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WO1990015657A1 - Process for the separation of polycyclic hydrocarbons and heavy metals from waste gases - Google Patents

Process for the separation of polycyclic hydrocarbons and heavy metals from waste gases Download PDF

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Publication number
WO1990015657A1
WO1990015657A1 PCT/EP1990/000921 EP9000921W WO9015657A1 WO 1990015657 A1 WO1990015657 A1 WO 1990015657A1 EP 9000921 W EP9000921 W EP 9000921W WO 9015657 A1 WO9015657 A1 WO 9015657A1
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Prior art keywords
heavy metals
polycyclic hydrocarbons
gases
adsorbent
separation
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Ceased
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PCT/EP1990/000921
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German (de)
French (fr)
Inventor
Mehdi Haji-Javad
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ABB Technology FLB AB
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ABB Flaekt AB
Flaekt AB
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Publication of WO1990015657A1 publication Critical patent/WO1990015657A1/en
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/02—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by adsorption, e.g. preparative gas chromatography
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F23—COMBUSTION APPARATUS; COMBUSTION PROCESSES
    • F23J—REMOVAL OR TREATMENT OF COMBUSTION PRODUCTS OR COMBUSTION RESIDUES; FLUES 
    • F23J15/00—Arrangements of devices for treating smoke or fumes
    • F23J15/006—Layout of treatment plant
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F23—COMBUSTION APPARATUS; COMBUSTION PROCESSES
    • F23J—REMOVAL OR TREATMENT OF COMBUSTION PRODUCTS OR COMBUSTION RESIDUES; FLUES 
    • F23J2215/00—Preventing emissions
    • F23J2215/30—Halogen; Compounds thereof
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F23—COMBUSTION APPARATUS; COMBUSTION PROCESSES
    • F23J—REMOVAL OR TREATMENT OF COMBUSTION PRODUCTS OR COMBUSTION RESIDUES; FLUES 
    • F23J2219/00—Treatment devices
    • F23J2219/30—Sorption devices using carbon, e.g. coke

Definitions

  • the polycyclic hydrocarbons e.g. Halogenated dibenzodioxins and dibenzofurans (PCDD and PCDF) or polychlorinated benzenes and phenols, as well as locks all (e.g. Hg, Cd) can emit with the exhaust gases from the combustion plants, especially from waste and hazardous waste incineration plants.
  • PCDD and PCDF Halogenated dibenzodioxins and dibenzofurans
  • PCDF polychlorinated benzenes and phenols
  • locks all e.g. Hg, Cd
  • the polycyclic hydrocarbons which are extremely harmful to health (carcinogenic), can arise during combustion through complex recombination reactions from organic and inorganic compounds. These connections can only be separated to a limited extent in downstream cleaning systems (with the dust in the electrostatic filter or in the exhaust gas washing system). Some heavy metals (Hg, Cd), which are also harmful to health, can emit from the exhaust gas cleaning system in part in the gaseous state or as fine dust and aerosols at the existing exhaust gas temperatures.
  • Hg, Cd heavy metals
  • Figures 1 and 2 are examples of the invented process in connection with a conventional exhaust gas cleaning system behind one
  • Waste incineration consisting of an electrostatic filter for dust separation, a two-stage wash for
  • Heavy metals are separated with the fly ash.
  • Aerosols that leave the E-filter, accumulate or are partly in a gaseous state cannot be removed to a large extent in the E-filter.
  • the exhaust gases are passed through a heat exchanger to a two-stage scrubber, whereby the cooling to approx. 60 - 70 ° C and the use of absorbents (NaOH; Ca (OH) 2) the acidic exhaust gas components (HCI, HF, SOx) and further heavy metal fractions are deposited.
  • absorbents NaOH; Ca (OH) 2
  • HCI, HF, SOx acidic exhaust gas components
  • further heavy metal fractions are deposited.
  • the remaining hydrocarbons and heavy metals leave the washing plant as fine rods, aerosols or gases and, if no additional measures are provided, will be emitted from the chimney with the exhaust gases.
  • the emissions of these pollutants are to be combined
  • Adsorption filtering processes can be prevented.
  • the exhaust gas after washing is heated in a heat exchanger to approx. 70 to 150 ° C and mixed intensively in a reactor with finely divided powdery adsorbent.
  • the reactor can e.g. consist of a circulating fluidized bed, through which a large contact area between exhaust gas and adsorbent can be realized.
  • the polycyclic hydrocarbons and the heavy metals are already partially attached to the adsorbent.
  • the exhaust gas from the reactor is fed to a downstream fabric filter, where the adsorbent separates from the filter bags to form a filter cake. Since the exhaust gas is forced to flow through the filter cake, an extensive adsorptive separation of the remaining polycyclic hydrocarbons and the heavy metals takes place simultaneously with the dedusting.
  • All selectively acting substances e.g. Activated carbon, hydrated lime, molecular sieves and sodium sulfite with a high specific surface area can be used.
  • the branched off portion can be sent to the incineration plant for disposal, where the bound organic compounds thermally decompose and the heavy metals are released again and ultimately separated in the downstream systems (e-filter and exhaust gas scrubbing).
  • the method can be used either after the exhaust gas scrubbing or after the SCR system (catalytic NOx reduction using ammonia) directly in front of the chimney.
  • ammonia residues and possible ammonium salts NH4HS04, (NH4) 2S04
  • NH4HS04, (NH4) 2S04 ammonium salts
  • the invented process is characterized by a high degree of flexibility and adaptability to the respective operating conditions.
  • the adsorption process and plant operation can be optimized by the following measures:

