炭基材料负载型低温NH3-SCR脱硝催化剂的研究进展

doi:10.16085/j.issn.1000-6613.2018-1390

化工进展 ›› 2019, Vol. 38 ›› Issue (05): 2329-2338.DOI: 10.16085/j.issn.1000-6613.2018-1390

炭基材料负载型低温NH₃-SCR脱硝催化剂的研究进展

顾甜¹(),高凤雨^1,²,唐晓龙^1,²(),易红宏^1,²,张润草¹,王雨禾¹

1. 北京科技大学能源与环境工程学院，北京 100083
2. 工业典型污染物资源化处理北京市重点实验室，北京 100083

收稿日期:2018-07-06 修回日期:2018-11-22 出版日期:2019-05-05 发布日期:2019-05-05
通讯作者: 唐晓龙
作者简介:<named-content content-type="corresp-name">顾甜</named-content>（1995—），女，硕士研究生，研究方向为环境污染控制与治理、环境功能材料等。E-mail：<email>gutianzp@163.com</email>。|唐晓龙，教授，博士生导师，研究方向为环境污染控制与治理、环境功能材料等。E-mail：<email>txiaolong@126.com</email>。
基金资助:
国家重点研发计划重点专项(2017YFC0210303);国家自然科学基金(U1660109、21806009);中国博士后基金(2018M631344)

Research progress on carbon-based material supported catalysts for the selective catalytic reduction of NO _x by NH₃ at low temperature

Tian GU¹(),Fengyu GAO^1,²,Xiaolong TANG^1,²(),Honghong YI^1,²,Runcao ZHANG¹,Yuhe WANG¹

1. School of Energy and Environmental Engineering，University of Science and Technology Beijing，Beijing 100083，China
2. Beijing Key Laboratory of Resource-oriented Treatment of Industrial Pollutants，Beijing 100083，China

Received:2018-07-06 Revised:2018-11-22 Online:2019-05-05 Published:2019-05-05
Contact: Xiaolong TANG

摘要/Abstract

摘要：

氮氧化物（NO _x ）是主要的大气污染物之一，对人体健康和生态环境造成了严重危害。低温选择性催化还原（SCR）技术是近年来烟气脱硝领域的主要研究方向。炭基材料具有较大的比表面积、发达的孔隙结构等特点，在SCR脱硝方面被广泛用作催化剂载体。本文综述了炭基材料包括活性炭（焦）、活性炭纤维、碳纳米管、石墨烯及碳包覆负载型催化剂在低温NH₃-SCR脱硝领域的研究成果与进展，阐述了表面官能团、反应条件及稀土元素等因素对炭基材料负载型催化剂脱硝性能的影响，并且讨论了炭基材料负载型催化剂的催化反应机理。指出采用多种手段改性催化剂，优化其中低温脱硝性能与稳定性，深入探究催化剂表面反应物种的吸附-活化行为和催化反应路径是炭基材料负载型低温NH₃-SCR催化剂研究的重点。

关键词: 环境, 选择催化还原, 脱硝, 炭基材料, 催化剂, 载体

Abstract:

Nitrogen oxides (NO _x ) are one class of the major air pollutants, which has brought serious problems to human health and ecological environment. Low temperature selective catalytic reduction (SCR) technology is the main research direction of flue gas denitrification in recent years. Carbon-based materials have been extensively studied as catalyst carriers in SCR field because of their large specific surface area, porous structure and many other characteristics. The researches about the carbon-based materials including activated carbon (coke), activated carbon fiber, carbon nanotubes, graphene, and about the carbon coated catalysts in the field of low-temperature ammonia selective catalytic reduction (NH₃-SCR) denitrification are reviewed. The effects of surface functional groups, reaction conditions and rare earth elements on the denitration performance of carbon-based supported catalysts are described. The catalytic reaction mechanism of carbon-based materials is also discussed. The future research focuses of the carbon-based SCR catalysts should be placed on modifying them by various methods, optimizing the denitrification performance and stability under moderate and low temperature conditions and further exploring the adsorption-activation behavior and catalytic pathway of the reaction species on the catalyst surface.

Key words: environment, selective catalytic reduction, denitrification, carbon-based materials, catalyst, support

中图分类号:

TQ426.99

顾甜, 高凤雨, 唐晓龙, 易红宏, 张润草, 王雨禾. 炭基材料负载型低温NH₃-SCR脱硝催化剂的研究进展[J]. 化工进展, 2019, 38(05): 2329-2338.

Tian GU, Fengyu GAO, Xiaolong TANG, Honghong YI, Runcao ZHANG, Yuhe WANG. Research progress on carbon-based material supported catalysts for the selective catalytic reduction of NO _x by NH₃ at low temperature[J]. Chemical Industry and Engineering Progress, 2019, 38(05): 2329-2338.

