching hangs on and is nested in the boiler tube outer radial periphery below the rail, the radio-frequency induction coil that can move along the boiler tube axial direction due, end in beginning moves towards axial the other end direction, can catch up with the impurity in the melted silicon to the boiler tube termination, after one short boiler tube of the impurity that concentrates and content silicon taken off, reinstall the end axle.Radio-frequency induction coil is transferred to an end of beginning, repeats aforesaid operations and become to catching up with impurity, remove the boiler tube segment of the impurity that concentrates again.
Based on aforesaid method, the present invention also provides the preparation method of other hyperpure silicon, carries out entering B operation, C operation, D operation and E operation or F operation again after the A operation.
In addition, carry out entering C operation, D operation and E operation or F operation again after the A operation.
In addition, carry out entering B operation, C operation and E operation or F operation again after the A operation.
In addition, carry out entering B operation and E operation or F operation again after the A operation.
In addition, carry out entering C operation and E operation or F operation again after the A operation.
In addition, carry out entering D operation and E operation or F operation again after the A operation.
The Pure Silicon Metal pulverizing is 5 millimeter for fine grain particle diameter in the above A operation.
Above-mentioned, the logical oxygen temperature of B operation is by normal temperature to 650 ℃, and 650 ℃ of constant temperature 1 hour;
Above-mentioned, the used hydrochloric acid of C operation is concentrated hydrochloric acid, and the carrying out along with reaction adds water gradually towards rare, to be fit to various impurity and the required dense and rare requirement of hydrochloric acid reaction in the silicon.
Above-mentioned, the temperature of the logical chlorine of D operation is by normal temperature to 260 ℃, and the logical chlorine time is 1 hour; The melt temperature of D operation silicon be 1900 ℃ and more than.
Above-mentioned, the melt temperature of F operation silicon be 1600 ℃ and more than.
Above-mentioned, the releasing agent in the bucket-shaped mold of E operation is the pulvis of 120 order left and right sides fineness of ferric oxide 35-45%, calcium oxide 25-35% and silicon-dioxide 20-30% weight composition.
Simultaneously, the present invention also provide realize above-mentioned preparation method preparation facilities, require to be configured according to concrete operation, comprise: be used for A operation crusher; Be used for B operation, the heating of D operation and molten silicon particulate high frequency furnace; The glassed steel reaction vessels that is used for the C operation; The bucket-shaped mold and the insulation adiabatic system that are used for the E operation; Be used for the horizontal multi-stage type boiler tube of F operation and in radial outer periphery, be used to the system that heats and walk towards axially movable radio-frequency induction coil etc.; Be used to hold the crucible and the multi-stage type tube furnace boiler tube of heating and molten silicon.
The horizontal multi-stage type boiler tube of the F operation of above-mentioned hyperpure silicon preparation facilities, it is characterized in that, the multi-stage type boiler tube is that many sections straight lengths are formed, connect with flange between pipeline section, two terminations of whole boiler tube respectively are equipped with the short bend pipe of import and export of bolster and melt silicon or silicon grain, and this axis of importing and exporting short bend pipe is parallel with the boiler tube axis.One end linking number of boiler tube cuts the pipeline section that accounts for boiler tube total length 5-20% length.
The B operation of above-mentioned hyperpure silicon preparation facilities, the heating of D operation and molten silicon particulate high frequency furnace, it is characterized in that, the inlet pipe of above-mentioned gas is equipped with in the bottom of high frequency furnace crucible, the onesize crucible that gas exhaust duct is housed of back-off above this crucible, vacuum fan after also having the waste gas absorption tower of pipe coupling therewith and being contained in tower.
The horizontal multi-stage type boiler tube of the F operation of above-mentioned hyperpure silicon preparation facilities and in radial outer periphery towards axially movable radio-frequency induction coil, is characterized in that, radio-frequency induction coil is for being nested in multi-stage type boiler tube external diameter periphery, and can move along the boiler tube axial direction due; Radio-frequency induction coil hangs on the rail below, and rail is same plane and parallel with the axial of multi-stage type boiler tube axially; Radio-frequency induction coil drives with the stepper-motor that is installed on the rail.
The bucket-shaped mold of the E operation of above-mentioned hyperpure silicon preparation facilities is characterized in that, mold is bucket-shaped, does the heat-insulating material insulation with the zirconium white hollow ball around its six.Multi-stage type boiler tube pipe is outward also with this lagging material insulation.
Above-mentioned hyperpure silicon preparation facilities.It is characterized in that, be used to heat with the crucible of molten silicon, bucket-shaped mold and multi-stage type tube furnace furnace tube material and be all graphite, but all serve as a contrast the silicon-dioxide lining at their inwall, and in multi-stage type tube furnace outer wall coated with silicon dioxide coating.
For describing better, so the positively effect of implementing technical solution of the present invention is described with the mode of following table.
Item compared Prior art The technical program
Subsidiary material Gases such as rare argon gas, helium Common materials such as oxygen, hydrochloric acid, nitrogen, chlorine
The electric heating utilization ratio Below 70% More than 90%
Installation cost Investment is big Investment descends 50%
Production cost The production cost height Production cost descends 30%
The product situation Silicon suitable for solar purposes Purity silicon goods such as 4N, 6N, 9N
Operating environment The big dust of noise is big Only noise and dust are arranged at broken process
Unit scale Easily maximize Easily maximize
Simple declaration to subordinate list:
Table 1, table 2 are materialization data of the part metal chloride in the Pure Silicon Metal impurity.
Table 3 is the part non-metallic element in the Pure Silicon Metal impurity and the materialization data of oxide compound thereof.
Embodiment
In force Pure Silicon Metal be crushed to particle diameter 5 millimeter, be in order more effectively to remove the impurity in the silicon.In the past in the fused melted silicon, plasma fluid and reactant gas with rare rare gas element are jetted on melt liquid level, and be blown into the reactant gas of rare rare gas element and oxidisability or reductibility from melt bottom, because silicon melt viscosity extra-high-speed, surface tension is especially big, and this melt is an external phase, gas then is disperse phase, so that gas contacts with melt with the form of bubble, and the useful area all too is little, so effect is very limited.After being broken for fine particle, its surface-area greatly increases, and at this moment gas and liquid all are external phase, and the silicon grain solid is a disperse phase, adds that silicon face is easily soaked into by water, hydrochloric acid, oxygen and chlorine, and their active area is the increase of quantitative series like this.So the present invention goes into to think that the operation combination that Pure Silicon Metal is removed impurity earlier in the fine particle mode comes conveniently, easier, rationally.
