CN107118820B - Coal dearsenification method - Google Patents

Coal dearsenification method Download PDF

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Publication number
CN107118820B
CN107118820B CN201710395415.7A CN201710395415A CN107118820B CN 107118820 B CN107118820 B CN 107118820B CN 201710395415 A CN201710395415 A CN 201710395415A CN 107118820 B CN107118820 B CN 107118820B
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coal
arsenic
additive
chloride
slurry
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CN201710395415.7A
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CN107118820A (en
Inventor
孙文寿
郭远峰
张敬帅
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QINGDAO SAINUOWEIER INDUSTRIAL WATER TREATMENT Co.,Ltd.
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Qingdao University
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    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
    • C10L9/00—Treating solid fuels to improve their combustion
    • C10L9/02—Treating solid fuels to improve their combustion by chemical means
    • 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
    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/46—Removing components of defined structure
    • B01D53/48—Sulfur compounds
    • B01D53/50—Sulfur oxides
    • 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
    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
    • B01D53/77—Liquid phase processes
    • B01D53/78—Liquid phase processes with gas-liquid contact
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
    • C10L9/00—Treating solid fuels to improve their combustion
    • C10L9/10—Treating solid fuels to improve their combustion by using additives
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2258/00—Sources of waste gases
    • B01D2258/02—Other waste gases
    • B01D2258/0283—Flue gases
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
    • C10L2290/00—Fuel preparation or upgrading, processes or apparatus therefore, comprising specific process steps or apparatus units
    • C10L2290/22—Impregnation or immersion of a fuel component or a fuel as a whole

Abstract

The invention discloses a coal dearsenification method and an additive thereof, belonging to the technical field of coal and flue gas purification. The additive is at least one of aluminum chloride, ferric chloride, sodium chloride, magnesium chloride, calcium chloride, ferric sulfate and aluminum sulfate or a composite additive prepared according to a certain proportion, and is added into coal slurry to wash flue gas containing sulfur dioxide, wherein the sulfur dioxide leaches inorganic arsenic in coal, and simultaneously, the flue gas desulfurization is realized. The adopted additive can promote the leaching of inorganic arsenic in coal and/or accelerate the oxidation of trivalent arsenic in the leaching solution into pentavalent arsenic, thereby reducing the toxicity of arsenic and being beneficial to the subsequent treatment of the leached arsenic.

