CN105561774B - A kind of preposition SCO reinforcings denitrating flue gas demercuration system in coal-burning power plant - Google Patents

A kind of preposition SCO reinforcings denitrating flue gas demercuration system in coal-burning power plant Download PDF

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CN105561774B
CN105561774B CN201510936577.8A CN201510936577A CN105561774B CN 105561774 B CN105561774 B CN 105561774B CN 201510936577 A CN201510936577 A CN 201510936577A CN 105561774 B CN105561774 B CN 105561774B
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sco
catalyst
coal
flue gas
units
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CN201510936577.8A
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CN105561774A (en
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胡将军
李鸿鹄
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武汉大学
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    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01DSEPARATION
    • B01D53/00Separation 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
    • B01D53/34Chemical or biological purification of waste gases
    • B01D53/74General processes for purification of waste gases; Apparatus or devices specially adapted therefor
    • B01D53/86Catalytic processes
    • B01D53/8637Simultaneously removing sulfur oxides and nitrogen oxides
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01DSEPARATION
    • B01D53/00Separation 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
    • B01D53/34Chemical or biological purification of waste gases
    • B01D53/74General processes for purification of waste gases; Apparatus or devices specially adapted therefor
    • B01D53/86Catalytic processes
    • B01D53/8665Removing heavy metals or compounds thereof, e.g. mercury
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01DSEPARATION
    • B01D2255/00Catalysts
    • B01D2255/20Metals or compounds thereof
    • B01D2255/207Transition metals
    • B01D2255/2073Manganese
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01DSEPARATION
    • B01D2255/00Catalysts
    • B01D2255/20Metals or compounds thereof
    • B01D2255/207Transition metals
    • B01D2255/20746Cobalt
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01DSEPARATION
    • B01D2258/00Sources of waste gases
    • B01D2258/02Other waste gases
    • B01D2258/0283Flue gases

Abstract

The present invention relates to a kind of preposition SCO in coal-burning power plant to strengthen denitrating flue gas demercuration technology, by advance by the NO and Hg in flue gas0It is oxidized to NO2And Hg2+, subsequently into SCR, to reach the purpose of NO_x Reduction by Effective demercuration.The catalyst that SCO units use is Co Mn Ti Ce catalyst series, and active component is one or both of cobalt/cobalt oxide or Mn oxide, and adjuvant component W, catalyst carrier is that Ce adulterates TiO2.Hg can be achieved under the premise of to coal-burning power plant's existing facility need not excessively change in the present invention0Efficient oxidation removing, Hg0Oxidation efficiency will not by ammonification process be influenced.Meanwhile with O2With NO as Hg0Oxidant broken away from the dependence to HCl, additional component need not be added into flue gas, set mercury oxidation removal efficiency can be realized;And SCR unit inlet 50%NO is converted by NO2 using preposition SCO techniques and is remarkably improved SCR process reaction efficiency, catalyst raw material of the present invention is easy to get, and technical matters is easy to implement, is conducive to industrial applications.

Description

A kind of preposition SCO reinforcings denitrating flue gas demercuration system in coal-burning power plant

Technical field

Strengthen denitrating flue gas the invention belongs to Air Pollution Control field more particularly to a kind of preposition SCO in coal-burning power plant to take off Mercury technology.

Background technology

With the continuous development of Chinese society economy and stepping up for living standards of the people, adjoint problem of environmental pollution Also it increasingly highlights.Energy resource structure of the China based on fire coal will not change in a short time, nitrogen oxides, the oxysulfide thus brought Wait flue gases problem of environmental pollution by getting worse.Simultaneously to meet the construction demand of conservation culture and scientific development, country is to big The governance standard of gas environmental contaminants is increasingly stringenter, newest revision《Fossil-fuel power plant atmospheric pollutant emission standard》In 2012 Year formal implementation, every cubic metre of mercurous milligram number has been given clearly limiting, Mercury Emissions from Coal-Fired Boilers contamination control gesture exists for the first time It must go.Activated carbon spraying technique and precious metal oxide catalyst all have a preferable demercuration efficiency, but due to its it is high at Originally practice is limited.Conventional WFGD system can remove most pollutants in flue gas, but due to its low aqueous solubility, The characteristics such as volatile, Hg0And NO capture rates are very low, cannot meet discharge standard.Therefore, practicable mercury and nitrogen oxygen are developed Compound control technology has become one of the hot issue of field of environment protection research instantly.