In addition, to the impurity in the metallic silicon particle, carry out oxidation with oxygen, also be in order more effectively to remove the impurity in the silicon, because the exhausted major part of the impurity in the Pure Silicon Metal exists with metal or with non-metallic element, silicon grain aerating oxygen temperature of reaction height to 650 ℃ in set, be enough to that the nitrogen in the silicon, oxygen (oxygen in oxidation two silicon and four silicon oxide), carbon, sulphur are oxidized to gas evaporation and go out (seeing attached list 3), what particularly point out is that silicon can be not oxidized at this temperature and time, on the contrary can also be removing in conjunction with oxygen in the silicon.Also have the silicon grain of gathering to be more conducive to the volatilization of gas than melted silicon.Boron, phosphorus oxidation are become oxide compound soluble in water, remove simultaneously kind of impurity surplus other ten all is oxidized to oxide compound, and most of oxide compounds, particularly metal oxide has eutectoid point between them, this eutectic point is approximately between 1100-1200 ℃, be lower than the fusing point of 1414 ℃ of Pure Silicon Metals, this has just opened convenience greatly for the application of directional solidification technique, has opened up good precondition.Also have a lot of metal oxides than its element simple substance easier with hydrochloric acid effect (see attached list 1 and table 2).The oxide compound that impurity element arranged again is individual bigger than impurity element molecule, the melted silicon cooled and solidified be not easy to be mixed in the silicon crystal, also be more conducive to the crystallization purifying of silicon.
In addition, in device of the present invention, utilize the silicon melt cooled and solidified to have middle characteristic of solidifying, use the reason of this characteristic, the observation post that puts into practice from the contriver gets; Removing its volume because of the silicon melt cooled and solidified increases about 10%, also because of the silicon melt cooled and solidified is middle coagulating type, and when the silicon water bag when their actings in conjunction are produced Pure Silicon Metal cools off, the silicon face generation type of silicon bag such as curvature of the spinal column shape.Utilize this characteristic just, six faces to the square type mold among the present invention adopt resistant to elevated temperatures senior heat-insulating material, cooled and solidified speed with the control melted silicon makes it less than impurity rate travel in the silicon, and this speed comprises oxide compound and utmost point individual element segregation rate travel.What also particularly point out is, individual metals such as titanium, chromium its difficult and hydrochloric acid and chlorine reaction, but its segregation coefficient is all very little, easily removes in the application of directional solidification technique.
Also have, in the device of the present invention, behind the silicon grain of packing in the high frequency furnace crucible, feed the chlorine operation lentamente in crucible bottom, be because chlorine can react about 300 ℃ with silicon, thus feed chlorine be make it with silicon in the temperature of impurity reaction, be strict controlled in 260 ℃ and following.And below minute-pressure power, carry out all the time in this subsystem, strict containment measures is arranged, promptly residue chlorine and waste gas are led to absorption and filtration in the packing tower that fritter unslaked lime or slaked lime are housed by pipeline, so that realize the zero release of pollutent fully.
Have again, in the device of the present invention, in horizontal multi-stage type tube furnace, the application of directional solidification technique has effect very easily, its radio-frequency induction coil is embedded in outside the boiler tube caliber, can move along the axial direction due of boiler tube, when powering up and moving this radio-frequency induction coil, at high temperature the impurity in the molten silicon moves and make orientation towards the direction that coil moves, thereby the impurity in the silicon is concentrated in the termination of many short tubes boiler tube because of the segregation effect that itself has and the characteristic of eutectoid point in the boiler tube, take off the silicon and the short boiler tube of the impurity that concentrates behind the powered-down, reinstall the end axle of boiler tube, mobile radio-frequency induction coil powers up the repetition aforesaid operations to an end that begins.Take off the silicon of a brachymemma boiler tube and within it the impurity that concentrates at each bout, the interior silicon melt of boiler tube obtains purifying once like this, and purifying so repeatedly finally obtains the silicon of enough purity.Here it may be noted that, short tube length in the multistage pipe is different, during first leg, high its amount of impurity concentration is big, and short tube length always is about 20% length at boiler tube, during second leg, impurity concentration descends, the short boiler tube length of 10%, the three bout that corresponding short boiler tube length accounts for length overall accounts for 5% of length overall, takes off short tube once until bout repeatedly.Also need point out, the multi-stage type tube furnace will remain on operation under the negative pressure all the time, to avoid at high temperature silicon and oxygen oxidizing reaction as much as possible, so the import and export Guan Zeyi after multi-stage type tube furnace boiler tube is packed silicon grain into is connected with waste gas absorption tower, utilize the gravitation of the vacuum fan behind the absorption tower to realize.Can avoid silicon oxidized like this, also can take the waste gas that is evaporated in the boiler tube away, and send into the waste gas absorption tower emission abatement.If also have the boiler tube total length to reach several meters, two radio-frequency induction coils then can be set, one in front and one in back spaced apart, this distance is when cooling off 1350 ℃ of left and right sides with silicon, to heat in order to energy-conservation with the second road coil again.
Preferred forms: at first with the fine particle of Pure Silicon Metal with crusher in crushing to 5 millimeter, pack into the crucible internal heating of high frequency furnace of whole silicon grains, aerating oxygen rises to 650 ℃ by room temperature, and 650 ℃ of constant temperature 1 hour, the oxidation of impurities in the grain silicon is become oxide compound.The glassed steel reaction vessels of packing into through the silicon grain of above-mentioned oxidation, add concentrated hydrochloric acid, be heated to 120-150 ℃ after 1 hour by room temperature, add the amount of clear water gradually to the hydrochloric acid volume, reacted 1 hour, reacted liquid is emitted in filter, with nitrogen silicon grain moisture content is dried up again.In the crucible of the high frequency furnace of packing into through peracid treatment and exsiccant silicon grain, buckle the left-hand thread crucible that is connected to vapor pipe, connect the pipeline that is connected with waste gas absorption tower, ℃ add chlorine lentamente by room temperature to 260, reacted 1 hour, and behind the logical chlorine of disconnection silicon grain was melted to more than 1900 ℃.Melted silicon is poured into the bucket-shaped mold that is placed as releasing agent in advance, middle characteristic of solidifying when utilizing the melted silicon cooling, cooled and solidified becomes ingot bar especially lentamente; Or last melted silicon poured in the horizontal multi-stage type tube furnace, its fill-up is about 80%, enable radio-frequency induction coil and be heated to 1600 ℃, and move from the other end of an end lentamente to how little pipeline section with the translational speed about average 5 mm/min, behind the termination, the silicon of the impurity that concentrates is taken off together with this short boiler tube section, reinstall boiler tube end axle, an end that moves on to beginning again repeats above-mentioned operation.As required, can repeatedly repeat above-mentioned operation, end until meeting the requirements.Then purified melted silicon like this is poured in the bucket-shaped mold that is placed as releasing agent in advance, carry out cooled and solidified especially lentamente, become the ingot bar goods after the cooling.