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  • Engineering & Computer Science (AREA)
  • Chemical & Material Sciences (AREA)
  • Mechanical Engineering (AREA)
  • General Engineering & Computer Science (AREA)
  • Analytical Chemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Treating Waste Gases (AREA)

Abstract

The invention concerns a process for the removal of traces of pollutants from the exhaust gases from waste incineration plants. The invention calls for the gases, pre-cleaned in a gas purification plant to remove dust, acid gases (HCl, HF, SOx), heavy metals and NOx, to be freed of the remaining polycyclic hydrocarbons (e.g. dioxins and furanes) and heavy metals (e.g. Hg, Cd) by means of a combined adsorption/filtration process. To this end, the gases, at a temperature of about 70 to 160°C, are mixed in a reactor (C4) with suitable adsorption agents (e.g. activated charcoal, molecular sieves or slaked lime) and subsequently passed through a fibrous filter (F2). The pollutants are bound to the adsorption agent in the reactor and subsequently in the filter cake on the fibrous filter.

Description

Verfahren zur Abscheidunα. von polvzvklischen Kohlenwasserstoffen und Schwermetallen aus Abαasen Process for Abscheidunα. of polyhydric hydrocarbons and heavy metals from waste gases

Die polyzyklischen Kohlenwasserstoffe, z.B. halogenierte Dibenzodioxine und Dibenzofurane (PCDD und PCDF) oder polychlorierte Benzole und Phenole, sowie Schwerrne alle (z.B. Hg, Cd) können mit den Abgasen der Feuerungsanlagen, besonders von Müll- und Sondermüllverbrennungsanlagen, emittieren.The polycyclic hydrocarbons, e.g. Halogenated dibenzodioxins and dibenzofurans (PCDD and PCDF) or polychlorinated benzenes and phenols, as well as locks all (e.g. Hg, Cd) can emit with the exhaust gases from the combustion plants, especially from waste and hazardous waste incineration plants.

