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CN116262975A - Preparation and application of a supported nanometer ruthenium dioxide catalyst - Google Patents

Preparation and application of a supported nanometer ruthenium dioxide catalyst Download PDF

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CN116262975A
CN116262975A CN202111545800.8A CN202111545800A CN116262975A CN 116262975 A CN116262975 A CN 116262975A CN 202111545800 A CN202111545800 A CN 202111545800A CN 116262975 A CN116262975 A CN 116262975A
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aqueous solution
reaction
ruo
sulfite
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王素力
李焕巧
孙公权
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Dalian Institute of Chemical Physics of CAS
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    • C25B11/093Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material consisting of at least one catalytic element and at least one catalytic compound; consisting of two or more catalytic elements or catalytic compounds at least one noble metal or noble metal oxide and at least one non-noble metal oxide

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Abstract

The invention discloses a supported RuO 2 The preparation method and application of the nano catalyst are as follows: step one, adding an aqueous solution containing sulfite ions into an Ru precursor aqueous solution to carry out complexation reaction to obtain [ Ru (SO) 3 ) 3 ] 3‑ A complex; step two, adding an alkaline aqueous solution into the reaction system of the step one to adjust the pH value, so that the complex is separated out in a precipitation form; step three, washing the precipitate and then mixing with H 2 O 2 Carrying out a reaction to obtain ruthenium oxide colloid dispersion; and step four, adding a carrier into the colloid dispersion liquid for soaking, centrifuging, washing and drying to obtain the supported ruthenium dioxide nano catalyst. The preparation method provided by the invention avoids adsorption poisoning of chloride ions on the surface of the catalyst, and simultaneously, H 2 O 2 The oxidant replaces air to raise temperature for oxidation, the reaction temperature is low, and the method can avoidRuO 2 The agglomeration grows up, which is helpful for improving the activity of the catalyst.

Description

Preparation and application of supported nano ruthenium dioxide catalyst
Technical Field
The invention belongs to the technical field of catalysis, and particularly relates to a preparation method and application of a ruthenium dioxide nano catalyst.
Background
Compared with other oxides, the ruthenium dioxide has good conductivity, ru has more chemical valence states, the ruthenium dioxide material has small internal stress and stable structure in the conversion process of different valence states, and has wide application prospect in the fields of chlor-alkali, chlorate production, electrocatalysis, super capacitor and the like. Numerous research surfaces, ruO 2 Catalytic performance of (C) and RuO 2 (110) RuO with nanoscale related to Ru atoms with unsaturated coordination on the face 2 Has better reactivity and high utilization efficiency, thus the supported RuO 2 The research and development of the nano catalyst have important significance.
The preparation of supported ruthenium dioxide nano catalyst usually adopts a method of sodium hydroxide sedimentation reoxidation, for example, chinese patent CN1522176A discloses a method for preparing alumina supported ruthenium and a method for oxidizing alcohol, and the applicant uses sodium hydroxide and RuCl 3 The reaction is carried out to obtain Ru (OH) 3 Alumina intermediate state, and then oxidized in air to obtain RuO 2 Alumina. Also, alkaline substances such as NaOH or NaHCO are used 3 For RuCl 3 Precipitating, then gelling, and then oxidizing with hydrogen peroxide or chlorine gas solution, or oxidizing by heat treatment to prepare nanometer RuO 2 . It has also been proposed to prepare nanoscale RuO by chemical vapor deposition using organoruthenium as a precursor 2 And is used for high performance supercapacitor materials and gas sensors, etc. (J Electrochem Soc, 2005). Liu et al propose the preparation of RuO by magnetron sputtering 2 (Small, 2005), US20130059078A1 discloses a RuO 2 Is prepared through depositing an organic metal atom to obtain seed layer, and RuO 4 Steam is used as a precursor, and RuO is utilized 4 Reacts with seed layers to form RuO 2 A nano-film. The RuO is prepared by decomposing and gasifying metallic ruthenium by a direct oxidation method and reacting the metallic ruthenium with oxygen in industry 2 However, the method has low preparation efficiency, difficult separation, uncontrollable granularity and high requirement on instruments in the whole process, and adopts a calcination method to directly calcine rutheniumThe obtained ruthenium dioxide powder has large granularity and grain shape difference and poor uniformity, is only suitable for manufacturing high-resistance materials, and has limited application range.