The preparation method of a kind of hyperpure silicon of having described above, also can select the another kind of method that only prepares the hyperpure silicon scheme according to qualifications from above-mentioned the preparation with metallurgical refining techniques, Pure Silicon Metal is crushed to 5 millimeter, in the crucible of the high frequency furnace of packing into through whole silicon grains of fragmentation, from the crucible bottom aerating oxygen, Heating temperature is raised to 650 ℃ from room temperature, and 650 ℃ of constant temperature 1 hour; And then in the silicon grain of oxidation is packed horizontal multi-stage type tube furnace into, loadings is 90% of a boiler tube total volume, after the unlatching radio-frequency induction coil is heated to the silicon fusion and rises to 1600 ℃, from an end of boiler tube to the other end that is connected with many brachymemmas boiler tube, move radio-frequency induction coil with the speed about average 5 mm/min, impurity in the melted silicon is become to arriving in the termination, the silicon of the impurity that concentrates is taken off together with short boiler tube section, reinstall the pipe end axle, radio-frequency induction coil is moved on to an end of beginning, repeat repeatedly aforesaid operations to index up to specification, pour into the bucket-shaped mold that is placed as releasing agent in advance, through slow especially cooled and solidified, the demoulding becomes hyperpure silicon ingot bar goods.
Embodiment 1: the plumbago crucible internal heating that the silicon-dioxide lining is arranged through the high frequency furnace of 10 kilograms of 100KVA that pack into of silicon grain that is crushed to 5 millimeters sizes, in room temperature to 650 ℃ temperature range, aerating oxygen, and under 650 ℃ of temperature constant temperature 1 hour.The glassed steel reaction vessels of packing into after the cooling adds concentrated hydrochloric acid, be heated to 120 ℃ by room temperature after, constant temperature is 1 hour again, adds the amount of clear water to the hydrochloric acid content volume gradually, reacts elimination reaction solution, and go into nitrogen from the still bottom blowing moisture content of silicon grain is dried up again 1 hour.Silicon grain is packed in the crucible of above-mentioned high frequency furnace, under room temperature to 260 ℃ temperature, feed chlorine lentamente, the whole logical chlorine time closed chlorine and continues to heat up a silicon fusion up to reaching 1900 ℃ in 1 hour.Silicon melt is poured in the bucket-shaped mold plumbago crucible that senior insulation efficiency is arranged of the good preheating of process that is placed with releasing agent in advance, cool off lentamente with in the middle of realizing and solidify, reach impurity get rid of the crucible inwall with than the periphery between pure silicon with conveniently stripped, demoulding cleaning back acquisition goods ingot bar.This ingot bar is crushed to Pure Silicon Metal product grain size, this silicon grain is packed in the high frequency furnace crucible, power-on melts to 1900 ℃ to silicon, pours in the bucket-shaped mold that is placed with releasing agent in advance, and cooling and demolding obtains ingot bar.Repeat so more once, get 6.9 kilograms of ingot bars after the demoulding, purity is 9N.
Embodiment 2: the plumbago crucible internal heating that the silicon-dioxide lining is arranged through the high frequency furnace of 10 kilograms of 100KVA that pack into of silicon grain that is crushed to 5 millimeters sizes, in room temperature to 650 ℃ temperature range, aerating oxygen, and under 650 ℃ of temperature constant temperature 1 hour.The glassed steel reaction vessels of packing into after the cooling adds concentrated hydrochloric acid, be heated to 120 ℃ by room temperature after, constant temperature is 1 hour again, adds the amount of clear water to the hydrochloric acid content volume gradually, reacts elimination reaction solution, and go into nitrogen from the still bottom blowing moisture content of silicon grain is dried up again 1 hour.Silicon grain is packed in the crucible of above-mentioned high frequency furnace, under room temperature to 260 ℃ temperature, feed chlorine lentamente, the whole logical chlorine time closed chlorine and continues to heat up a silicon fusion up to reaching more than 1900 ℃ in 1 hour.It is 100 millimeters that silicon melt is poured into caliber, length is 1.5 meters, be lined with in the carbon tube in the boiler tube of multi-stage type tube furnace of silicon-dioxide, its loading level is 80%, the radio-frequency induction coil heating of startup 100KVA is also mobile lentamente with the speed of 5 mm/min to the other end of the short boiler tube of multistage by an end of boiler tube, deenergization behind the termination, radio-frequency induction coil is moved on to an end of beginning, take off the short tube that the termination accounts for boiler tube length overall 20% length and the silicon of the impurity that concentrates within it, reinstall the pipe end axle.End in beginning is opened the direction of radio-frequency induction coil along the axial end of boiler tube heavily again, speed with 5 mm/min moves, deenergization behind the termination, again radio-frequency induction coil is moved on to an end of beginning, take off the short boiler tube that the termination accounts for boiler tube length overall 10% length and the silicon of the impurity that concentrates within it, reinstall the end axle.End in beginning is opened the direction of radio-frequency induction coil along the axial end of boiler tube once more, moves with the speed of 5 mm/min, and deenergization behind the termination takes off the silicon that short boiler tube that the termination accounts for boiler tube length overall 5% length reaches the impurity that concentrates within it.Reinstall the end axle that has downstream end, the starting end of boiler tube is raise, make it to form the tilt angled down of 35 degree, open extreme direction heating and slow move of radio-frequency induction coil to beginning, up to the silicon melt in the boiler tube all being poured in the bucket-shaped mold that is placed with releasing agent in advance, cooled and solidified especially lentamente in bucket-shaped mold becomes 6.9 kilograms in hyperpure silicon goods after the demoulding.Through the analysis to ingot bar, the purity of its silicon reaches 9N.