Description

Coal dearsenification method
Technical Field
The invention relates to a coal dearsenification method and an additive adopted by the coal dearsenification method, and belongs to the technical field of coal and flue gas purification.
Background
China mainly uses coal as energy. The coal contains harmful trace element arsenic, most of the arsenic in the coal can be released into the air in the coal combustion process, and the environment can be seriously damaged. Although arsenic can be concentrated on the surface of fly ash, and the emission of arsenic can be effectively reduced by dust removal, the arsenic in fly ash can cause serious harm to the environment if not properly treated.
Arsenic in coal includes inorganic arsenic, organic arsenic and the like, the inorganic arsenic is mainly used, the inorganic arsenic in the coal can be leached by nitric acid and the like, and the purpose of removing arsenic from the coal is achieved, but the method needs to consume acid. The common valence states of arsenic in the leaching solution are trivalent positive and pentavalent positive, the toxicity of the pentavalent positive arsenic is lower than that of the trivalent positive arsenic, and if the leached arsenic can be oxidized into pentavalent arsenic at the same time, the toxicity of the arsenic can be reduced, and the subsequent treatment of the leached arsenic is facilitated.
Disclosure of Invention
The invention aims to provide a method for removing arsenic from coal and an additive thereof. The method comprises the steps of crushing coal into coal powder, adding water and an additive to prepare slurry, contacting the coal slurry containing the additive with sulfur dioxide in flue gas in a spray tower or a bubbling reactor to perform mass transfer reaction, leaching inorganic arsenic in the coal by the sulfur dioxide, and simultaneously realizing flue gas desulfurization.
The technical scheme of the invention is as follows:
coal is crushed into coal powder with the grain size less than 600 mu m, water is added to prepare slurry, an additive is added into the slurry to wash flue gas containing sulfur dioxide, inorganic arsenic in the coal is leached into the solution, and the sulfur dioxide in the flue gas is simultaneously removed and oxidized into sulfate radicals.
The solid-liquid mass ratio of the coal powder to the water is generally 1: 80-3: 10, the pH value of the slurry is 1-3, and the temperature is 20-75 ℃.
Further, the preferable range of the pH value of the slurry in the dearsenifying process is 1.4-2.5.
The additive is at least one of aluminum chloride, ferric chloride, sodium chloride, magnesium chloride, calcium chloride, ferric sulfate and aluminum sulfate or a composite additive prepared according to a certain proportion.
If the leached arsenic is to be prepared into a pentavalent arsenic product or subjected to solidification treatment, at least one of aluminum chloride, ferric chloride, sodium chloride, magnesium chloride and calcium chloride is used as an additive, or a composite additive prepared from aluminum chloride, ferric chloride, sodium chloride, magnesium chloride, calcium chloride, ferric sulfate and aluminum sulfate is used, wherein the sum of mole fractions of aluminum chloride, ferric chloride, sodium chloride, magnesium chloride and calcium chloride in the composite additive is 0.2-1.
If the leached arsenic is to be made into a trivalent arsenic product, one of ferric sulfate and aluminum sulfate is used as an additive, or a mixed additive prepared from ferric sulfate and aluminum sulfate is used.
The additive is added into the coal slurry at one time or intermittently. The concentration of the additive in the liquid phase can be 1-15 mmol/L.
In the leaching process, the contact mass transfer reaction equipment of the flue gas and the coal slurry can be a spray tower, a bubble reactor and the like.
The invention has the advantages that:
the additives of aluminum chloride, ferric sulfate and aluminum sulfate adopted by the invention can promote the leaching of inorganic arsenic in coal, improve the leaching rate of arsenic, improve the removal rate of sulfur dioxide, and reduce the investment cost and the operation cost of equipment; the additives of sodium chloride, magnesium chloride, calcium chloride, ferric chloride and aluminum chloride can accelerate the oxidation of the leached trivalent arsenic into pentavalent arsenic, thereby reducing the toxicity of the arsenic and facilitating the subsequent treatment of the leached arsenic; the invention adopts the flue gas to leach the coal arsenic, uses waste to treat waste, and can realize flue gas desulfurization while dearsenizing the coal.
Detailed Description
The flue gas containing sulfur dioxide enters from the lower part of the absorption tower, the coal slurry containing the additive is sprayed from top to bottom to wash the flue gas flowing upwards in a countercurrent manner, and in the contact reaction process of the flue gas and the coal slurry, the sulfur dioxide in the flue gas leaches inorganic arsenic in coal, and the sulfur dioxide is also removed.
The gas fume is introduced into the bubbling reactor, and the gas fume and coal slurry containing additive are made to contact and transfer mass reaction in the bubbling reactor to reach dearsenifying and desulfurizing aim.
Example analyses were performed as follows:
example 1