To sum up, currently supported nano RuO 2 The catalyst still faces the complex preparation process and RuO 2 The nano particles are larger, the agglomeration of the particles is serious, the nano particles are difficult to uniformly disperse on the carrier, the acting force with the carrier is weak, and the like. With development and utilization of ruthenium resources, ruO 2 Because of the outstanding electrochemical performance and catalytic performance of the nano RuO catalyst, people are increasingly focused in the new energy field, how to prepare the high-performance supported nano RuO 2 A catalyst such that RuO 2 The catalyst is highly and evenly dispersed on the surface of the carrier, has smaller particle size, has less impurity content on the surface of the catalyst and high reaction activity, is an important research content about Ru utilization at home and abroad at present, and is also one of important technologies for Ru resource development and utilization.
Disclosure of Invention
Aiming at the problems in the prior art, the invention provides a supported RuO 2 The preparation method of the nano catalyst is different from the prior method for preparing RuO by directly adopting RuCl3 to precipitate with alkali solution and then oxidize 2 According to the traditional method, chloride ions in RuCl3 are replaced based on a ligand replacement method, so that adsorption poisoning of the chloride ions on the surface of the catalyst is avoided, and the activity of the catalyst is high; next, the invention uses liquid H 2 O 2 The oxidant is used for replacing air to raise the temperature for oxidization, the reaction temperature is lower, and RuO can be avoided 2 Agglomeration and growth; thirdly, the invention has simple steps for synthesizing the water system, and can solve the existing supported RuO 2 The preparation process of the nano catalyst is complex, the conditions are harsh, and the mass preparation is difficult.
In order to achieve the technical purpose, the technical scheme of the invention is as follows:
supported RuO 2 The preparation method of the nano catalyst comprises the following steps:
step one, adding an aqueous solution containing sulfite ions into an Ru precursor aqueous solution to carry out complexation reaction to obtain [ Ru (SO) 3 ) 3 ] 3- A complex;
step two, adding an alkaline aqueous solution into the reaction system of the step one to adjust the pH value, so that the complex is separated out in a precipitation form;
step three, washing the precipitate and then mixing with H 2 O 2 Carrying out a reaction to obtain ruthenium oxide colloid dispersion;
step four, adding a carrier into the colloid dispersion liquid for soaking, centrifuging, washing and drying after soaking to obtain the supported RuO 2 A nano catalyst.
Preferably, the preparation method specifically comprises the following steps:
step 1, adding a water-soluble Ru precursor into deionized water, and performing ultrasonic treatment until the Ru precursor is completely dissolved to prepare an Ru precursor aqueous solution;
step 2, slowly adding an aqueous solution containing sulfite ions into a precursor aqueous solution of Ru dropwise at room temperature, stirring at the same time, stopping dropwise adding when the color of the solution changes from red to light green, and converting a ligand of Ru from chloride ions into sulfite ions at the moment;
step 3, slowly adding the alkaline aqueous solution into the reaction system in the step 2, stirring at the same time, and adjusting the pH of the reaction system to 8-11, wherein the reaction system gradually changes from light green to dark green;
step 4, maintaining the pH value of the reaction system unchanged, continuously dropwise adding the aqueous solution containing sulfite ions into the dark green solution in the step 3 under the stirring condition, wherein blue-green precipitates are generated in the reaction system, stopping dropwise adding after the blue-green precipitates are not separated out, and continuously reacting for 1-2 hours after the dropwise adding is finished so as to ensure that the precipitates are complete;
step 5, washing, filtering and drying the blue-green precipitate generated in the step 4 by using a large amount of deionized water to obtain blue-green ruthenium sulfite powder;
step 6, dissolving blue-green ruthenium sulfite powder in a dilute acid aqueous solution under the stirring condition, adding a carrier material, and dropwise adding H into a reaction system after ultrasonic dispersion 2 O 2 The aqueous solution is heated to react for 2 to 3 hours, then cooled, and the acidic aqueous solution is continuously added to promote RuO 2 Sedimentation on the surface of the support;
step 7, centrifugally separating the reaction liquid in the step 6, washing the reaction liquid with a large amount of deionized water, and drying the reaction liquid after solid-liquid separation to obtain the supported RuO 2 A nano catalyst.