Die polyzyklischen Kohlenwasserstoffe, die stark gesundheitsschädigend wirken (krebserregend), können bei der Verbrennung durch komplexe Rekombinationsreaktionen aus organischen und anorganischen Verbindungen entstehen. Diese Verbindungen können nur begrenzt in nachgeschalteten Reinigungsanlagen (mit dem Flugstaub in Elektrofilter oder in der Abgaswaschanlage) abgeschieden werden. Auch einige Schwermetalle (Hg, Cd), die ebenfalls gesundheitsschädigend sind, können bei den vorliegenden Abgastemperaturen zum Teil im gasförmigen Zustand oder als Feinstäube und Aerosole aus der Abgasreinigungsanlage emittieren.The polycyclic hydrocarbons, which are extremely harmful to health (carcinogenic), can arise during combustion through complex recombination reactions from organic and inorganic compounds. These connections can only be separated to a limited extent in downstream cleaning systems (with the dust in the electrostatic filter or in the exhaust gas washing system). Some heavy metals (Hg, Cd), which are also harmful to health, can emit from the exhaust gas cleaning system in part in the gaseous state or as fine dust and aerosols at the existing exhaust gas temperatures.

Durch diese Erfindung können alle konventionell anwendbaren Abgasreinigungsverfahren hinsichtlich der Abscheidung von gesundheitsschädigenden organischen Verbindungen und Schwermetallen optimiert werden. In den Bildern 1 und 2 sind beispielhaft das erfundende Verfahren in Verbindung mit einer konventionellen Abgasreinigungsanlage hinter einerWith this invention, all conventionally applicable exhaust gas purification processes can be optimized with regard to the separation of harmful organic compounds and heavy metals. Figures 1 and 2 are examples of the invented process in connection with a conventional exhaust gas cleaning system behind one

Müllverbrennung, bestehend aus einem Elektrofilter zur Staubabscheidung, einer zweistufigen W sche zurWaste incineration, consisting of an electrostatic filter for dust separation, a two-stage wash for

Abscheidung von sauren Gasen (HCI, HF, SOx) und einerSeparation of acid gases (HCI, HF, SOx) and one

SCR-Anlage zur NOx-Reduzierung, dargestellt. Die aus der Verbrennungsanlage kommenden Abgase werden mit ca. 200 - 350°C zwecks Staubabscheidung zuerst zu einem Elektrofilter geführt. Abhängig von derSCR system for NOx reduction, shown. The exhaust gases coming from the incinerator are first led to an electrostatic precipitator at approx. 200 - 350 ° C for the purpose of dust separation. Depends on the

Auslegung des E-Filters und der Eigenschaften desDesign of the e-filter and the properties of the

Abgases und des Staubs können hoheExhaust and dust can be high

Staubabscheidegrade bzw. sehr niedrigeDegrees of dust separation or very low

3 Staubkonzentrationen (ca. 50 - 30 mg/m , i.N.) erreicht werden. Hierbei kann gleichzeitig ein hoher3 dust concentrations (approx. 50 - 30 mg / m, i.N.) can be reached. This can be a high one at the same time

Anteil der polyzyklischen Kohlenwasserstoffe undProportion of polycyclic hydrocarbons and

Schwermetalle mit der Flugasche abgeschieden werden.Heavy metals are separated with the fly ash.

Da diese Stoffe sich aber zum Teil an Feinstäube undHowever, since these substances partially adhere to fine dust and

Aerosolen, die den E-Filter verlassen, anlagern oder zum Teil in gasförmigem Zustand befinden, ist ihre weitgehende Entfernung im E-Filter nicht möglich.Aerosols that leave the E-filter, accumulate or are partly in a gaseous state cannot be removed to a large extent in the E-filter.