Studies have shown that SCR catalyst is to Hg0There are certain oxidation, many scholars have carried out numerous studies according to this And it is prepared for various modifieds and synchronizes denitration demercuration SCR catalyst.However, all kinds of SCR catalysts are to Hg0Oxidation efficiency in It is not fully up to expectations during strip part and field experiment.There are two this quality factors for limiting its demercuration efficiency:First, NH3It is right Hg0There are competitive relation, a large amount of NH of SCR processes3Penetrating can seriously inhibit Hg0It is reacted with the solid gas interface of SCR catalyst, from And lead to the reduction of oxidation efficiency;Secondly:SCR processes are to Hg0Oxidation efficiency heavy dependence flue gas in HCl, however China Coal-fired Cl contents want much lower compared to other countries, artificially to SCR processes add HCl come improve mercury oxidation efficiency be clearly not Economical.

On the other hand, SCR techniques denitration efficiency in theory does not have a upper limit, but during practice primary concern is that Cost problem.How while improving SCR technique denitration efficiencies, it is also problem to be solved instantly to reduce its operating cost One of.Experimental study shows as NO and NO2Ratio is about 1:When 1, denitration reaction efficiency reaches highest.In coal-fired flue-gas NO contents are 90% or more, therefore the NO for controlling SCR inlet 50% is converted into NO2It will be greatly facilitated the promotion of SCR efficiency, from And the usage amount of SCR catalyst can be reduced to reduce cost.In conclusion starting with from the angle of selective catalytic oxidation, fill Divide the self performance and flue gas condition using catalyst, catalytic oxidation NO and Hg are synchronized using preposition SCO technologies0, subsequently into The participation reaction of SCR processes, will effectively solve above-mentioned problem, combine the exploitation of removing new technology to flue gas pollutant and with tool It is significant.

Invention content

In order to overcome disadvantage of the existing technology, the purpose of the present invention is to provide a kind of preposition SCO in coal-burning power plant is strong Change denitration demercuration technology, by advance by the NO and Hg in flue gas0It is oxidized to NO2And Hg2+, NO is restored subsequently into SCR processes2、 NO is N2, Hg2+It is then removed by facilities such as dedusters, to reach the purpose of NO_x Reduction by Effective demercuration.

To achieve the goals above, the present invention uses following technical scheme:

A kind of preposition SCO reinforcings denitrating flue gas demercuration system in coal-burning power plant, includes the SCR unit being connect with coal-burning boiler, It is characterized in that:SCO units are provided between coal-burning boiler and SCR unit.

The SCO units include vertical, the channel that multiple row is equidistant being made of catalyst, and the catalyst is Co-Mn- Ti-Ce catalyst series.

The SCO cell operations temperature is 300~350 DEG C.

The Co-Mn-Ti-Ce catalyst series include active component, carrier and auxiliary agent;The active component is cobalt oxide One or both of with manganese oxide, the carrier is that Ce adulterates TiO2, TiO2For Detitanium-ore-type;The adjuvant component is oxidation Tungsten.

In the Co-Mn-Ti-Ce catalyst series, the mass percent of active component is 5~10%, wherein cobalt oxide The mass percent for accounting for catalyst is 0%~5%, and the mass percent that manganese oxide accounts for catalyst is 0%~5%;The auxiliary agent Mass percent be 3%~5%;Surplus is carrier, and the mass percent of cerium oxide is 10%~20% in the carrier.

The SCO units are 45%~50%, SCO units pair to the oxygenation efficiency of NO by air speed adjusting control SCO units Hg0Oxidation efficiency be not less than 80%.

The air speed is adjusted, and arranges that the number of plies and arrangement adjust SCO unit air speeds, control by changing SCO catalyst The oxygenation efficiency of SCO units NO processed is 45%~50%.SCO units are to Hg0Oxidation efficiency be not less than 80%.

The experiment installation of SCO catalyst is carried out first, and the initial number of plies of installing is two layers.

If the oxygenation efficiency of SCO units NO is 45%~50%, meet the requirements.

If the oxygenation efficiency of SCO units NO is less than 45%, it can increase and be installed for three layers, or using two layers of installation, but fit As the direct percent of pass δ of flue gas for reducing SCO units.