Preferably, the Ru precursor in the step 1 is one or more of ruthenic acid chloride, ruthenium trichloride, potassium ruthenate chloride, sodium ruthenate chloride and ammonium ruthenate chloride, and the Ru concentration in the Ru precursor aqueous solution is 5-50g/[.
Preferably, the slow dropping speed in the step 2 is 1-3mL/min, the stirring rotating speed is 200-1000r/min, the sulfite aqueous solution is one or more of sulfite, sodium bisulfate, potassium sulfite and potassium bisulfate aqueous solution, and the concentration of the sulfite in the aqueous solution is 50-100g/L; when the solution turns to light green, the pH of the reaction system is 4-5, and the molar ratio of sulfite to Ru ions in the reaction system is 5:1-20:1.
Preferably, the dropping speed of the alkaline aqueous solution in the step 3 is 5-10mL/min, the stirring speed is 200-1000r/min, and the alkaline aqueous solution adopts one or more of sodium carbonate, sodium bicarbonate, sodium hydroxide, potassium hydroxide or aqueous ammonia.
Preferably, the pH of the reaction system in the step 4 is 7.5-10, the stirring speed is 200-1000rpm, and the reaction temperature is 0-60 ℃.
Preferably, the dilute acid solution in the step 6 is one or more of dilute sulfuric acid, dilute hydrochloric acid and acetic acid aqueous solution, the concentration is 0.05-0.2mol/L, the pH of the reaction system is 2-5, and the pH in the step 6 is H 2 O 2 The molar ratio of the addition amount to the ruthenium sulfite is 1:1-5:1; the reaction temperature is 60-90 ℃; the carrier comprises one or more of active carbon, conductive carbon, mesoporous carbon, carbon aerosol, aluminum oxide, silicon dioxide, zirconium dioxide and cerium dioxide.
Preferably, the solid-liquid separation in the step 7 is centrifugation or filtration; the drying temperature is 30-60 ℃.
RuO in the catalyst prepared by the method 2 The particle size of the nano particles is 1-5 nanometers.
The invention also discloses the supported RuO prepared by the method 2 The nano catalyst can be used for electrolytic water oxygen evolution reaction.
The reason that the water-soluble Ru precursor is adopted in the step 1 is that the water-soluble Ru precursor is easy to prepare and low in price, and the water phase synthesis is beneficial to subsequent batch amplification, so that the environmental pollution is small, and the preparation cost is low;
step 2 by slowly adding sulfite precursor solution into Ru precursor water solution, complexing with Ru by strong coordination of sulfite to obtain [ Ru (SO) 3 ) 3 ] 3- The complex can replace chloride ions, and the adsorption of the chloride ions on the surface of the catalyst leads to RuO 2 The main reason for the low performance of the nano catalyst is that [ SO ] 3 ] 2- After the ligand replaces the chloride ion, SO 3 2- Is an inorganic compound stabilizer, can protect ruthenium oxide nano particles formed subsequently from agglomeration and SO 3 2- Can be automatically removed in the subsequent oxidation and drying process, and can not be strongly adsorbed on the surface of the catalyst.