Nach der Entεtaubung werden die Abgase über einen Wärmetauscher zu einem zweistufigen Wäscher geführt, wodurch die Abkühlung auf ca. 60 - 70°C und den Einsatz von Absorptionsmitteln (NaOH; Ca(OH)2) die sauren Abgasbestandteile (HCI, HF, SOx) und weitere Schwermetallanteile abgeschieden werden. Die verbleibenden Kohlenwasserstoffe und Schwermetalle verlassen die Waschanlage als Feinstäbe, Aerosole oder Gase und werden, wenn keine zusätzlichen Maßnahmen vorgesehen, mit den Abgasen aus dem Schornstein emittieren. Erfindungsgemäß sollen die Emissionen dieser Schadstoffe durch ein kombiniertesAfter dedusting, the exhaust gases are passed through a heat exchanger to a two-stage scrubber, whereby the cooling to approx. 60 - 70 ° C and the use of absorbents (NaOH; Ca (OH) 2) the acidic exhaust gas components (HCI, HF, SOx) and further heavy metal fractions are deposited. The remaining hydrocarbons and heavy metals leave the washing plant as fine rods, aerosols or gases and, if no additional measures are provided, will be emitted from the chimney with the exhaust gases. According to the invention, the emissions of these pollutants are to be combined

Adsorptions-Filterations-Verfahren verhindert werden. Für diesen Zweck wird das Abgas nach der Wäsche in einem Wäremtauscher auf ca. 70 bis 150°C aufgeheizt und in einem Reaktor mit feinverteilten pulverförmigen Adsorptionsmittel intensiv vermischt. Der Reaktor kann z.B. aus einer zirkulierenden Wirbelschicht bestehen, durch die eine große Berührungsfläche zwischen Abgas und Adsorptionsmittel realisiert werden kann. Hier erfolgt bereits eine Teilanlagerung der polyzyklischen Kohlenwasserstoffe und der Schwermetalle an das Adsorptionsmittel. Das Abgas aus dem Reaktor wird zu einem nachgeschalteten Gewebefilter geführt, wo sich das Adsorptionsmittel unter Bildung eines Filterkuchens an den Filterschläuchen abscheidet. Da das Abgas zwangsweise durch den Filterkuchen strömen muß, findet hier gleichzeitig mit der Entstaubung eine weitgehende adsorptive Abscheidung der restlichen polyzyklischen Kohlenwasserstoffe und der Schwermetalle statt.Adsorption filtering processes can be prevented. For this purpose, the exhaust gas after washing is heated in a heat exchanger to approx. 70 to 150 ° C and mixed intensively in a reactor with finely divided powdery adsorbent. The reactor can e.g. consist of a circulating fluidized bed, through which a large contact area between exhaust gas and adsorbent can be realized. The polycyclic hydrocarbons and the heavy metals are already partially attached to the adsorbent. The exhaust gas from the reactor is fed to a downstream fabric filter, where the adsorbent separates from the filter bags to form a filter cake. Since the exhaust gas is forced to flow through the filter cake, an extensive adsorptive separation of the remaining polycyclic hydrocarbons and the heavy metals takes place simultaneously with the dedusting.

Als Adsorptionsmittel können alle selektiv wirkenden Stoffe, z.B. Aktivkohle, Kalkhydrat, Molekularsiebe und Natriumsulfit, mit einer hohen spezifischen Oberfläche zum Einsatz kommen.All selectively acting substances, e.g. Activated carbon, hydrated lime, molecular sieves and sodium sulfite with a high specific surface area can be used.

Durch die Rückführung des im Gewebefilter abgeschiedenen Adsorptionsmittels zum Reaktor wird eine hohe Staubkonzentration (ca. 5000 bis 50.000 mg/m 3 i.N.) und folglich ein hoher Kontakt zwischen Adsorptionsmittel und Abgas hergestellt. Je nach betrieblichen Erfordernissen wird zurBy returning the adsorbent separated in the fabric filter to the reactor, a high dust concentration (approx. 5000 to 50,000 mg / m 3 i.N.) and consequently a high contact between adsorbent and exhaust gas is produced. Depending on operational requirements,

Ausschleusung von adsorbierten Schadstoffen ein kleiner Anteil der rückgeführten Menge durch frisches Additiv ersetzt. Die abgezweigte Teilmenge kann für die Entsorgung zur Verbrennungsanlage geführt werden, wo die gebundenen organischen Verbindungen thermisch zersetzt und die Schwermetalle wieder freigesetzt und letztlich in den nachgeschalteten Anlagen (E-Filter und Abgaswäsche) abgeschieden werden.Removal of adsorbed pollutants small proportion of the returned quantity replaced by fresh additive. The branched off portion can be sent to the incineration plant for disposal, where the bound organic compounds thermally decompose and the heavy metals are released again and ultimately separated in the downstream systems (e-filter and exhaust gas scrubbing).