The composite additive in the embodiment comprises ferric sulfate, aluminum sulfate, sodium chloride, aluminum chloride and ferric chloride, wherein the mass percentages of the ferric sulfate, the aluminum sulfate, the sodium chloride, the aluminum chloride and the ferric chloride in the composite additive are respectively 50%, 24%, 8% and 10%.
The solid-liquid mass ratio of coal to water in the high-arsenic coal slurry is 1: 10, the pH value of the slurry is 2, the temperature is 50 ℃, the concentration of the composite additive is 1550mg/L, the slurry is used for circularly washing flue gas containing sulfur dioxide, the leaching rate of inorganic arsenic in coal reaches 93%, pentavalent arsenic in the leaching solution accounts for 92% of total arsenic, and the desulfurization rate of the flue gas is 95%; under the same conditions, when no additive is used, the leaching rate of inorganic arsenic is 39%, the pentavalent arsenic in the leaching solution accounts for 14% of the total arsenic, and the flue gas desulfurization rate is 84%.
Example 2
The composite additive in the embodiment is composed of sodium chloride, aluminum chloride, magnesium chloride and calcium chloride, and the mass percentages of the sodium chloride, the aluminum chloride, the magnesium chloride and the calcium chloride in the composite additive are respectively 6%, 84%, 5% and 5%.
The solid-liquid mass ratio of coal to water in the high-arsenic coal slurry is 1: 20, the pH value of the slurry is 1.4, the temperature is 50 ℃, the concentration of the composite additive is 950mg/L, the slurry is used for circularly washing flue gas containing sulfur dioxide, the leaching rate of inorganic arsenic in coal reaches 97%, the pentavalent arsenic in the leaching solution accounts for 96% of total arsenic, and the desulfurization rate of the flue gas is 91%; under the same conditions, when no additive is used, the leaching rate of inorganic arsenic is 41%, the pentavalent arsenic in the leaching solution accounts for 16% of the total arsenic, and the flue gas desulfurization rate is 66%.
Example 3
The composite additive in the embodiment is composed of ferric sulfate, sodium chloride, ferric chloride, magnesium chloride and calcium chloride, and the mass percentages of the ferric sulfate, the sodium chloride, the ferric chloride, the magnesium chloride and the calcium chloride in the composite additive are respectively 30%, 5%, 60%, 3% and 2%.
The solid-liquid mass ratio of coal to water in the high-arsenic coal slurry is 1: 20, the pH value of the slurry is 1.4, the temperature is 50 ℃, the concentration of the composite additive is 1350mg/L, the slurry is used for circularly washing flue gas containing sulfur dioxide, the leaching rate of inorganic arsenic in coal can reach 96%, pentavalent arsenic in the leaching solution accounts for 93% of total arsenic, and the desulfurization rate of the flue gas is 90%; under the same condition, when no additive is used, the leaching rate of inorganic arsenic is 43 percent, the pentavalent arsenic in the leaching solution accounts for 14 percent of the total arsenic, and the flue gas desulfurization rate is 68 percent
Example 4
The composite additive in the embodiment consists of sodium chloride, magnesium chloride and calcium chloride, and the mass percentages of the sodium chloride, the magnesium chloride and the calcium chloride in the composite additive are respectively 68%, 22% and 10%.
The solid-liquid mass ratio of coal to water in the raw coal slurry is 1: 10, the pH value of the slurry is 2.1, the temperature is 50 ℃, the concentration of the composite additive is 1200mg/L, the composite additive is used for circularly washing the flue gas containing sulfur dioxide, and pentavalent arsenic in the leachate accounts for 92 percent of total arsenic; under the same conditions, when no additive is used, the pentavalent arsenic in the leaching solution accounts for 15 percent of the total arsenic.
Example 5
The composite additive in the embodiment consists of ferric chloride and aluminum chloride, and the mass percentages of the ferric chloride and the aluminum chloride in the composite additive are respectively 55% and 45%.
The solid-liquid mass ratio of coal to water in the raw coal slurry is 1: 20, the pH value of the slurry is 1.8, the temperature is 55 ℃, the concentration of the composite additive is 1200mg/L, the slurry is used for circularly washing flue gas containing sulfur dioxide, the leaching rate of inorganic arsenic in coal can reach 97%, the pentavalent arsenic in the leaching solution accounts for 97% of the total arsenic, and the desulfurization rate of the flue gas is 92%; under the same condition, when no additive is used, the leaching rate of inorganic arsenic is 42%, the pentavalent arsenic in the leaching solution accounts for 17% of the total arsenic, and the flue gas desulfurization rate is 70%.
Example 6
The composite additive in the embodiment consists of ferric sulfate and aluminum chloride, and the mass percentages of the ferric sulfate and the aluminum chloride in the composite additive are respectively 60% and 40%.
The solid-liquid mass ratio of coal to water in the coal slurry is 1: 10, the pH value of the slurry is 2, the temperature is 50 ℃, the concentration of the composite additive is 2000mg/L, the slurry is used for circularly washing the flue gas containing sulfur dioxide, the leaching rate of inorganic arsenic in coal can reach 95%, pentavalent arsenic in the leaching solution accounts for 94% of total arsenic, and the desulfurization rate of the flue gas is 94%; under the same conditions, when no additive is used, the leaching rate of inorganic arsenic is 44%, the pentavalent arsenic in the leaching solution accounts for 10% of the total arsenic, and the flue gas desulfurization rate is 81%.