图/表 5

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催化剂（质量分数）	制备方法	反应条件	NO转化率/%	参考文献
5% V₂O₅/ACF	等体积浸渍法 (500℃/8h)	[NO]=[NH₃]=600μL/L，[O₂]=5%， Ar to balance，GHSV=2000h^-1	96(180℃)	[20]
10% Fe₂O₃/ACF	浸渍法(300℃/5h)	[NO]=[NH₃]=200μL/L，[O₂]=10.5%，[H₂O]= 8%， N₂to balance，Q/W=200mL·min^-1·g^-1	约38(150℃)	[21]
10% Co₂O₃/ACF			约38 (150℃)
10% Mn₂O₃/ACF			90 (150℃)
9% CeO₂/ACF	浸渍法(350℃/6h)	[NO]=[NH₃]=1000μL/L，[O₂]=5%， Ar to balance，GHSV=11000h^-1	93.96(180℃)	[19]
10% CeO₂/ACF	浸渍法(360℃/2h)	[NO]=1000μL/L，[NH₃]=1100μL/L，[O₂]=5%， N₂to balance，GHSV=5000h^-1	80～90 (200～300℃)	[22]
20% La₂O₃/ACF	浸渍法(360℃/2h)	[NO]=1000μL/L，[NH₃]=1100μL/L，[O₂]=5%， N₂to balance，GHSV=5000h^-1	55～85 (200～300℃)	[22]
12% MnO _x -CeO _x /ACF_N	等体积浸渍法 (500℃/6h)	[NO]=600μL/L, [NH₃]=650μL/L, [O₂]=3.6%, N₂ to balance, W/F=3mg/(mL·min^-1)	100(100～150℃)	[23]
10% urea-(0.5CeO₂-0.5MnO₂)/ACF	浸渍法 (420℃/2h)	[NO]=1000μL/L, [O₂]=21%, N₂ to balance, GHSV=10000h^-1	90(30℃)	[24]
1.2% Mn_(0.75)-Fe/ACF	浸渍法 (300℃/0.5h)	[NO]=500μL/L, [NH₃]=500μL/L, [O₂]=5%, N₂ to balance, GHSV= 56000h^-1	92(200℃)	[25]
10%Ce-2%Fe/ACF	浸渍法 (300℃/4h)	[NO]=1000μL/L, [NH₃]=1080μL/L, [O₂]=5%, N₂ to balance, GHSV= 5000h^-1	97(80～120℃)	[26]

催化剂（质量分数）	制备方法	反应条件	NO转化率/%	参考文献
5% V₂O₅/ACF	等体积浸渍法 (500℃/8h)	[NO]=[NH₃]=600μL/L，[O₂]=5%， Ar to balance，GHSV=2000h^-1	96(180℃)	[20]
10% Fe₂O₃/ACF	浸渍法(300℃/5h)	[NO]=[NH₃]=200μL/L，[O₂]=10.5%，[H₂O]= 8%， N₂to balance，Q/W=200mL·min^-1·g^-1	约38(150℃)	[21]
10% Co₂O₃/ACF			约38 (150℃)
10% Mn₂O₃/ACF			90 (150℃)
9% CeO₂/ACF	浸渍法(350℃/6h)	[NO]=[NH₃]=1000μL/L，[O₂]=5%， Ar to balance，GHSV=11000h^-1	93.96(180℃)	[19]
10% CeO₂/ACF	浸渍法(360℃/2h)	[NO]=1000μL/L，[NH₃]=1100μL/L，[O₂]=5%， N₂to balance，GHSV=5000h^-1	80～90 (200～300℃)	[22]
20% La₂O₃/ACF	浸渍法(360℃/2h)	[NO]=1000μL/L，[NH₃]=1100μL/L，[O₂]=5%， N₂to balance，GHSV=5000h^-1	55～85 (200～300℃)	[22]
12% MnO _x -CeO _x /ACF_N	等体积浸渍法 (500℃/6h)	[NO]=600μL/L, [NH₃]=650μL/L, [O₂]=3.6%, N₂ to balance, W/F=3mg/(mL·min^-1)	100(100～150℃)	[23]
10% urea-(0.5CeO₂-0.5MnO₂)/ACF	浸渍法 (420℃/2h)	[NO]=1000μL/L, [O₂]=21%, N₂ to balance, GHSV=10000h^-1	90(30℃)	[24]
1.2% Mn_(0.75)-Fe/ACF	浸渍法 (300℃/0.5h)	[NO]=500μL/L, [NH₃]=500μL/L, [O₂]=5%, N₂ to balance, GHSV= 56000h^-1	92(200℃)	[25]
10%Ce-2%Fe/ACF	浸渍法 (300℃/4h)	[NO]=1000μL/L, [NH₃]=1080μL/L, [O₂]=5%, N₂ to balance, GHSV= 5000h^-1	97(80～120℃)	[26]

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炭基材料负载型低温NH₃-SCR脱硝催化剂的研究进展

Research progress on carbon-based material supported catalysts for the selective catalytic reduction of NO _x by NH₃ at low temperature

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