The purpose of adopting the slow dropwise adding of sulfite in the step 2 is to control the adding amount of sulfite, because the sulfite has a certain reducibility, the Ru precursor is easy to directly reduce and generate due to the excessively fast dropwise adding, and [ Ru (SO) 3 ) 3 ] 3- A complex;
the slow addition of the alkaline aqueous solution in step 3 is to adjust the pH of the reaction system to weakly alkaline because [ Ru (SO) 3 ) 3 ] 3- The complex exists in the form of ions in strong acid and strong alkaline solutions, and can be separated out from the solution in the form of green precipitation only when the pH is weak alkaline;
continuously adding a sulfite solution in the step 4 ensures that precipitation is complete, and ensures that 100% of Ru species in the solution are separated out from the solution and are completely converted into ruthenium sulfite;
in the step 5, a large amount of deionized water is adopted for washing so as to ensure the effective removal of impurity ions;
in step 6, H is adopted 2 O 2 Is an oxidizing agent due to H 2 O 2 After the reaction, the product is water, so that pollution to a reaction system is avoided; and liquid H 2 O 2 The oxidant is used for replacing air to raise the temperature for oxidization, the reaction temperature is lower, and RuO can be avoided 2 The agglomeration grows up, and dilute acid aqueous solution is added after the reaction to destroy RuO 2 Colloid stability, and subsequent solid-liquid separation to obtain supported RuO 2 A nano-catalyst;
the drying temperature in the step 7 is maintained at 30-60 ℃ to avoid RuO caused by high-temperature drying 2 Agglomeration phenomenon of nanoparticles.
From the above description, it can be seen that the present invention has the following advantages:
1. unlike the prior art in which RuCl is directly adopted 3 Precipitating with alkali solution and oxidizing to prepare RuO 2 The present invention relates to a ligand-displacement method for RuCl 3 The medium chloride ions are replaced, so that adsorption poisoning of the chloride ions on the surface of the catalyst is avoided, and the activity of the catalyst is high;
2. the invention uses liquid H 2 O 2 The oxidant is used for replacing air to raise the temperature for oxidization, the reaction temperature is lower, and RuO can be avoided 2 Agglomeration and growth;
3. the invention can prepare RuO with small size and good dispersivity in aqueous solution without adding protective agent 2 The nano catalyst has the advantages of simple operation, mild reaction condition, environmental protection, low production cost and easy amplified synthesis.
Drawings
FIG. 1 is a RuO prepared in comparative example 1 of the present invention 2 TEM pictures of catalyst.
FIG. 2 is a RuO prepared in comparative example 1 of the present invention 2 XRD spectrum of catalyst/C.
FIG. 3 is a RuO prepared in example 1 of the present invention 2 TEM pictures of catalyst.
FIG. 4 is a RuO prepared in example 1 of the present invention 2 XRD spectrum of catalyst/C.
Detailed Description
The invention is described in detail below with reference to examples. Unless otherwise specified, the raw materials used in the following examples and comparative examples were all commercially available conventional raw materials.
Comparative example 1
Activated carbon supported RuO 2 Preparation of C nanocatalyst
1 g RuCl was added at room temperature 3 And 1.5 g XC-72R carbon black are dissolved in 10mL deionized water in an ultrasonic dispersion way, 50g/L sodium hydroxide aqueous solution is added dropwise, the dropping speed is 2 mL/min, the dropwise addition is stopped when the pH value of the reaction system rises to 13, ru (OH) is arranged at the bottom of the container after the reaction is continued for five days after the reaction is continued 3 precipitating/XC-72R, centrifuging, and drying to obtain Ru (OH) 3 The solid powder of XC-72R is heat treated for 1 hour at 300 ℃ in air atmosphere to obtain RuO 2 The XRD and TEM characterization shows that the ruthenium oxide particles in the prepared catalyst have large size and serious agglomeration, and partial ruthenium oxide is decomposed into reduced metal Ru in the heat treatment of air.
The electrochemical activity of the obtained catalyst is evaluated by adopting a rotary disk electrode, and the specific steps are as follows: accurately weigh 5mg of RuO 2 And (3) mixing the catalyst/C with 20 microliters of Nafion (5 wt%) solution and 5 milliliters of ethanol, performing ultrasonic treatment to obtain uniformly dispersed catalyst slurry, transferring 10 microliters of catalyst slurry to coat on a GC rotating disc electrode with the area of 0.19625 square centimeters, and drying to obtain the working electrode. The activity of the catalyst on the oxygen evolution reaction of electrolyzed water was evaluated in a 0.1M sulfuric acid aqueous solution with nitrogen gas, by scanning from 0 to 1.2 volts at a scan rate of 10mV/s at room temperature, recording 10mA/cm 2 The oxygen evolution reaction corresponding to the electrolysis current has overpotential, and the lower the overpotential is, the indication of RuO 2 The oxygen evolution reaction activity of/C is high. RuO obtained in comparative example 1 2 XC-72R at 10mA/cm 2 The corresponding oxygen evolution reaction overpotential was 400mV.