Embodiment 3: packing into into glassed steel reaction vessels for 10 kilograms through the silicon grain that is crushed to 5 millimeters sizes, add concentrated hydrochloric acid, after being heated to 120 ℃ by room temperature, constant temperature is 1 hour again, add the amount of clear water gradually to the hydrochloric acid content volume, reacted again 1 hour, the elimination reaction solution, and go into nitrogen from the still bottom blowing moisture content of silicon grain is dried up.Silicon grain is packed in the crucible of above-mentioned high frequency furnace, under room temperature to 260 ℃ temperature, feed chlorine lentamente, the whole logical chlorine time closed chlorine and continues to heat up a silicon fusion up to reaching 1900 ℃ in 1 hour.Silicon melt poured into be placed with releasing agent in advance, through in the bucket-shaped mold plumbago crucible that senior insulation efficiency is arranged of good preheating, cool off lentamente with in the middle of realizing and solidify, reach impurity get rid of the crucible inwall with than the periphery between pure silicon with conveniently stripped, demoulding cleaning back acquisition goods ingot bar.This ingot bar is crushed to Pure Silicon Metal product grain size, this silicon grain is packed in the high frequency furnace crucible, power-on melts to 1900 ℃ to silicon, pours in the bucket-shaped mold that is placed with releasing agent in advance, and cooling and demolding obtains ingot bar.Repeat so more once, get 7.1 kilograms of ingot bars after the demoulding, purity is 8N.
Embodiment 4: packing into into glassed steel reaction vessels for 10 kilograms through the silicon grain that is crushed to 5 millimeters sizes, add concentrated hydrochloric acid, after being heated to 120 ℃ by room temperature, constant temperature is 1 hour again, add the amount of clear water gradually to the hydrochloric acid content volume, reacted again 1 hour, the elimination reaction solution, and go into nitrogen from the still bottom blowing moisture content of silicon grain is dried up.Silicon grain is packed in the crucible of above-mentioned high frequency furnace, under room temperature to 260 ℃ temperature, feed chlorine lentamente, the whole logical chlorine time closed chlorine and continues to heat up a silicon fusion up to reaching 1900 ℃ in 1 hour.It is 100 millimeters that silicon melt is poured into caliber, length is 1.5 meters, be lined with in the carbon tube in the boiler tube of multi-stage type tube furnace of silicon-dioxide, its loading level is 80%, the radio-frequency induction coil heating of startup 100KVA is also mobile lentamente with the speed of 5 mm/min to the other end of the short boiler tube of multistage by an end of boiler tube, deenergization behind the termination, radio-frequency induction coil is moved on to an end of beginning, take off the short tube that the termination accounts for boiler tube length overall 20% length and the silicon of the impurity that concentrates within it, reinstall the pipe end axle.End in beginning is opened the direction of radio-frequency induction coil along the axial end of boiler tube heavily again, speed with 5 mm/min moves, deenergization behind the termination, again radio-frequency induction coil is moved on to an end of beginning, take off the short tube that the termination accounts for boiler tube length overall 10% length and the silicon of the impurity that concentrates within it, reinstall the end axle.End in beginning is opened the direction of radio-frequency induction coil along the axial end of boiler tube once more, moves with the speed of 5 mm/min, and deenergization behind the termination takes off the silicon that short boiler tube that the termination accounts for boiler tube length overall 5% length reaches the impurity that concentrates within it.Reinstall the end axle that has downstream end, beginning one end of boiler tube is raise, make it to form the tilt angled down of 35 degree, open extreme direction heating and slow move of radio-frequency induction coil to beginning, up to the silicon melt in the boiler tube all being poured in the bucket-shaped mold that is placed with releasing agent in advance, cooled and solidified especially lentamente in bucket-shaped mold becomes 7.1 kilograms in hyperpure silicon goods after the demoulding.Through the analysis to ingot bar, the purity of its silicon reaches 8N.
Embodiment 5: the plumbago crucible internal heating that the silicon-dioxide lining is arranged through the high frequency furnace of 10 kilograms of 100KVA that pack into of silicon grain that is crushed to 5 millimeters sizes, in room temperature to 650 ℃ temperature range, aerating oxygen, and under 650 ℃ of temperature constant temperature 1 hour.The glassed steel reaction vessels of packing into after the cooling adds concentrated hydrochloric acid, be heated to 120 ℃ by room temperature after, constant temperature is 1 hour again, adds the amount of clear water to the hydrochloric acid content volume gradually, reacts elimination reaction solution, and go into nitrogen from the still bottom blowing moisture content of silicon grain is dried up again 1 hour.Silicon grain is packed in the crucible of above-mentioned high frequency furnace, power-on a silicon fusion up to reaching 1900 ℃.Silicon melt poured into be placed with releasing agent in advance, through in the bucket-shaped mold plumbago crucible that senior insulation efficiency is arranged of good preheating, cool off lentamente with in the middle of realizing and solidify, reach impurity get rid of the crucible inwall with than the periphery between pure silicon with conveniently stripped, demoulding cleaning back acquisition goods ingot bar.This ingot bar is crushed to Pure Silicon Metal product grain size, this silicon grain is packed in the high frequency furnace crucible, power-on melts to 1900 ℃ to silicon, pours in the bucket-shaped mold that is placed with releasing agent in advance, and cooling and demolding obtains ingot bar.Repeat so more once, get 7.1 kilograms of ingot bars after the demoulding, purity is 8N.
