微波技术在脱硝催化剂制备及NH3-SCR中的应用进展

doi:10.11949/0438-1157.20250941

摘要/Abstract

摘要：

氮氧化物（NO _x ）作为主要大气污染物之一，其排放控制技术一直是环境催化领域的研究热点。选择性催化还原（SCR）技术是目前最有效的脱硝方法之一，而催化剂的性能直接决定了SCR技术的应用效果。微波法作为一种高效、节能的制备技术，凭借均匀加热、促进活性组分高度分散与小尺寸颗粒形成、调控催化剂微观结构、且绿色环保的独特优势，在脱硝催化剂制备中展现出较强的应用前景。本文系统综述了微波法在脱硝催化剂制备及作为反应场热源中的应用进展，重点讨论了微波法对催化剂结构、性能的影响及其作用机制，总结了微波辅助制备的各类脱硝催化剂（包括金属氧化物、分子筛、金属有机骨架材料、碳材料）的性能特点，并对微波法在脱硝催化剂制备中的发展趋势和面临的挑战进行了展望。

关键词: 微波法, 催化剂, 选择性催化还原, 传热, 应用进展

Abstract:

As one of the major air pollutants, the emission control technology of nitrogen oxides (NO _x ) has been a research hotspot in the field of environmental catalysis. Selective catalytic reduction (SCR) technology is currently one of the most effective denitration methods, and the catalytic performance directly determines the application effectiveness of SCR technology. As a high-efficiency and energy-saving preparation technology, microwave method, with the unique advantages of uniform heating, promoting high dispersion of active components and formation of small-sized particles, regulating the microstructure of catalysts, and being green and environmentally friendly, has shown strong application prospects in the preparation of denitrification catalysts. This paper systematically reviews the application progress of the microwave method in the preparation of denitration catalysts, focuses on discussing the effects of the microwave method on the structure and performance of catalysts as well as their action mechanisms, summarizes the performance characteristics of various microwave-assisted prepared denitration catalysts (including metal oxides, molecular sieves, metal-organic frameworks, and carbon materials), and prospects the development trends and challenges of the microwave method in the preparation of denitration catalysts.

Key words: Microwave method, Catalyst, SCR, Heat transfer, Application progress

中图分类号:

X511

王成志, 张忠良, 常琛朝. 微波技术在脱硝催化剂制备及NH₃-SCR中的应用进展[J]. 化工学报, DOI: 10.11949/0438-1157.20250941.

Chengzhi WANG, Zhongliang ZHANG, Chenchao CHANG. Progress in Microwave Technology for Denitration Catalyst Preparation and NH₃-SCR Application[J]. CIESC Journal, DOI: 10.11949/0438-1157.20250941.

图/表 14

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催化剂	制备方法	微波功率/W	微波时间/分钟	NO _x 转化率/%	利弊	参考文献
MnO _x	微波水热法	100	3	100	制备效率高，活性好、N₂选择性高；但抗硫性能仍然较差	^[29]
CeO₂	微波焙烧	300	120	70	比表面积大、晶粒尺寸小且晶粒分散均匀；温窗较窄	^[32]
γ-Fe₂O₃	微波热解法	700	10.8	96	工艺简单、晶相单一、结晶程度高；煅烧过程中存在一定程度的烧结现象，会导致部分孔结构遭到破坏	^[36]
V₂O₅@AC	微波浸渍法	300	-	99.7	诱导V₂O₅的高分散性和活性位点的暴露，产生更多的配位不饱和V和缺陷；会使部分催化剂比表面积和孔体积减小	^[37]
VWTi-多孔纤维陶瓷	微波干燥	385	40.2	98	分散均匀，改变载体TiO₂的形貌、晶粒和孔结构以增大比表面积；高功率微波会降低TiO₂中锐钛矿相比例，对活性有不利影响	^[38]
Mn₂CoO₄@rGO	微波辐照法	125	30	95	微波可快速同步实现氧化石墨烯还原及Mn₂CoO₄纳米片的规则生长，具有大比表面积、Lewis酸位点；负载量需严格控制，过高将抑制活性	^[40]
Ce-La-Fe/γ-Al₂O₃	微波水热法	-	-	95.2	助力形成Ce-La-Fe-O固溶体，增加比表面积、表面酸位点及氧空位；制备过程复杂	^[41]
Fe_0.65Ce_0.05Ti_0.30Oz	微波水热法	255	15	100	使活性温窗向低温偏移；但会降低催化剂的高温活性及比表面积	^[42]
Fe_0.85Ce_0.10W_0.05O_z	微波辅助溶胶-凝胶法	291	10	100	优化催化剂性能且优于传统水热法，表面吸附氧含量多；高温活性差且NH₃氧化副反应较强	^[23]
Fe_0.8Mg_0.2O_z	微波辅助共沉淀法	-	-	99.1	高温使颗粒团聚、微孔坍塌，温窗较窄不利于应用	^[44]
NdV/Ti	微波辅助沉积-沉淀法	500	-	100	促使Nd与VO₃⁻快速反应并在TiO₂表面形成均匀沉淀，利于钒酸盐分散	^[17]
Fe₂O₃@稀土精矿	微波焙烧	-	20	80.6	微波处理后可增加Ce³⁺和Fe²⁺含量，产生更多氧空位；温度过高，稀土精矿易烧结	^[24]
Ce _x Zr_1-_x O₂	微波焙烧	350	120	88.5	微波非热效应能够较大的提高脱硝效率，并且使反应的窗口温度前移	^[25]
(Ce，La)PO₄	微波焙烧		20	95	降低样品结晶度、增强活性物质分散性、增大比表面积、增加酸性位点	^[45]
CeO₂-TiO₂	微波辅助共沉淀法	200	120	97	微波可加速催化剂的结晶速率、增大比表面积、增加酸性位点及表面化学吸附氧浓度、提高Ce³⁺/Ce⁴⁺比例	^[46]
MnV₂O _x /TiO₂	微波辅助沉积-沉淀法	阶段1: 700, 阶段2: 800	阶段1:2，阶段2：6	86	能够快速加热并促进均匀沉积；但其高功率和较长时间可能对催化剂结构产生一定影响	^[47]
Mn-Fe/Al₂O₃	微波干燥	350	15	100	微波导致催化剂孔隙发达，减缓硫酸铵盐沉积的抑制效应	^[48]