Example 1
Step 1, 1 g RuCl at room temperature 3 Ultrasonic dispersing and dissolving in 75mL deionized water to prepare RuCl 3 The concentration of the aqueous solution is 5gRu/L according to Ru;
step 2, to RuCl 3 Adding the concentrated solution dropwiseThe dropping speed of the aqueous solution of sodium bisulphite with the temperature of 50g/L is 2 ml/min, and the dropping is stopped when the reaction system turns from reddish brown to light green, and the pH of the solution is about 4-5;
step 3, adjusting the pH of the reaction system to be 12 by using a sodium carbonate aqueous solution, stopping dripping, and gradually changing the reaction system from light green to dark green;
step 4, maintaining the pH value of the reaction system unchanged by using a sodium carbonate aqueous solution, continuously dropwise adding a sulfite aqueous solution into the dark green solution in the step 3 under the stirring condition, generating blue-green precipitate in the reaction system, and continuously stirring and reacting for 1 hour under the room temperature condition to ensure that the precipitate is complete;
and 5, separating the white precipitate from the supernatant by adopting a centrifugal machine, and washing the blue-green precipitate by adopting a large amount of deionized water until no chloride ions exist in the precipitate.
Step 6, dissolving the washed blue-green precipitate with 0.2mol/L dilute sulfuric acid solution to obtain light blue transparent liquid, adding 1.48g of Xc-72R carbon black, and adding excessive H after ultrasonic dispersion 2 O 2 Aqueous solution (30 wt% H) 2 O 2 Aqueous solution, wherein H 2 O 2 The molar ratio of Ru to Ru is 2:1), the reaction temperature of the reaction system is controlled to be 80 ℃, a condensing tube is required to be installed during the heating process and the reaction to prevent excessive volatilization loss of moisture, the concentration of reactants in the reaction system is kept unchanged, the reaction is carried out for 3 hours, 20 milliliters of sulfuric acid solution with the concentration of 0.5 mol/L is added into the reaction system after the temperature is reduced, and the reaction system is kept stand for 1 hour;
and 7, centrifugally separating the reaction solution in the step 6, washing with a large amount of deionized water, putting the obtained solid after centrifugation in a vacuum oven, drying at 40 ℃ for 4 hours, and taking out to obtain the ruthenium oxide nano catalyst.
FIG. 2 shows the prepared RuO 2 XRD spectrum of XC-72R nano catalyst, from the extent of broadening of corresponding XRD diffraction peak, the prepared RuO 2 The XC-72R nano catalyst particles are smaller, and the average grain size of the ruthenium oxide particles is about 1.0nm as calculated by using the Shelle formula.
Adopts and connectsComparative example 1 the same apparatus and Activity evaluation method test the RuO prepared in example 1 2 Catalytic Activity of the XC-72R catalyst. As a result, it was found that under the same test conditions, ruO prepared in example 1 2 XC-72R corresponds to 10mA/cm 2 The overpotential of the oxygen evolution reaction under the current density is 250mV, which is 150mV lower than that of the catalyst prepared by the comparative example, and the oxygen evolution reaction activity is high.