Embodiment 6: the plumbago crucible internal heating that the silicon-dioxide lining is arranged through the high frequency furnace of 10 kilograms of 100KVA that pack into of silicon grain that is crushed to 5 millimeters sizes, in room temperature to 650 ℃ temperature range, aerating oxygen, and under 650 ℃ of temperature constant temperature 1 hour.The glassed steel reaction vessels of packing into after the cooling adds concentrated hydrochloric acid, be heated to 120 ℃ by room temperature after, constant temperature is 1 hour again, adds the amount of clear water to the hydrochloric acid content volume gradually, reacts elimination reaction solution, and go into nitrogen from the still bottom blowing moisture content of silicon grain is dried up again 1 hour.Is the silicon grain caliber of packing into 100 millimeters, length is 1.5 meters, be lined with in the carbon tube in the boiler tube of multi-stage type tube furnace of silicon-dioxide, its loading level is 80%, the radio-frequency induction coil heating of startup 100KVA is also mobile lentamente with the speed of 5 mm/min to the other end of the short boiler tube of multistage by an end of boiler tube, deenergization behind the termination, radio-frequency induction coil is moved on to an end of beginning, take off the short tube that the termination accounts for boiler tube length overall 20% length and the silicon of the impurity that concentrates within it, reinstall the pipe end axle.End in beginning is opened the direction of radio-frequency induction coil along the axial end of boiler tube heavily again, speed with 5 mm/min moves, deenergization behind the termination, again radio-frequency induction coil is moved on to an end of beginning, take off the short tube that the termination accounts for boiler tube length overall 10% length and the silicon of the impurity that concentrates within it, reinstall the end axle.End in beginning is opened the direction of radio-frequency induction coil along the axial end of boiler tube once more, moves with the speed of 5 mm/min, and deenergization behind the termination takes off the silicon that short boiler tube that the termination accounts for boiler tube length overall 5% length reaches the impurity that concentrates within it.Reinstall the end axle that has downstream end, the starting end of boiler tube is raise, make it to form the tilt angled down of 35 degree, open extreme direction heating and slow move of radio-frequency induction coil to beginning, up to the silicon melt in the boiler tube all being poured in the bucket-shaped mold that is placed with releasing agent in advance, cooled and solidified especially lentamente in bucket-shaped mold becomes 7.1 kilograms in hyperpure silicon goods after the demoulding.Through the analysis to ingot bar, the purity of its silicon reaches 8N.
Embodiment 7: the crucible internal heating that the high frequency furnace that passes through the 10 kilograms of 100KVA that pack into of silicon grain that are crushed to 5 millimeters sizes is had the silicon-dioxide lining, in room temperature to 650 ℃ temperature range, aerating oxygen, and 650 ℃ of constant temperature 1 hour, pack into after the cooling silicon grain packed in the crucible of above-mentioned high frequency furnace, power-on a silicon fusion up to reaching 1900 ℃.Silicon melt is poured in the bucket-shaped mold plumbago crucible that senior insulation efficiency is arranged of the good preheating of process that is placed as releasing agent in advance, cool off lentamente with in the middle of realizing and solidify, reach impurity get rid of the crucible inwall with than the periphery between pure silicon with conveniently stripped, demoulding cleaning back acquisition goods ingot bar.This ingot bar is crushed to Pure Silicon Metal product grain size, this silicon grain is packed in the high frequency furnace crucible, power-on melts to 1900 ℃ to silicon, pours in the bucket-shaped mold that is placed with releasing agent in advance, and cooling and demolding obtains ingot bar.Repeat so more once, get 7.2 kilograms of ingot bars after the demoulding, purity is 8N.
Embodiment 8: the crucible internal heating that the high frequency furnace that passes through the 10 kilograms of 100KVA that pack into of silicon grain that are crushed to 5 millimeters sizes is had the silicon-dioxide lining, in room temperature to 650 ℃ temperature range, aerating oxygen, and 650 ℃ of constant temperature 1 hour, packing into the silicon grain caliber of packing into after the cooling is 100 millimeters, length is 1.5 meters, be lined with in the carbon tube in the boiler tube of multi-stage type tube furnace of silicon-dioxide, its loading level is 80%, the radio-frequency induction coil heating of startup 100KVA is also mobile lentamente with the speed of 5 mm/min to the other end of the short boiler tube of multistage by an end of boiler tube, deenergization behind the termination, radio-frequency induction coil is moved on to an end of beginning, take off the short tube that the termination accounts for boiler tube length overall 20% length and the silicon of the impurity that concentrates within it, reinstall the pipe end axle.End in beginning is opened the direction of radio-frequency induction coil along the axial end of boiler tube heavily again, speed with 5 mm/min moves, deenergization behind the termination, again radio-frequency induction coil is moved on to an end of beginning, take off the short tube that the termination accounts for boiler tube length overall 10% length and the silicon of the impurity that concentrates within it, reinstall the end axle.End in beginning is opened the direction of radio-frequency induction coil along the axial end of boiler tube once more, moves with the speed of 5 mm/min, and deenergization behind the termination takes off the silicon that short boiler tube that the termination accounts for boiler tube length overall 5% length reaches the impurity that concentrates within it.Reinstall the end axle that has downstream end, the starting end of boiler tube is raise, make it to form the tilt angled down of 35 degree, open extreme direction heating and slow move of radio-frequency induction coil to beginning, up to the silicon melt in the boiler tube all being poured in the bucket-shaped mold that is placed with releasing agent in advance, cooled and solidified especially lentamente in bucket-shaped mold becomes 7.1 kilograms in hyperpure silicon goods after the demoulding.Through the analysis to ingot bar, the purity of its silicon reaches 8N.
Embodiment 9: packing into into glassed steel reaction vessels for 10 kilograms through the silicon grain that is crushed to 5 millimeters sizes, add concentrated hydrochloric acid, after being heated to 120 ℃ by room temperature, constant temperature is 1 hour again, add the amount of clear water gradually to the hydrochloric acid content volume, reacted again 1 hour, the elimination reaction solution, and go into nitrogen from the still bottom blowing moisture content of silicon grain is dried up.Silicon grain is packed in the crucible of above-mentioned high frequency furnace, heat up a silicon fusion up to reaching 1900 ℃.Silicon melt poured into is placed with releasing agent in advance, through in the bucket-shaped mold plumbago crucible that senior insulation efficiency is arranged of good preheating, cool off lentamente with in the middle of realizing and solidify, reach impurity get rid of the crucible inwall with than the periphery between pure silicon with conveniently stripped, demoulding cleaning back acquisition goods ingot bar.This ingot bar is crushed to Pure Silicon Metal product grain size, this silicon grain is packed in the high frequency furnace crucible, power-on melts to 1900 ℃ to silicon.Silicon melt poured into be placed with releasing agent in advance, through in the bucket-shaped mold plumbago crucible that senior insulation efficiency is arranged of good preheating, cool off lentamente with in the middle of realizing and solidify, reach impurity get rid of the crucible inwall with than the periphery between pure silicon with conveniently stripped, demoulding cleaning back acquisition goods ingot bar.Repeat so more once, get 7.2 kilograms of ingot bars after the demoulding, silicon purity is 6N.