Example 7
The composite additive in the embodiment consists of aluminum sulfate and aluminum chloride, and the mass percentages of the aluminum sulfate and the aluminum chloride in the composite additive are respectively 51% and 49%.
The solid-liquid mass ratio of coal to water in the high-arsenic coal slurry is 1: 10, the pH value of the slurry is 2.1, the temperature is 50 ℃, the concentration of the composite additive is 1350mg/L, the slurry is used for circularly washing flue gas containing sulfur dioxide, the leaching rate of inorganic arsenic in coal can reach 93 percent, pentavalent arsenic in the leaching solution accounts for 92 percent of total arsenic, and the desulfurization rate of the flue gas is 95 percent; under the same condition, when the additive is not used, the leaching rate of inorganic arsenic in the coal is 31 percent, the pentavalent arsenic in the leaching solution accounts for 15 percent of the total arsenic, and the flue gas desulfurization rate is 82 percent.
Example 8
The composite additive in the embodiment consists of 75% and 25% of aluminum chloride and sodium chloride in percentage by mass respectively.
The solid-liquid mass ratio of coal to water in the raw coal slurry is 1: 10, the pH value of the slurry is 2.2, the temperature is 50 ℃, the concentration of the composite additive is 710mg/L, the slurry is used for circularly washing flue gas containing sulfur dioxide, the leaching rate of inorganic arsenic in coal can reach 91 percent, pentavalent arsenic in the leaching solution accounts for 92 percent of total arsenic, and the desulfurization rate of the flue gas is 93 percent; under the same condition, when the additive is not used, the leaching rate of inorganic arsenic in the coal is 28%, the pentavalent arsenic in the leaching solution accounts for 13% of the total arsenic, and the flue gas desulfurization rate is 84%.
Example 9
The compound additive in the embodiment consists of aluminum sulfate and sodium chloride, and the mass percentages of the aluminum sulfate and the sodium chloride in the compound additive are respectively 88% and 12%.
The solid-liquid mass ratio of coal to water in the high-arsenic coal slurry is 1: 10, the pH value of the slurry is 2.2, the temperature is 50 ℃, the concentration of the composite additive is 1540mg/L, the slurry is used for circularly washing flue gas containing sulfur dioxide, the leaching rate of inorganic arsenic in coal can reach 91 percent, pentavalent arsenic in the leaching solution accounts for 88 percent of total arsenic, and the desulfurization rate of the flue gas is 94 percent; under the same condition, when the additive is not used, the leaching rate of inorganic arsenic in the coal is 28%, the pentavalent arsenic in the leaching solution accounts for 13% of the total arsenic, and the flue gas desulfurization rate is 84%.
Example 10
The composite additive in the embodiment consists of sodium chloride and calcium chloride, and the mass percentages of the sodium chloride and the calcium chloride in the composite additive are respectively 80% and 20%.
The solid-liquid mass ratio of coal to water in the raw coal slurry is 1: 10, the pH value of the slurry is 1.4, the temperature is 55 ℃, the concentration of the composite additive is 1200mg/L, the composite additive is used for circularly washing the flue gas containing sulfur dioxide, and pentavalent arsenic in the leachate accounts for 98 percent of the total arsenic; under the same conditions, when no additive is used, the pentavalent arsenic in the leachate accounts for 17 percent of the total arsenic.
Example 11
The composite additive in the embodiment consists of aluminum sulfate and ferric sulfate, and the mass percentages of the aluminum sulfate and the ferric sulfate in the composite additive are 63% and 37%, respectively.
The solid-liquid mass ratio of coal to water in the coal slurry is 1: 10, the pH value of the slurry is 1.7, the temperature is 53 ℃, the concentration of the composite additive is 2200mg/L, the slurry is used for circularly washing the flue gas containing sulfur dioxide, the leaching rate of inorganic arsenic in coal can reach 95%, and the desulfurization rate of the flue gas is 91%; under the same conditions, when the additive is not used, the leaching rate of inorganic arsenic in the coal is 35%, and the flue gas desulfurization rate is 70%.
Example 12
The additive in this example is aluminum chloride.
The solid-liquid mass ratio of coal to water in the coal slurry is 1: 10, the pH value of the slurry is 2, the temperature is 55 ℃, the concentration of aluminum chloride is 1100mg/L, the slurry is used for circularly washing the flue gas containing sulfur dioxide, the leaching rate of inorganic arsenic in coal can reach 93 percent, pentavalent arsenic in the leaching solution accounts for 95 percent of total arsenic, and the desulfurization rate of the flue gas is 93 percent; under the same condition, when the additive is not used, the leaching rate of inorganic arsenic in the coal is 30%, the pentavalent arsenic in the leaching solution accounts for 19% of the total arsenic, and the flue gas desulfurization rate is 78%.