Example 2
The specific experimental procedure of this example is similar to that of example 1, except that KB-300J conductive carbon black is used as the carbon support and 50g of Ru precursor is used Ru Potassium chlororuthenate/L, a sulfite precursor solution is 50g/L potassium sulfite aqueous solution, wherein the dropping speed of sulfite into Ru precursor is 5ml/min, when the solution turns from reddish brown to light green, the mole ratio of the sulfite solution to Ru precursor in a reaction system is 10:1, the pH value is about 4, the stirring speed of 1000rpm is kept, the dropping is stopped when the pH value of the reaction system is regulated to be 10 by using sodium hydroxide aqueous solution, and the solution turns into dark green and has a small amount of blue-green precipitate; continuously dropwise adding a potassium sulfite aqueous solution into the reaction system until precipitation is not increased any more; the subsequent steps are the same as in example 1. RuO prepared in this example 2 The loading of the catalyst/KB-300J was 30wt%, in which RuO 2 The mass ratio of the catalyst to KB-300J is 3:7.
The obtained RuO is treated 2 The oxygen evolution reaction activity of the KB-300J catalyst was evaluated by using a rotating disk electrode, and the specific procedure was as in example 1. As a result, it was found that 10mA/cm 2 RuO prepared in example 2 at oxygen evolution current density 2 The oxygen evolution reaction overpotential corresponding to the ratio of KB-300J is 243mV, compared with RuO prepared in comparative example 2 A decrease in/XC-72R was 157mV.
Example 3
The experimental procedure of this example is similar to that of example 1, except that the carbon support is a carbon nanotube and the Ru precursor is 40g Ru Ruthenium acetate/L, sulfite precursor solution 80g/L potassium sulfite aqueous solution, wherein the dropping speed of sulfite into Ru precursor is 4ml/min, when the solution turns from reddish brown to light green, the reaction systemThe mol ratio of the sulfite solution to the Ru precursor is 20:1, the pH is about 5 at the moment, the stirring speed of 800rpm is kept, the dropwise addition is stopped when the pH of the reaction system is regulated to be 10.5 by using sodium hydroxide aqueous solution, and the color of the solution is changed into dark green and a small amount of blue-green precipitate is separated out; continuously dropwise adding a potassium sulfite aqueous solution into the reaction system until precipitation is not increased any more; the subsequent steps are the same as in example 1. RuO prepared in this example 2 The loading of the carbon nanotube catalyst was 40wt%, where RuO 2 The mass ratio of the catalyst to KB-300J is 4:6.
The obtained RuO is treated 2 The carbon nanotube catalyst was evaluated for oxygen evolution reactivity by using a rotating disk electrode, and the procedure was the same as in example 1. As a result, it was found that 10mA/cm 2 RuO prepared in example 3 at oxygen evolution current density 2 The overpotential of oxygen evolution reaction corresponding to/KB-300J is 213mV, compared with RuO prepared in comparative example 2 The decrease in XC-72R was 187mV.
It is to be understood that the foregoing detailed description of the invention is merely illustrative of the invention and is not limited to the embodiments of the invention. It will be understood by those of ordinary skill in the art that the present invention may be modified or substituted for elements thereof to achieve the same technical effects; as long as the use requirement is met, the invention is within the protection scope of the invention.