Wie aus den Bildern 1 und 2 hervorgeht, kann das Verfahren entweder nach der Abgaswäsche oder nach der SCR-Anlage (katalytische NOx-Reduktion mittels Ammoniak) direkt vor dem Schornstein zur Anwendung kommen. Für letztgenannten Fall können aus der SCR-Anlage stammende Ammoniakreste und mögliche Ammoniumsalze (NH4HS04, (NH4)2S04) ebenfalls mit abgeschieden werden.As can be seen in Figures 1 and 2, the method can be used either after the exhaust gas scrubbing or after the SCR system (catalytic NOx reduction using ammonia) directly in front of the chimney. In the latter case, ammonia residues and possible ammonium salts (NH4HS04, (NH4) 2S04) originating from the SCR system can also be separated.

Das erfundene Verfahren zeichnet sich durch eine hohe Flexibilität und Anpassungsf higkeit an die jeweiligen Betriebsverhältnisse aus. Je nach Anwendungsfall und vorliegenen Randbedingungen können Adsorptionsvorgang und Anlagenbetrieb durch folgende Maßnahmen optimiert werden:The invented process is characterized by a high degree of flexibility and adaptability to the respective operating conditions. Depending on the application and the existing boundary conditions, the adsorption process and plant operation can be optimized by the following measures:

Optimierung durch den Einsatz von verschiedenen selektiv wirkenden Adsorptionsmitteln in beliebigen Mengenverhälntissen (z.B. 20 % Aktivkohle und 80 % Kalkhydrat),Optimization through the use of various selectively acting adsorbents in any proportions (e.g. 20% activated carbon and 80% hydrated lime),

Optimierung durch die Anpassung des Abgas/Adsorptionsmittel-Kontakts durch die Regelung der vom Gewebefilter zurückgeführten Feststoffmengen, Optimierung durch die Anpassung des Verhältnisses von frischem zugeführtem Adsorptionsmittel,Optimization by adjusting the exhaust gas / adsorbent contact by regulating the amount of solids returned by the fabric filter, Optimization by adjusting the ratio of freshly supplied adsorbent,

Optimierung durch die Anpassung der Dicke des Filterkuchens durch entsprechende Regelung der Abreinigungszeiten des Gewebefilters,Optimization by adjusting the thickness of the filter cake by regulating the cleaning times of the fabric filter,

Optimierung durch die Einstellung der Betriebstemperatur in einem relativ weiten Bereich von ca. 70 bis 160°C. Optimization by setting the operating temperature in a relatively wide range from approx. 70 to 160 ° C.