Embodiment 10: packing into into glassed steel reaction vessels for 10 kilograms through the silicon grain that is crushed to 5 millimeters sizes, add concentrated hydrochloric acid, after being heated to 120 ℃ by room temperature, constant temperature is 1 hour again, add the amount of clear water gradually to the hydrochloric acid content volume, reacted again 1 hour, the elimination reaction solution, and go into nitrogen from the still bottom blowing moisture content of silicon grain is dried up.Is the silicon grain caliber of packing into 100 millimeters, length is 1.5 meters, be lined with in the carbon tube in the boiler tube of multi-stage type tube furnace of silicon-dioxide, its loading level is 80%, the radio-frequency induction coil heating of startup 100KVA is also mobile lentamente with the speed of 5 mm/min to the other end of the short boiler tube of multistage by an end of boiler tube, deenergization behind the termination, radio-frequency induction coil is moved on to an end of beginning, take off the short tube that the termination accounts for boiler tube length overall 20% length and the silicon of the impurity that concentrates within it, reinstall the pipe end axle.End in beginning is opened the direction of radio-frequency induction coil along the axial end of boiler tube heavily again, speed with 5 mm/min moves, deenergization behind the termination, again radio-frequency induction coil is moved on to an end of beginning, take off the short tube that the termination accounts for boiler tube length overall 10% length and the silicon of the impurity that concentrates within it, reinstall the end axle.End in beginning is opened the direction of radio-frequency induction coil along the axial end of boiler tube once more, moves with the speed of 5 mm/min, and deenergization behind the termination takes off the silicon that short boiler tube that the termination accounts for boiler tube length overall 5% length reaches the impurity that concentrates within it.Reinstall the end axle that has downstream end, the starting end of boiler tube is raise, make it to form the tilt angled down of 35 degree, open extreme direction heating and slow move of radio-frequency induction coil to beginning, up to the silicon melt in the boiler tube all being poured in the bucket-shaped mold that is placed with releasing agent in advance, cooled and solidified especially lentamente in bucket-shaped mold becomes 7.2 kilograms in hyperpure silicon goods after the demoulding.Through the analysis to ingot bar, the purity of its silicon reaches 6N.
Embodiment 11: the crucible internal heating that the high frequency furnace that passes through the 10 kilograms of 100KVA that pack into of silicon grain that are crushed to 5 millimeters sizes is had the silicon-dioxide lining, under room temperature to 260 ℃ temperature, feed chlorine lentamente, the whole logical chlorine time closed chlorine and continues to heat up a silicon fusion up to reaching 1900 ℃ in 1 hour.Silicon melt poured into be placed with releasing agent in advance, through in the bucket-shaped mold plumbago crucible that senior insulation efficiency is arranged of good preheating, cool off lentamente with in the middle of realizing and solidify, reach impurity get rid of the crucible inwall with than the periphery between pure silicon with conveniently stripped, demoulding cleaning back acquisition goods ingot bar.This ingot bar is crushed to Pure Silicon Metal product grain size; this silicon grain is packed in the high frequency furnace crucible; power-on melts to 1900 ℃ to silicon; pour in the bucket-shaped mold that is placed with releasing agent in advance; cooling and demolding obtains ingot bar; repeat so more once, get 7.2 kilograms of ingot bars after the demoulding, purity is 6N.
Embodiment 12: the crucible internal heating that the high frequency furnace that passes through the 10 kilograms of 100KVA that pack into of silicon grain that are crushed to 5 millimeters sizes is had the silicon-dioxide lining, under room temperature to 260 ℃ temperature, feed chlorine lentamente, the whole logical chlorine time is in 1 hour, closing the caliber of packing into after chlorine cools off is 100 millimeters, length is 1.5 meters, tubing is that the multi-stage type tube furnace inwall of graphite is lined with in the boiler tube of silicon-dioxide, the radio-frequency induction coil heating of unlatching 100KVA is also mobile lentamente with the speed of 5 mm/min to the other end of the short boiler tube of multistage by an end of boiler tube, deenergization behind the termination, radio-frequency induction coil is moved on to an end of beginning, take off the short tube that the termination accounts for boiler tube length overall 20% length and the silicon of the impurity that concentrates within it, reinstall the pipe end axle.End in beginning is opened the direction of radio-frequency induction coil along the axial end of boiler tube heavily again, speed with 5 mm/min moves, deenergization behind the termination, again radio-frequency induction coil is moved on to an end of beginning, take off the short tube that the termination accounts for boiler tube length overall 10% length and the silicon of the impurity that concentrates within it, reinstall the end axle.End in beginning is opened the direction of radio-frequency induction coil along the axial end of boiler tube once more, moves with the speed of 5 mm/min, and deenergization behind the termination takes off the silicon that short boiler tube that the termination accounts for boiler tube length overall 5% length reaches the impurity that concentrates within it.Reinstall the end axle that has downstream end, the starting end of boiler tube is raise, make it to form the tilt angled down of 35 degree, open extreme direction heating and slow move of radio-frequency induction coil to beginning, until the silicon melt in the boiler tube all being poured in the bucket-shaped mold that is placed with releasing agent in advance, cooled and solidified especially lentamente in bucket-shaped mold becomes 7.1 kilograms in hyperpure silicon goods after the demoulding.Through the analysis to ingot bar, the purity of its silicon reaches 6N.