催化剂	制备方法	微波功率/W	微波时间/分钟	NO _x 转化率/%	利弊	参考文献
MnO _x	微波水热法	100	3	100	制备效率高，活性好、N₂选择性高；但抗硫性能仍然较差	^[29]
CeO₂	微波焙烧	300	120	70	比表面积大、晶粒尺寸小且晶粒分散均匀；温窗较窄	^[32]
γ-Fe₂O₃	微波热解法	700	10.8	96	工艺简单、晶相单一、结晶程度高；煅烧过程中存在一定程度的烧结现象，会导致部分孔结构遭到破坏	^[36]
V₂O₅@AC	微波浸渍法	300	-	99.7	诱导V₂O₅的高分散性和活性位点的暴露，产生更多的配位不饱和V和缺陷；会使部分催化剂比表面积和孔体积减小	^[37]
VWTi-多孔纤维陶瓷	微波干燥	385	40.2	98	分散均匀，改变载体TiO₂的形貌、晶粒和孔结构以增大比表面积；高功率微波会降低TiO₂中锐钛矿相比例，对活性有不利影响	^[38]
Mn₂CoO₄@rGO	微波辐照法	125	30	95	微波可快速同步实现氧化石墨烯还原及Mn₂CoO₄纳米片的规则生长，具有大比表面积、Lewis酸位点；负载量需严格控制，过高将抑制活性	^[40]
Ce-La-Fe/γ-Al₂O₃	微波水热法	-	-	95.2	助力形成Ce-La-Fe-O固溶体，增加比表面积、表面酸位点及氧空位；制备过程复杂	^[41]
Fe_0.65Ce_0.05Ti_0.30Oz	微波水热法	255	15	100	使活性温窗向低温偏移；但会降低催化剂的高温活性及比表面积	^[42]
Fe_0.85Ce_0.10W_0.05O_z	微波辅助溶胶-凝胶法	291	10	100	优化催化剂性能且优于传统水热法，表面吸附氧含量多；高温活性差且NH₃氧化副反应较强	^[23]
Fe_0.8Mg_0.2O_z	微波辅助共沉淀法	-	-	99.1	高温使颗粒团聚、微孔坍塌，温窗较窄不利于应用	^[44]
NdV/Ti	微波辅助沉积-沉淀法	500	-	100	促使Nd与VO₃⁻快速反应并在TiO₂表面形成均匀沉淀，利于钒酸盐分散	^[17]
Fe₂O₃@稀土精矿	微波焙烧	-	20	80.6	微波处理后可增加Ce³⁺和Fe²⁺含量，产生更多氧空位；温度过高，稀土精矿易烧结	^[24]
Ce _x Zr_1-_x O₂	微波焙烧	350	120	88.5	微波非热效应能够较大的提高脱硝效率，并且使反应的窗口温度前移	^[25]
(Ce，La)PO₄	微波焙烧		20	95	降低样品结晶度、增强活性物质分散性、增大比表面积、增加酸性位点	^[45]
CeO₂-TiO₂	微波辅助共沉淀法	200	120	97	微波可加速催化剂的结晶速率、增大比表面积、增加酸性位点及表面化学吸附氧浓度、提高Ce³⁺/Ce⁴⁺比例	^[46]
MnV₂O _x /TiO₂	微波辅助沉积-沉淀法	阶段1: 700, 阶段2: 800	阶段1:2，阶段2：6	86	能够快速加热并促进均匀沉积；但其高功率和较长时间可能对催化剂结构产生一定影响	^[47]
Mn-Fe/Al₂O₃	微波干燥	350	15	100	微波导致催化剂孔隙发达，减缓硫酸铵盐沉积的抑制效应	^[48]