Claims (10)

1.一种担载型RuO2纳米催化剂的制备方法,其特征在于,所述方法包括如下步骤:1. a loaded type RuO The preparation method of nano - catalyst, is characterized in that, described method comprises the steps: 步骤一、将含有亚硫酸根离子的水溶液加入Ru前体水溶液中,进行络合反应,制得[Ru(SO3)3]3-络合物;Step 1, adding an aqueous solution containing sulfite ions into the Ru precursor aqueous solution to carry out complexation reaction to obtain [Ru(SO 3 ) 3 ] 3- complex; 步骤二、向步骤一的反应体系中加入碱性水溶液调节pH值,使所述络合物以沉淀的形式析出;Step 2, adding an alkaline aqueous solution to the reaction system in step 1 to adjust the pH value, so that the complex is precipitated in the form of precipitation; 步骤三、将所述沉淀洗涤后与H2O2进行反应,得到氧化钌胶体分散液;Step 3, washing the precipitate and reacting it with H 2 O 2 to obtain a colloidal dispersion of ruthenium oxide; 步骤四、向所述胶体分散液中加入载体进行浸渍,浸渍后,离心、洗涤、干燥,得到所述担载型RuO2纳米催化剂。Step 4, adding a carrier to the colloidal dispersion for impregnation, centrifuging, washing, and drying after impregnation to obtain the supported RuO 2 nanometer catalyst. 2.根据权利要求1所述的制备方法,其特征在于,所述方法具体包括以下步骤:2. preparation method according to claim 1, is characterized in that, described method specifically comprises the following steps: 步骤1,将水溶性Ru前体溶解于去离子水中,配置Ru前体水溶液;Step 1, dissolving the water-soluble Ru precursor in deionized water to prepare an aqueous Ru precursor solution; 步骤2,将含有亚硫酸根离子的水溶液室温下逐滴加入Ru前体水溶液中,同时进行搅拌,待溶液颜色由红色变为浅绿色时停止滴加,Ru的配体由氯离子转化为亚硫酸根离子;Step 2, add the aqueous solution containing sulfite ions dropwise to the Ru precursor aqueous solution at room temperature, and stir at the same time, stop the dropwise addition when the color of the solution changes from red to light green, and the Ru ligand is converted from chloride ion to sulfite. Sulfate ion; 步骤3,将碱性水溶液逐滴加入步骤2的反应体系中,同时进行搅拌,调节反应体系的pH为8-11,反应体系由浅绿色溶液逐渐变为深绿色溶液;Step 3, adding the alkaline aqueous solution to the reaction system of step 2 dropwise, stirring at the same time, adjusting the pH of the reaction system to 8-11, and the reaction system gradually changes from light green solution to dark green solution; 步骤4,维持反应体系的pH值不变,搅拌条件下继续向步骤3的深绿色溶液中滴加含有亚硫酸根离子的水溶液,反应体系中有蓝绿色沉淀生成,待蓝绿色沉淀不再继续析出后停止滴加,然后继续反应1-2小时以保证沉淀完全;Step 4, keep the pH value of the reaction system unchanged, and continue to add the aqueous solution containing sulfite ions dropwise to the dark green solution in step 3 under stirring conditions, a blue-green precipitate will be formed in the reaction system, and the blue-green precipitate will not continue After the precipitation, stop the dropwise addition, and then continue the reaction for 1-2 hours to ensure that the precipitation is complete; 步骤5,将步骤4中生成的蓝绿色沉淀用去离子水洗涤、过滤并烘干,得到蓝绿色的亚硫酸钌盐;Step 5, washing the blue-green precipitate generated in step 4 with deionized water, filtering and drying to obtain blue-green ruthenium sulfite; 步骤6,搅拌条件下,将蓝绿色的亚硫酸盐粉末溶解在酸性水溶液中,并加入载体,超声分散后向反应体系中滴加H2O2水溶液,升温反应2-3小时,降温,继续加入酸性水溶液促进RuO2在载体表面的沉降;Step 6, under stirring conditions, dissolve the blue-green sulfite powder in the acidic aqueous solution, and add the carrier, after ultrasonic dispersion, add the H 2 O 2 aqueous solution to the reaction system dropwise, heat up the reaction for 2-3 hours, cool down, and continue Adding an acidic aqueous solution promotes the precipitation of RuO2 on the surface of the carrier; 步骤7,将步骤6的反应液离心分离并用去离子水洗涤,固液分离后烘干,得到担载型RuO2纳米催化剂。