Claims

Patentansprüche: Claims: 1. Verfahren zur Absscheidung von gesundheitsschädigenden polyzyklischen Kohlenwasserstoffen (z.B. Dioxine und Furane) und Schwermetallen aus den Abgasen von1.Process for the separation of health-damaging polycyclic hydrocarbons (e.g. dioxins and furans) and heavy metals from the exhaust gases of Äbfallverbrennungsanlagen (z.B. Müll- und Sondermüllverbrennung), dadurch gekennzeichnet, daß die von Staub, HCI, HF, SOx, NOx und Schwermetallen vorgereinigten Abgase durch Adsorption/Filtration im Temperaturbereich von 70 - 160°C von den restlichen polyzyklischen Kohlenwasserstoffen und Schwermetallen befreit werden.Waste incineration plants (e.g. waste and special waste incineration), characterized in that the waste gases pre-cleaned of dust, HCI, HF, SOx, NOx and heavy metals are freed from the remaining polycyclic hydrocarbons and heavy metals by adsorption / filtration in the temperature range of 70 - 160 ° C. 2. Verfahren nach Anspruch 1, dadurch gekennzeichnet, daß die vorgereinigten Abgase zuerst in einem Reaktor (C 4) mit feinverteilten Adsorptionsmitteln vermischt werden und anschließend zu einem filternden Abscheider2. The method according to claim 1, characterized in that the pre-cleaned exhaust gases are first mixed in a reactor (C 4) with finely divided adsorbents and then to a filtering separator (F 2) geführt werden, wo auf dem Filtergewebe ein Adsorptionsmittelkuchen erzeugt wird, den die Abgase durchströmen müssen, daß bei der Durchströmung des Filterkuchens eine weitgehende adsorptive Abscheidung von polyzyklischen Kohlenwasserstoffen und Schwermetallen stattfindet.(F 2) are performed, where an adsorbent cake is generated on the filter fabric, which the exhaust gases have to flow through, so that a large adsorptive separation of polycyclic hydrocarbons and heavy metals takes place when flowing through the filter cake. 3. Verfahren nach Anspruch 2, dadurch gekennzeichnet, daß in Abhänigkeit von den örtlichen Randbedingungen die Abscheideleistung des Verfahrens durch Art, Menge und Zusammensetzung des Adsorptionsmittels, Abgas/Additiv-Mengenverhältnis, Dicke des Filterkuchens und Reaktionstemperatur optimiert wird.3. The method according to claim 2, characterized in that, depending on the local boundary conditions, the separation efficiency of the method by type, amount and composition of the adsorbent, exhaust gas / additive ratio, thickness of the Filter cake and reaction temperature is optimized. Verfahren nach Anspruch 1, 2 und 3, dadurch gekennzeichnet, daß als Adsorptionsmittel Stoffe mit einer hohen Selektivität (z.B. Aktivkohle, Molekularsiebe, Natriumsulfid, Kalkhydrat) in unterschiedlichen Mengenverhältnissen eingesetzt werden können, daß zur Minimierung des Adsorptionsmittelverbrauchs und der anfallenden Reststoffmengen, das im Filter abgeschiedene Adsorptionsmittelgemisch im Kreislauf geführt und nur wegen der Ausschleusung der adsorbierten Schadstoffe geringfügig durch frisches Additiv ersetzt wird, daß die vom Rezirkulationskreislauf ausgeschleuste Teilmenge zur thermischen Zersetzung von polyzyklischen Kohlenwasserstoffen zu der Verbrennungsanlage geführt wird. A method according to claim 1, 2 and 3, characterized in that substances with a high selectivity (e.g. activated carbon, molecular sieves, sodium sulfide, hydrated lime) can be used as adsorbents in different proportions, that in order to minimize the adsorbent consumption and the accumulated residues, that in the filter separated adsorbent mixture in the circuit and only slightly replaced by fresh additive because of the removal of the adsorbed pollutants, that the part removed from the recirculation circuit is led to the thermal decomposition of polycyclic hydrocarbons to the incinerator.
PCT/EP1990/000921 1989-06-12 1990-06-12 Process for the separation of polycyclic hydrocarbons and heavy metals from waste gases Ceased WO1990015657A1 (en)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE19893919124 DE3919124A1 (en) 1989-06-12 1989-06-12 METHOD FOR SEPARATING POLYCYLCIC HYDROCARBONS AND HEAVY METALS FROM EXHAUST GASES
DEP3919124.9 1989-06-12

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WO1990015657A1 true WO1990015657A1 (en) 1990-12-27

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DE (1) DE3919124A1 (en)
WO (1) WO1990015657A1 (en)

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AU5859790A (en) 1991-01-08

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