Table 1
The materialization data of part metal chloride
The muriate title Fusing point (℃) Boiling point (℃) The heat of sublimation (or heat of gasification) (kilocalorie/mol) Vapour pressure and other The generation method
CaCl 2And 2 hydrate 772 More than 1600 0.018 Bristol, 661.4 ℃, 54 928K, 12.17mm mercury column 1026K, 59.98mm mercury column " " the P514 calcium oxide salt acid system under the handbook of P545 calcium metal salt acid system under the handbook
MnCl 2And 4 hydrate 650 58 1,193 106 1atm, 1146.3 ℃, 28.8 (heat of gasification) The decomposition of heating anhydride discharges HCl, Mn in the air 3O 4778-1190 ℃, the 10-760mm mercury column. " reagent " P85 manganese metal salt acid system " P798 manganese oxide salt acid system on the handbook
FeCl 3 309 319 315 ℃, 11300 (heat of gasification) 3310 Decompose the boiling point lower section, facile hydrolysis.194--310 ℃, the 1-760mm mercury column. " P424 metallic iron salt acid system ferric oxide salt acid system on the handbook
AlCl 3And 6 hydrate 186--190 (2atm) 182 (755.4mm mercury column) 1atm, 180.6 ℃ of distillations, 26.7 Reveal and to put in the air, easily absorb moisture content and hydrogenchloride is emitted in hydrolysis.100--180.2 ℃, the 1--760mm mercury column. " P379 metallic aluminium salt acid system aluminum oxide salt acid system on the handbook
ZnCl 2 313 732 1atm, 1029K, 30.9 (heat of gasification) 428--732 ℃, 1--760mm mercury column, facile hydrolysis. " P462 metallic zinc salt acid system zinc oxide salt acid system on the handbook
CoCl 2 86 Can distillation 24.19-49.23 ℃, the 14.7--44.8mm mercury column. " P407 Cobalt salts acid oxidation cobalt salt acid system on the handbook
LiCl 614 1360 Lithium can be emitted hydrogen with water and acid effect, and easy and oxidation is closed. " dictionary " P806 lithium hydroxide salt acid system
NiCl 2 80 973 ℃ of distillations Dissociation pressure: 20 ℃, the 4.6mm mercury column.Ni2O3 is dissolved in hot hydrochloric acid and emits chlorine, and NiO is dissolved in acid. " " the P527 nickel oxide salt acid system under the handbook of P434 nickel salts acid system on the handbook
Table 2
The materialization data of part metal chloride
The muriate title Fusing point (℃) Boiling point (℃) The heat of sublimation (or heat of gasification) (kilocalorie/mol) Vapour pressure and other The generation method
CuCl 2 498 (anhydrides) 993 (being decomposed into CuCl) (-) 50.3--226.3 ℃ of 62--185mmHg CuO is dissolved in dilute hydrochloric acid " meticulous " P47 metallic copper adds thermal chlorination " P416 cupric oxide salt acid system on the handbook
BiCl 3 230 447 430 ℃ of distillations Facile hydrolysis forms subsalt Bi2O3 and is dissolved in hydrochloric acid and becomes BiCI3 " reagent " P70 bismuth metal adds thermal chlorination " reagent " P15 oxygen salt acid system
AgCl 455 1550 Ag2O is dissolved in the concentrated hydrochloric acid that boils " reagent " P32, P97 silver suboxide salt acid system
InCl 3 600 ℃ of distillations Facile hydrolysis is dissolved in hot acid.The hydrochloric acid that In2O5 is dissolved in heat becomes InCI3 " meticulous " P17 125 ℃ of chlorinations of indium metal " reagent " P21 Indium sesquioxide salt acid system
GaCl 77.9 Be dissolved in hot water, be slightly soluble in hot acid.The trivalent of gallium is an amphoteric substance " meticulous " P16 200 ℃ of chlorinations of gallium " reagent " P20 " dictionary " P944
SbCl 3 73.4 223 118 ℃, 12.11 (heat of gasification) 50.3-226.3 ℃, 12.6--797.3mm mercury column Sb2O3 is dissolved in concentrated hydrochloric acid becomes SbCI3 " " the P509 weisspiessglanz salt acid system under the handbook of 200 ℃ of chlorinations of P393 metallic antimony on the handbook
SnCl 4 -30.2 114 (32.6 heat of gasification) -0---319.35 ℃, 2.78--28079mm mercury column SnO2 is dissolved in hot hydrochloric acid becomes SnCI4 " 110 ℃ of chlorination metals of P455 metallic tin pink salt acid system on the handbook
GeCI4 49.5 83.1 Yi Yushui plays hydrolytic action.GeO2 is dissolved in acid becomes GeCI4 " reagent " P78 500-600 ℃ of chlorination of germanium " reagent " P29 germanium oxide salt acid system
Table 3
The materialization data of part non-metallic element and oxide compound thereof
Title Fusing point (℃) Boiling point (℃) The heat of sublimation (or heat of gasification) (kilocalorie/mol) Vapour pressure and other Data source
B2O3 450 1860 Certain solubility is arranged in the water.The water temperature high-dissolvability increases. " reagent " P16
P2O5 569 300 ℃ of distillations The water-soluble formation metaphosphoric acid of 591 ℃ of 760mmHg of 481 ℃ of 440mmHg. " reagent " P29 " P148 under the handbook
As2O3 312.3 193 ℃ of distillations Be dissolved in hydrochloric acid and generate arsenic trichloride. " reagent " P13
B 2100 2500 2550 ℃ of distillations 300 ℃ of oxidized generation B2O3. " complete works " P50
P 44.1 280 200 ℃ of oxidized generation P2O5. " dictionary " P966
As 817 615 ℃ of distillations " dictionary " P587
C 400 ℃ of oxidized generation CO2. The graphite data
S 119.6 446.4 363 ℃ of oxidized generation SO2 " dictionary " P763
O Oxygen is emitted in 650 ℃ of Si2O SiO4 decomposition half an hour.

Claims (19)

1. the preparation method of a hyperpure silicon is characterized in that, prepares hyperpure silicon by following operation by Pure Silicon Metal:
A. Pure Silicon Metal is pulverized and be fine particle;
B. silicon grain is packed into the crucible internal heating of high frequency furnace, aerating oxygen makes the impurity in the silicon be oxidized to oxide compound;
C. silicon grain is packed in the glassed steel reaction vessels, add hydrochloric acid and heating, make the impurity reaction in the silicon become muriate, leach reaction solution, feed nitrogen silicon grain moisture content is dried up;
D. silicon grain is packed into the crucible internal heating of high frequency induction furnace feeds chlorine in certain temperature range, make the impurity in the silicon further generate muriate, stops to make the silicon fusion until higher temperature behind the logical chlorine;
E. silicon melt is poured into and to be placed with releasing agent in advance, have in the bucket-shaped mold of senior insulation efficiency, cool off lentamente with in the middle of realizing and solidify, reach impurity is got rid of periphery between crucible inwall and content silicon, after cooling and demolding and the cleaning, acquisition ingot bar goods.
F. silicon melt or silicon grain are packed in the horizontal multi-stage type tube furnace, unlatching hangs on and is nested in the boiler tube outer radial periphery below the rail, the radio-frequency induction coil that can move along the boiler tube axial direction due, end in beginning moves towards axial the other end direction, can catch up with the impurity in the melted silicon to the boiler tube termination, after one short boiler tube of the impurity that concentrates and content silicon taken off, reinstall the end axle, radio-frequency induction coil is transferred to an end of beginning, repeat aforesaid operations and become to catching up with impurity, remove the boiler tube segment of the impurity that concentrates again.
2. the preparation method of hyperpure silicon as claimed in claim 1 is characterized in that, carries out entering B operation, C operation, D operation and E operation or F operation again after the A operation.