If the oxygenation efficiency of SCO units NO is higher than 50%, one layer of installation can be reduced to;Or using two layers of installation, but fit As the direct percent of pass δ of flue gas for improving SCO units.

Define the direct percent of pass δ of flue gas:

V is SCO catalyst space volumes, and V is the flue volume corresponding to SCO catalyst space volumes.

A kind of embodiment that the preposition SCO in coal-burning power plant strengthens denitration demercuration technology catalyst is as follows:

Suitably boiler flue is transformed, extends SCR unit front end smoke canal length, to arrange SCO units.

Catalyst of the present invention is used for NO and Hg in catalysis oxidation flue gas0Reaction process be:In 300~350 DEG C of reaction At a temperature of, original O in flue gas2With NO as oxygen donor, catalytic oxidation is completed using catalyst of the present invention, reaction equation is such as Under:

2NO+O2→2NO2 2Hg+O2→2HgO 2Hg+2NO→2HgO+N2

SCR unit, NO and NO2Ratio is 1:1 NO_x Reduction by Effective reaction process is:

2NH3+NO+NO2→2N2+3H2O

The oxide of active component Co and Mn used in catalyst of the present invention are to Hg0There is preferable catalysis oxidation with NO Effect, especially to Hg0Oxidation efficiency reach as high as 95% or more, have both to NO have certain catalytic oxidation effect, Oxygenation efficiency to NO is 35%~65%.Ce containing a small amount of W components adulterates TiO2Stablize as carrier structure, has preferable anti- Sulphur performance, the evenly dispersed load of active component, while Ce can improve the Oxygen storage capacity of catalyst, accelerate catalyst surface active The generation and migration of oxygen, and then promote the progress of catalytic oxidation.

The present invention passes through in advance by the NO and Hg in flue gas0It is oxidized to NO2And Hg2+, NO is restored subsequently into SCR processes2、 NO is N2, Hg2+It is then removed by facilities such as dedusters, to reach the purpose of NO_x Reduction by Effective demercuration.The catalyst that SCO units use is Co-Mn-Ti-Ce catalyst series, active component be one or both of cobalt/cobalt oxide or Mn oxide, adjuvant component W, Catalyst carrier is that Ce adulterates TiO2.The invention discloses the formula of the catalyst and the embodiments of technology, compared to original Hg can be achieved under the premise of to coal-burning power plant's existing facility need not excessively change in technology0Efficient oxidation removing, Hg0 Oxidation efficiency will not by ammonification process be influenced.Meanwhile with O2With NO as Hg0Oxidant broken away to HCl according to Rely, additional component need not be added into flue gas, set mercury oxidation removal efficiency can be realized.Moreover, using preposition SCO works Skill converts SCR unit inlet 50%NO to NO2It is remarkably improved SCR process reaction efficiency.

Compared with prior art, the present invention has following significant advantage:

(1) this technology uses preposition SCO techniques combination SCR unit, need not carried out to coal-burning power plant's existing facility Hg is realized under the premise of more changes0Efficient oxidation removing, Hg0Oxidation efficiency will not by ammonification process be influenced.Meanwhile With O2With NO as Hg0Oxidant broken away from the dependence to HCl, additional component need not be added into flue gas and can be realized both Fixed mercury oxidation removal efficiency.

(2) SCR unit inlet 50%NO is converted by NO using preposition SCO techniques2It is remarkably improved SCR process reactions Efficiency reaches set denitration efficiency so as to reduce SCR catalyst usage amount, controls process costs.

(3) catalyst raw material of the present invention is easy to get, and technical matters is easy to implement, is conducive to industrial applications.

Description of the drawings

Fig. 1 is schematic structural view of the invention;

Fig. 2, the direct percent of pass δ of flue gas illustrate figure.

Specific implementation mode

Following example to invention elaborate, the embodiment provided be the technical scheme is that under the premise of Implemented, but protection scope of the present invention is not limited to following embodiments.

