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

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

Abstract

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

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

CLC Number:

TQ426.99

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.

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.

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

炭基材料负载型低温NH₃-SCR脱硝催化剂的研究进展

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