3. the preparation method of hyperpure silicon as claimed in claim 1 is characterized in that, carries out entering C operation, D operation and E operation or F operation again after the A operation.
4. the preparation method of hyperpure silicon as claimed in claim 1 is characterized in that, carries out entering B operation, C operation and E operation or F operation again after the A operation.
5. the preparation method of hyperpure silicon as claimed in claim 1 is characterized in that, carries out entering B operation and E operation or F operation again after the A operation.
6. the preparation method of hyperpure silicon as claimed in claim 1 is characterized in that, carries out entering C operation and E operation or F operation again after the A operation.
7. the preparation method of hyperpure silicon as claimed in claim 1 is characterized in that, carries out entering D operation and E operation or F operation again after the A operation.
8. as the preparation method of claim 1,2,3,4,5,6,7 described hyperpure silicons, it is characterized in that it is that fine grain diameter is 5 millimeter that described Pure Silicon Metal is pulverized.
9. as the preparation method of claim 1,2,4,5 described hyperpure silicons, it is characterized in that the logical oxygen temperature of B operation is by normal temperature to 650 ℃, and 650 ℃ of constant temperature 1 hour.
10. as the preparation method of claim 1,2,4,6 described hyperpure silicons, it is characterized in that the used hydrochloric acid of C operation is concentrated hydrochloric acid, the carrying out along with reaction adds water gradually towards rare, to be fit to various impurity and the required dense and rare requirement of hydrochloric acid reaction in the silicon.
11. the preparation method as claim 1,2,3 described hyperpure silicons is characterized in that, the temperature of the logical chlorine of D operation is by normal temperature to 260 ℃, and the logical chlorine time is 1 hour; The melt temperature of D operation silicon be 1900 ℃ and more than.
12. the preparation method as claim 1,2,3,4,5,6,7 described hyperpure silicons is characterized in that, the melt temperature of F operation silicon be 1600 ℃ and more than.
13. preparation method as claim 1,2,3,4,5,6,7 described hyperpure silicons, it is characterized in that the releasing agent that is used in the bucket-shaped mold of E operation is the pulvis of 120 order left and right sides fineness of ferric oxide 35-45%, calcium oxide 25-35% and silicon-dioxide 20-30% weight composition.
14. the preparation facilities of a hyperpure silicon is characterized in that, requires to be configured according to claim 1,2,3,4,5,6,7 described concrete operations, comprises: be used for A operation crusher; Be used for B operation, the heating of D operation and molten silicon particulate high frequency furnace; The glassed steel reaction vessels that is used for the C operation; The bucket-shaped mold and the insulation adiabatic system that are used for the E operation; Be used for the horizontal multi-stage type boiler tube of F operation and in radial outer periphery, be used to the system that heats and walk towards axially movable radio-frequency induction coil etc.; Be used to hold the crucible and the multi-stage type tube furnace boiler tube of heating and molten silicon.
15. the horizontal multi-stage type boiler tube of the F operation of hyperpure silicon preparation facilities as claimed in claim 14, it is characterized in that, the multi-stage type pipe is that many sections straight lengths are formed, connect with flange between pipeline section, two terminations of whole boiler tube respectively are equipped with the short bend pipe of import and export of bolster and melt silicon or silicon grain, and this axis of importing and exporting short bend pipe is parallel with the boiler tube axis.One end linking number of boiler tube cuts the pipeline section that accounts for boiler tube total length 5-20% length.
16. the B operation of hyperpure silicon preparation facilities as claimed in claim 14, the heating of D operation and molten silicon particulate high frequency furnace, it is characterized in that, the inlet pipe of above-mentioned gas is equipped with in the bottom of high frequency furnace crucible, the onesize crucible that gas exhaust duct is housed of back-off above this crucible, vacuum fan after also having the waste gas absorption tower of pipe coupling therewith and being contained in tower.
17. the horizontal multi-stage type boiler tube of the F operation of hyperpure silicon preparation facilities as claimed in claim 14 and in radial outer periphery, towards axially movable radio-frequency induction coil, it is characterized in that radio-frequency induction coil is for being nested in multi-stage type boiler tube external diameter periphery, and can move along the boiler tube axial direction due; Radio-frequency induction coil hangs on the rail below, and rail is same plane and parallel with the axial of multi-stage type boiler tube axially; Radio-frequency induction coil drives with the stepper-motor that is installed on the rail.
18. the bucket-shaped mold of the E operation of hyperpure silicon preparation facilities as claimed in claim 14 is characterized in that, mold is bucket-shaped, does the heat-insulating material insulation with the zirconium white hollow ball around its six.Multi-stage type boiler tube pipe is outward also with this lagging material insulation.
19. hyperpure silicon preparation facilities as claimed in claim 14.It is characterized in that, be used to heat with the crucible of molten silicon, bucket-shaped mold and multi-stage type tubular type furnace tube material and be all graphite, but all serve as a contrast the silicon-dioxide lining at their inwall, and in multi-stage type tube furnace outer wall coated with silicon dioxide coating.
CN 200410003090 2004-01-19 2004-01-19 Method and device for preparing super pure silicon from metal silicon Pending CN1648041A (en)

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RU2388691C2 (en) * 2008-04-29 2010-05-10 Российская Академия сельскохозяйственных наук Государственное научное учреждение Всероссийский научно-исследовательский институт электрификации сельского хозяйства (ГНУ ВИЭСХ РОССЕЛЬХОЗАКАДЕМИИ) Method of purifying powdered silicon (versions)
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CN102425933A (en) * 2011-08-25 2012-04-25 南京邮电大学 Zone melting device for highly purifying polymer semiconductor and method
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CN104271506B (en) * 2012-03-08 2015-11-11 菲罗索拉硅太阳能公司 For the manufacture of the method for HIGH-PURITY SILICON, the HIGH-PURITY SILICON obtained by the method and the silicon raw material for the manufacture of HIGH-PURITY SILICON
CN102849741B (en) * 2012-04-19 2014-05-14 北京民海艳科技有限公司 Intermediate-frequency induction furnace for solar energy polysilicon purification by metallurgy method and polysilicon purification method
CN102849741A (en) * 2012-04-19 2013-01-02 北京民海艳科技有限公司 Intermediate-frequency induction furnace for solar energy polysilicon purification by metallurgy method and polysilicon purification method
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CN106608629A (en) * 2016-12-21 2017-05-03 上海杉杉科技有限公司 Method and device for preparing high-purity silicon monoxide by medium-frequency induction heating way
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