Embodiment 1

Preposition SCO is carried out in certain unit coal-powder boiler coal-burning power plant and strengthens the experiment of denitration demercuration technical testing, and SCR unit is quotient Industry V-W-Ti catalyst, original denitration efficiency are 85%.Measure a concentration of 25.6ug/m of SCO unit entrance mercury3, NO contents are 0.1%, C(NO)/C(NOX)=0.95, oxygen content 4.6%.Used SCO catalyst cobalt oxide accounts for the quality percentage of catalyst Number is 5%, and the mass percent that tungsten oxide accounts for catalyst is 3%, and the mass percent that cerium oxide accounts for catalyst carrier is 10%, Arrange that temperature is 300 DEG C.Pre-installation experiment is carried out, SCO catalyst uses rebuilding, true empty-running speed 3500h-1, flue gas is straight It is 0% to meet percent of pass δ, and experiment measures SCO units Hg0Oxygenation efficiency is that 96%, NO oxygenation efficiency is 47%, meets given requirements.Through After crossing SCR unit and dust removing units, Hg removal efficiencies are that 98%, NO removal efficiencies are 93%.

Embodiment 2

Preposition SCO is carried out in certain unit coal-powder boiler coal-burning power plant and strengthens the experiment of denitration demercuration technical testing, and SCR unit is quotient Industry V-W-Ti catalyst, original denitration efficiency are 83%.Measure a concentration of 19.6ug/m of SCO unit entrance mercury3, NO contents are 0.15%, C(NO)/C(NOX)=0.98, oxygen content 5%.Used SCO catalyst manganese oxide accounts for the quality percentage of catalyst Number is 5%, and the mass percent that tungsten oxide accounts for catalyst is 5%, and the mass percent that cerium oxide accounts for catalyst carrier is 20%, Arrange that temperature is 350 DEG C.Pre-installation experiment is carried out, SCO catalyst uses rebuilding, and the direct percent of pass δ of flue gas is 0%, real Border air speed is 3900h-1, measure SCO units Hg0Oxygenation efficiency is that 97%, NO oxygenation efficiency is 36%.SCO catalyst elements are used instead Three layer arrangements, SCO units Hg0Oxygenation efficiency is that 98%, NO oxygenation efficiency is 45%.After SCR unit and dust removing units, Hg removings Efficiency is that 99%, NO removal efficiencies are 89%.

Embodiment 3

Preposition SCO is carried out in certain unit coal-powder boiler coal-burning power plant and strengthens the experiment of denitration demercuration technical testing, and SCR unit is quotient Industry V-W-Ti catalyst, original denitration efficiency are 87%.Measure a concentration of 22.6ug/m of SCO unit entrance mercury3, NO contents are 0.15%, C(NO)/C(NOX)=0.92, oxygen content 5.5%.Used SCO catalyst manganese oxide accounts for the quality hundred of catalyst Score is 2.5%, and the mass percent that cobalt oxide accounts for catalyst is 2.5%, and the mass percent that tungsten oxide accounts for catalyst is 4%, the mass percent that cerium oxide accounts for catalyst carrier is 15%, and arrangement temperature is 325 DEG C.Pre-installation experiment is carried out, SCO is urged It is 0% that agent, which uses rebuilding, the direct percent of pass δ of flue gas, true empty-running speed 3100h-1.Measure SCO units Hg0Oxygenation efficiency is 96%, NO oxygenation efficiency are 58%.Use SCO catalyst elements instead single layer arrangement, SCO units Hg0Oxygenation efficiency is 82%, NO oxidations Rate is 46%, and after SCR unit and dust removing units, Hg removal efficiencies are that 86%, NO removal efficiencies are 94%.

Embodiment 4

Preposition SCO is carried out in certain unit coal-powder boiler coal-burning power plant and strengthens the experiment of denitration demercuration technical testing, and SCR unit is quotient Industry V-W-Ti catalyst, original denitration efficiency are 87%.Measure a concentration of 21.6ug/m of SCO unit entrance mercury3, NO contents are 0.09%, C(NO)/C(NOX)=0.95, oxygen content 5%.Used SCO catalyst cobalt oxide accounts for the quality percentage of catalyst Number is 5%, and the mass percent that manganese oxide accounts for catalyst is 5%, and the mass percent that tungsten oxide accounts for catalyst is 3%, oxidation The mass percent that cerium accounts for catalyst carrier is 10%, and arrangement temperature is 300 DEG C.Pre-installation experiment is carried out, SCO catalyst uses Rebuilding, true empty-running speed 3300h-1.Measure SCO units Hg0Oxygenation efficiency is that 97%, NO oxygenation efficiency is 54%.SCO is reduced to urge Agent size, the direct percent of pass δ of control flue gas is 5%, measures SCO units Hg0Oxygenation efficiency is that 91%, NO oxygenation efficiency is 46%. After SCR unit and dust removing units, Hg removal efficiencies are that 93%, NO removal efficiencies are 94%.