催化剂	制备方法	微波功率/W	微波时间/分钟	NO _x 转化率/%	利弊	参考文献
Cu^II-SSZ-13	微波水热法	400	540	100	微波辅助水热合成可缩短CuII-SSZ-13的结晶时间，影响其成核与生长，形成稳定骨架结构并增强Al-O-Si键	^[49]
Cu/SSZ-13	微波活化	250	30	90	拓宽活性温窗、增加活性位点；但功率过大或时间过长会消耗大量能量并可能对催化剂表面造成局部损伤	^[50]
CuCe@ZIF-7	微波水热法	900	240	95	快速、高效制备前驱体	^[51]
Cu-SSZ-13	微波水热法	400	540	100	缩短SSZ-13的结晶时间，促进其成核与生长，使颗粒分散性优异、形貌规则，增强离子交换能力及NH₃/NO吸附能力	^[52]
Cu-ZSM-5	微波干燥	800	10	87	影响催化剂的孔道结构及活性物质的晶粒大小与分布；但会破坏微孔结构导致有效活性位点减少	^[53]
Cu-SSZ-13	微波水热法	-	360	100	缩短SSZ-13分子筛晶化时间，促进晶核形成与生长，提高结晶度	^[54]
Fe-Al-SBA-15	微波水热法	-	-	95	促进Fe-Al-SBA-15形成更多低聚Fe _x Oᵧ簇和四面体骨架铝	^[21]
MCM-41	微波晶化法	阶段1: 300，阶段2: 60	阶段1: 15，阶段2: 25	-	快速合成、晶粒直径小、分散均匀、比表面积大、具有良好高温和水热稳定性，且操作便利、节能、环境污染少，无转晶现象	^[56]

催化剂	制备方法	微波功率/W	微波时间/分钟	NO _x 转化率/%	利弊	参考文献
Cu^II-SSZ-13	微波水热法	400	540	100	微波辅助水热合成可缩短CuII-SSZ-13的结晶时间，影响其成核与生长，形成稳定骨架结构并增强Al-O-Si键	^[49]
Cu/SSZ-13	微波活化	250	30	90	拓宽活性温窗、增加活性位点；但功率过大或时间过长会消耗大量能量并可能对催化剂表面造成局部损伤	^[50]
CuCe@ZIF-7	微波水热法	900	240	95	快速、高效制备前驱体	^[51]
Cu-SSZ-13	微波水热法	400	540	100	缩短SSZ-13的结晶时间，促进其成核与生长，使颗粒分散性优异、形貌规则，增强离子交换能力及NH₃/NO吸附能力	^[52]
Cu-ZSM-5	微波干燥	800	10	87	影响催化剂的孔道结构及活性物质的晶粒大小与分布；但会破坏微孔结构导致有效活性位点减少	^[53]
Cu-SSZ-13	微波水热法	-	360	100	缩短SSZ-13分子筛晶化时间，促进晶核形成与生长，提高结晶度	^[54]
Fe-Al-SBA-15	微波水热法	-	-	95	促进Fe-Al-SBA-15形成更多低聚Fe _x Oᵧ簇和四面体骨架铝	^[21]
MCM-41	微波晶化法	阶段1: 300，阶段2: 60	阶段1: 15，阶段2: 25	-	快速合成、晶粒直径小、分散均匀、比表面积大、具有良好高温和水热稳定性，且操作便利、节能、环境污染少，无转晶现象	^[56]

催化剂	制备方法	微波功率/W	微波时间/分钟	NO _x 转化率/%	利弊	参考文献
Cu-BTC	微波合成法	600	30	97.8	与非热等离子体协同作用可激活Cu-BTC产生配位不饱和位点，增加羰基含量，提升表面催化活性和化学吸附性能	^[60]
CuFe₂O₄	微波合成法	900	240	92	分散性和稳定性良好	^[22]
Ce-Cu-BTC	微波辅助加热-分步浸渍法	-	120	91	促进形成高比表面积、规则多孔结构及丰富活性位点，增强Ce与Cu的协同作用；但热稳定性差，并且在高于300 ℃时骨架易坍塌	^[61]
Ti_0.2-Ni_0.8-MOF	微波辐照	100	120	100	更高的合成效率、更好的结晶度、晶粒细小且更加均匀	^[62]
活性焦	微波辐照	500	30	90	可提高活性焦的比表面积和孔容，减小孔径，激活表面官能团	^[63]
活性焦负载Fe/Mn/Cu	微波辐照	200	-	85.6	增强活性焦极化、提高等离子体强度、增加含氧官能团	^[64]
CuO/AC	微波活化	700	7	52	可增加介孔比例、优化孔结构和表面碱性基团；但脱硝性能不理想	^[65]
活性炭负载Cu-Fe	微波活化	-	-	86	微波处理的椰壳活性炭作为载体，经Cu、Fe改性后可提供丰富表面活性位点，利于NO和Hg⁰的吸附与转化；但活性炭吸附作用贡献无法考量	^[66]
Mn₂CoO₄@rGO	微波水热法	125	30	100	可同时实现氧化石墨烯的还原和Mn₂CoO₄纳米片在还原石墨烯层上的直立规则生长	^[40]

微波技术在脱硝催化剂制备及NH₃-SCR中的应用进展

Progress in Microwave Technology for Denitration Catalyst Preparation and NH₃-SCR Application

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