Claims (4)

1. A coal dearsenification method is characterized in that: crushing coal into coal powder with the particle size of less than 600 mu m, adding water and an additive to prepare slurry, wherein the solid-liquid mass ratio of the coal to the water is 1: 80-3: 10, the pH value of the slurry is 1-3, the temperature is 20-75 ℃, the coal slurry containing the additive is contacted with sulfur dioxide in flue gas in a spray tower or a bubbling reactor to carry out mass transfer reaction, the sulfur dioxide leaches inorganic arsenic in the coal, and the flue gas desulfurization is realized at the same time; the adopted additive is one of aluminum chloride, ferric chloride, sodium chloride, magnesium chloride and calcium chloride or a composite additive prepared according to a certain proportion, the sodium chloride, the magnesium chloride and the calcium chloride in the adopted additive can accelerate the oxidation of the leached trivalent arsenic into pentavalent arsenic, and the aluminum chloride and the ferric chloride can promote the leaching of inorganic arsenic in coal and accelerate the oxidation of the trivalent arsenic in the leaching solution into pentavalent arsenic, so that the toxicity of the arsenic is reduced, and the subsequent treatment of the leached arsenic is facilitated.
2. The coal dearsenification method according to claim 1, wherein: the concentration of the additive in the liquid phase is 1-15 mmol/L.
3. The coal dearsenification method according to claim 1, wherein: the pH value of the slurry in the arsenic removal process is 1.4-2.5.
4. The coal dearsenification method according to claim 1, wherein: the additive is added into the coal slurry at one time or intermittently.
CN201710395415.7A 2017-05-19 2017-05-19 Coal dearsenification method Active CN107118820B (en)

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CN108939852A (en) * 2018-07-27 2018-12-07 昆明冶金研究院 A kind of method that tin smelts the arsenic removal of arsenical fume washing, purifying
CN109266418A (en) * 2018-09-30 2019-01-25 青岛大学 A method of arsenic in coal being leached under ultraviolet light using flue gas
CN113832347B (en) * 2021-09-18 2023-04-11 青岛赛诺威尔工业水处理有限公司 Method for enhancing arsenic leaching of coal by using organic additive

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CN103071383B (en) * 2013-01-19 2015-10-21 青岛大学 Reinforced by additive coal slurry method flue gas desulfurization technique

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