Embodiment 5

Preposition SCO is carried out in certain unit coal-powder boiler coal-burning power plant and strengthens the experiment of denitration demercuration technical testing, and SCR unit is quotient Industry V-W-Ti catalyst, original denitration efficiency are 84%.Measure a concentration of 29.6ug/m of SCO unit entrance mercury3, NO contents are 0.1%, C(NO)/C(NOX)=0.93, oxygen content 4.5%.Used SCO catalyst manganese oxide accounts for the quality percentage of catalyst Number is 2.5%, and the mass percent that tungsten oxide accounts for catalyst is 4%, and the mass percent that cerium oxide accounts for catalyst carrier is 15%, arrangement temperature is 325 DEG C.Pre-installation experiment is carried out, SCO catalyst is using rebuilding, the direct percent of pass δ of flue gas 0%, true empty-running speed 3100h-1.Measure SCO units Hg0Oxygenation efficiency is that 92%, NO oxygenation efficiency is 45%, meets given requirements. After SCR unit and dust removing units, Hg removal efficiencies are that 95%, NO removal efficiencies are 89%.

Claims (2)

  1. Include the SCR units being connect with coal-burning boiler 1. a kind of preposition SCO in coal-burning power plant strengthens denitrating flue gas demercuration system, It is characterized in that:SCO units are provided between coal-burning boiler and SCR units;The SCO units include being made of catalyst Vertical, channel that multiple row is equidistant, the catalyst is Co-Mn-Ti-Ce catalyst series;The SCO cell operations temperature is 300~350 DEG C;The Co-Mn-Ti-Ce catalyst series include active component, carrier and auxiliary agent;The active component is oxygen Change one or both of cobalt and manganese oxide, the carrier is that Ce adulterates TiO2, TiO2For Detitanium-ore-type;The adjuvant component is Tungsten oxide;In the Co-Mn-Ti-Ce catalyst series, the mass percent of active component is 5~10%, and wherein cobalt oxide accounts for The mass percent of catalyst is 0%~5%, and the mass percent that manganese oxide accounts for catalyst is 0%~5%;The quality of the auxiliary agent Percentage is 3%~5%;Surplus is carrier, and the mass percent of cerium oxide is 10%~20% in the carrier.
  2. 2. the preposition SCO in coal-burning power plant as described in claim 1 strengthens denitrating flue gas demercuration system, it is characterised in that:The SCO Unit is 45%~50%, SCO units to Hg to the oxygenation efficiency of NO by air speed adjusting control SCO units0Oxidation efficiency it is not low In 80%.
CN201510936577.8A 2015-12-15 2015-12-15 A kind of preposition SCO reinforcings denitrating flue gas demercuration system in coal-burning power plant CN105561774B (en)

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CN106311291A (en) * 2016-09-07 2017-01-11 武汉大学 Composite catalyst based on denitration and demercuration reinforcing function of prepositive SCO smoke of coal-fired power plant and preparation method thereof
CN107362807B (en) * 2017-07-31 2020-09-22 华南理工大学 Mn/Co-based low-temperature SCO catalyst and preparation method thereof
CN109046326A (en) * 2018-08-29 2018-12-21 香港大学 A kind of vacuum ultraviolet light catalytic purifying material and its preparation method and application

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CN102527205A (en) * 2012-01-09 2012-07-04 广东电网公司电力科学研究院 Method and system for simultaneously removing sulfur, niter and mercury from smoke based on catalytic oxidation
CN104162349A (en) * 2014-07-23 2014-11-26 浙江大学 Method for inhibiting low-temperature denitration catalyst poisoning caused by SO2
CN104289227A (en) * 2014-09-25 2015-01-21 哈尔滨工业大学深圳研究生院 Mn, Co, Ce and Ti four-component NH3-SCR supported catalyst for low-temperature flue gas denitrification

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CN104162349A (en) * 2014-07-23 2014-11-26 浙江大学 Method for inhibiting low-temperature denitration catalyst poisoning caused by SO2
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