In step 7, the reaction solution in step 6 is centrifuged and washed with deionized water, and dried after solid-liquid separation to obtain a supported RuO 2 nano-catalyst. 3.根据权利要求2所述的制备方法,其特征在于,所述步骤1中,Ru前体为氯钌酸、三氯化钌、氯钌酸钾、氯钌酸钠、氯钌酸铵中的一种或多种,Ru前体水溶液中Ru浓度为5-50g/L。3. the preparation method according to claim 2 is characterized in that, in described step 1, Ru precursor is in chlororuthenate acid, ruthenium trichloride, potassium chlororuthenate, sodium chlororuthenate, ammonium chlororuthenate One or more, the Ru concentration in the Ru precursor aqueous solution is 5-50g/L. 4.根据权利要求2所述的制备方法,其特征在于,所述步骤2中,滴加速度为1-3mL/min,搅拌速度为200-1000r/min,所述亚硫酸盐水溶液为亚硫酸、亚硫酸钠、亚硫酸氢钠、亚硫酸钾、亚硫酸氢钾水溶液中的一种或多种,亚硫酸根在水溶液中的浓度为50-100g/L;溶液变为浅绿色时,反应体系的pH为4-5,反应体系中亚硫酸根与Ru离子的摩尔比为5∶1~20∶1。4. preparation method according to claim 2, is characterized in that, in described step 2, rate of addition is 1-3mL/min, and stirring speed is 200-1000r/min, and described sulfite aqueous solution is sulfurous acid, One or more of sodium sulfite, sodium bisulfite, potassium sulfite, potassium bisulfite aqueous solution, the concentration of sulfite in the aqueous solution is 50-100g/L; when the solution turns light green, the pH of the reaction system 4-5, and the molar ratio of sulfite to Ru ions in the reaction system is 5:1-20:1. 5.根据权利要求2所述的制备方法,其特征在于,所述步骤3中,碱性水溶液的滴加速度为5-10mL/min,搅拌速度为200-1000r/min,所述碱性水溶液为碳酸钠、碳酸氢钠、氢氧化钠、氢氧化钾或氨水的水溶液中的一种或多种。5. preparation method according to claim 2, is characterized in that, in described step 3, the rate of addition of alkaline aqueous solution is 5-10mL/min, and stirring speed is 200-1000r/min, and described alkaline aqueous solution is One or more of sodium carbonate, sodium bicarbonate, sodium hydroxide, potassium hydroxide or aqueous ammonia. 6.根据权利要求2所述的制备方法,其特征在于,所述步骤4中,反应体系的pH为7.5-10,搅拌速度为200-1000rpm,反应温度为0-60℃。6. The preparation method according to claim 2, characterized in that, in the step 4, the pH of the reaction system is 7.5-10, the stirring speed is 200-1000 rpm, and the reaction temperature is 0-60°C. 7.根据权利要求2所述的制备方法,其特征在于,所述步骤6中,酸性水溶液为稀硫酸、稀盐酸、醋酸水溶液中的一种或多种,酸性水溶液的浓度为0.05-0.2mol/L,所述加酸调节后升温反应前反应体系的pH为2-5,H2O2加入量与亚硫酸盐的摩尔比为1∶1-5∶1;反应温度为60-90℃;所述载体包括活性碳、导电碳、中孔碳、碳气溶胶、三氧化二铝、二氧化硅、二氧化锆、二氧化铈中一种或多种;所述步骤7中,固液分离方式为离心或过滤;烘干温度为30-60℃。7. preparation method according to claim 2 is characterized in that, in described step 6, acidic aqueous solution is one or more in dilute sulfuric acid, dilute hydrochloric acid, acetic acid aqueous solution, and the concentration of acidic aqueous solution is 0.05-0.2mol /L, the pH of the reaction system before the temperature rise reaction after adding acid is 2-5, the molar ratio of H 2 O 2 added to sulfite is 1:1-5:1; the reaction temperature is 60-90°C The carrier includes one or more of active carbon, conductive carbon, mesoporous carbon, carbon aerosol, aluminum oxide, silicon dioxide, zirconium dioxide, and cerium oxide; in the step 7, the solid-liquid The separation method is centrifugation or filtration; the drying temperature is 30-60°C. 8.一种权利要求1-7任一所述的方法所制备的担载型RuO2纳米催化剂。8. a supported RuO nanometer catalyst prepared by the arbitrary described method of claim 1-7. 9.根据权利要求8所述的担载型RuO2纳米催化剂,其特征在于,RuO2纳米颗粒的粒径为1-5纳米。9. The supported RuO 2 nanocatalyst according to claim 8, characterized in that the particle diameter of the RuO 2 nanoparticles is 1-5 nanometers. 10.一种权利要求8所述的担载型RuO2纳米催化剂在电解水析氧反应中的应用。10. a kind of supported type RuO as claimed in claim 8 The application of nanometer catalyst in electrolysis water oxygen evolution reaction.
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