选择催化还原（SCR）反应机理研究进展

doi:10.16085/j.issn.1000-6613.2018-1195

化工进展 ›› 2019, Vol. 38 ›› Issue (04): 1611-1623.DOI: 10.16085/j.issn.1000-6613.2018-1195

选择催化还原（SCR）反应机理研究进展

张道军¹(),马子然²,孙琦²,徐文强²,李永龙²,竹涛³,王宝冬²()

1. 北京化工大学化工资源有效利用国家重点实验室，北京100029
2. 北京低碳清洁能源研究所，北京 102211
3. 中国矿业大学（北京）化学与环境工程学院，北京 100083

收稿日期:2018-06-07 修回日期:2018-12-03 出版日期:2019-04-05 发布日期:2019-04-05
通讯作者: 王宝冬
作者简介:张道军（1989—），男，博士，主要研究方向为大气污染控制。E-mail: <email>zhangdaojun@nicenergy.com</email>。|王宝冬，教授级高级工程师，青年千人计划专家，主要研究方向为大气污染控制。E-mail: <email>wangbaodong@nicenergy.com</email>。
基金资助:
中组部青年千人启动经费-洁净煤（燃煤电厂）污染物控制(GB9300120001);北京低碳清洁能源研究所科技项目(CF9300171821)

Progress in the mechanism of selective catalytic reduction （SCR） reaction

Daojun ZHANG¹(),Ziran MA²,Qi SUN²,Wenqiang XU²,Yonglong LI²,Tao ZHU³,Baodong WANG²()

1. State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China
2. National Institute of Clean-and-Low-Carbon Energy，Beijing 102211，China
3. School of Chemical & Environmental Engineering，China University of Mining & Technology Beijing, Beijing 100083，China

Received:2018-06-07 Revised:2018-12-03 Online:2019-04-05 Published:2019-04-05
Contact: Baodong WANG

摘要/Abstract

摘要：

简述了NH₃和NO在催化剂表面吸附、转化活化和反应历程及H₂O和SO₂对以上反应行为的影响。分析表明，NH₃氧化脱氢进而与NO反应是决定NH₃反应性和最终产物的关键。NO以气态（Eley-Rideal机理）或硝基类物质等吸附态（Langmuir-Hinshelwood机理）形式参与选择催化还原（SCR）反应。提高催化剂酸性和氧化还原循环性能，利于NH₃和NO吸附和转化及相互间反应。高温时，H₂O影响轻微，而SO₂增强催化剂酸性，提高脱硝活性。低温时，H₂O和SO₂抑制NO吸附和转化活化，导致硫铵盐累积和活性位转变为硫酸盐使催化剂失活。因此，提高抗H₂O、抗SO₂性能是低温脱硝催化剂研发的重要方向。而发展在线升温等再生工艺以解决硝酸盐或含硫化合物导致的失活问题，对保障低温脱硝系统长期稳定运行具有重要意义。

关键词: 选择催化还原, 催化剂, 氨气, 氮氧化物, 吸附, 活化, 活性

Abstract:

In this work, adsorption, activation, and reactivity of NH₃ and NO on the selective catalytic reduction （SCR） catalysts and the effects of H₂O and SO₂ on the reaction behaviors of NH₃ and NO were reviewed. The analysis shows that the co-reaction between the H-abstraction products of the adsorbed NH₃ and the adsorbed NO species (or gas phase NO) is the key to determine the NH₃ reactivity and the final SCR product. The gas phase NO could react with the H-abstraction products of the adsorbed NH₃ directly (Eley-Rideal mechanism). In addition, a lot of conversion products, such as nitrites and nitrates species, could form after NO was adsorbed and activated on the catalyst surface. These species could also react with adsorbed NH₃ species (Langmuir-Hinshelwood mechanism). This is another important pathway for NO to participate in the SCR reaction, especially at low temperature. It is beneficial for the adsorption and conversion of NH₃ and NO to enhance the catalyst acidity and redox ability. The effects of H₂O and SO₂ on the catalyst are influenced by the temperature. At high temperature, the effect of H₂O on the catalyst is very little, while the catalyst acidity could be enhanced by SO₂, which enhance NH₃ adsorption. At low temperature, however, the adsorption and conversion of NO could be inhibited severely by H₂O and SO₂, especially the SO₂. The accumulation of ammonia sulphate and the conversion of active sites to sulphate could result in severe deactivation of the catalyst. Therefore, it is still a severe challenge to improve the H₂O and SO₂ resistance ability for developing low temperature SCR catalyst. It is of great significance to increase the catalyst temperature to decompose the nitrate and sulfate to regenerate the catalyst in operation.

Key words: selective catalytic reduction (SCR), catalyst, ammonia, nitrogen oxides, adsorption, activation, reactivity

中图分类号:

X511

张道军, 马子然, 孙琦, 徐文强, 李永龙, 竹涛, 王宝冬. 选择催化还原（SCR）反应机理研究进展[J]. 化工进展, 2019, 38(04): 1611-1623.

Daojun ZHANG, Ziran MA, Qi SUN, Wenqiang XU, Yonglong LI, Tao ZHU, Baodong WANG. Progress in the mechanism of selective catalytic reduction （SCR） reaction[J]. Chemical Industry and Engineering Progress, 2019, 38(04): 1611-1623.

图/表 8

图1 V2O5上Lewis酸性位向Br?nsted酸性位转化机理示意图[11]

图2 Tops?e等[9,21]提出的V2O5/TiO2催化剂上的SCR反应机理

图3 Liu等[18]提出的FeTiO x 催化剂上SCR反应机理示意图

图4 NH3脱氢程度对反应的影响

表1 催化剂表面吸附态NO存在形式及热稳定性[20]

吸附物种	峰位置/cm^-1	结构式	脱附或分解温度/K
亚硝酰基	1835	Mn ⁿ ⁺—N $?$ O ^δ ^-	323
桥联状硝基	1620/1220		423～573
“Ⅰ型”双齿状硝基类	1580/1220		473～573
“Ⅱ型”双齿状硝基类	1555/1290		573～698
线状亚硝基	1466/1075	M ⁿ ⁺—O—N $?$ O	323～473
单齿状亚硝基	1415/1322		323～473
桥联线状亚硝基	1230		323～523

表1 催化剂表面吸附态NO存在形式及热稳定性[20]

吸附物种	峰位置/cm^-1	结构式	脱附或分解温度/K
亚硝酰基	1835	Mn ⁿ ⁺—N $?$ O ^δ ^-	323
桥联状硝基	1620/1220		423～573
“Ⅰ型”双齿状硝基类	1580/1220		473～573
“Ⅱ型”双齿状硝基类	1555/1290		573～698
线状亚硝基	1466/1075	M ⁿ ⁺—O—N $?$ O	323～473
单齿状亚硝基	1415/1322		323～473
桥联线状亚硝基	1230		323～523

图5 Chen等[34]提出的NO在Ti0.9Mn0.05Fe0.05O2-δ催化剂表面反应机理示意图

图6 Jiang等[35]提出的NO在Mn基催化剂表面吸附和转化示意图

图7 Ruggeri等[44]提出的快速SCR反应机理示意图

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选择催化还原（SCR）反应机理研究进展

Progress in the mechanism of selective catalytic reduction （SCR） reaction

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