低温脱硝催化剂研究进展

doi:10.19964/j.issn.1006-4990.2021-0602

Abstract

Abstract:

On the basis of conventional selective catalytic reduction（SCR） catalysts,the research progress on low-temperature SCR catalysts was introduced by taking V-Ti catalysts,solid solution catalysts and new MnO _x catalysts as key points.The preparation methods,element doping,reaction mechanism and resistance of composite catalysts with different active components were reviewed.By analyzing the characterization of different composite catalysts,the performance and low-temperature denitration efficiency of the catalyst were summarized.The excellent denitration characteristics of the new MnO _x catalyst was emphatically expounded.It was considered that improving the water and sulfur resistance of new MnO _x by modification would become the development direction and research hotspot in this field in the future.Finally,the influence of different carriers on the catalytic efficiency of the new MnO _x catalyst was introduced.It was found that TiO₂ carrier had good H₂O resistance,Al₂O₃ carrier could significantly enhance the catalytic activity,and CeO₂ carrier had good thermal stability.

Key words: SCR catalyst, V-Ti catalyst, solid solution catalyst, new MnO _x catalyst, water and sulfur resistance

CLC Number:

O643.36

YU Wohui,ZHANG Pan,ZHAO Yiming,ZHA Zhongfa,WU Ruilong,QI Liqiang. Research progress on low-temperature denitration catalysts[J]. Inorganic Chemicals Industry, 2022, 54(10): 57-68.

Figures/Tables 15

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Table 5

Properties and characteristics of SCR catalysts with different supports"

负载体	晶型	负载体特性	常见活性组分		催化剂的特性
TiO₂	八面体	弱酸性或无酸性负载,具有路易斯酸性中心,适合负载非惰性金属氧化物	MnO _x /TiO₂		在高Mn负载量下,以微晶和聚合物的形式存在,促进脱硝反应
			MnO _x -CeO₂/TiO₂		在高Mn负载量下,复合催化剂抗水性良好
			Fe-Mn-Ce/TiO₂		TiO₂使活性组分均匀分布在负载体上
γ- Al₂O₃	八面体	支撑和均匀分散活性成分,具有良好分散性、适度氧化还原性、较多酸性位	MnO _x /γ-Al₂O₃		具有良好分散性、适度氧化还原性、较多酸性位、优良NO_x吸附性能以及含有丰富的Mn⁴⁺
γ- Al₂O₃	八面体	支撑和均匀分散活性成分,具有良好分散性、适度氧化还原性、较多酸性位	MnO _x -CeO₂/Al₂O₃		Al³⁺的引入可以减小CeO₂-MnO _x 催化剂的晶粒尺寸,且Al³⁺显著增加了其比表面积和孔容,这是由于微晶尺寸的减小
CeO₂	三角双锥	CeO₂与其他金属氧化物之间的协同作用能提高催化剂活性、选择性及稳定性	LaMnO₃/CeO₂		LaMnO₃和CeO₂之间的相互作用在低温段有利于晶格氧的移动,促进部分NO氧化成NO₂,具有较好的催化性能
CeO₂	三角双锥	CeO₂与其他金属氧化物之间的协同作用能提高催化剂活性、选择性及稳定性	CuO/CeO₂		在高温下不会形成复合物,热稳定性良好
SiO₂	表面不存在空位	酸性氧化物,化学性质比较稳定,具有较好催化效率、催化活性、催化剂负载的牢固性	V-Mo-Ce/TiO₂-SiO₂		SiO₂可以显著增加比表面积,并影响表面原子间的相互作用；SiO₂对于催化剂的脱硝性能影响较小,但在SO₂存在下表现出较好的催化活性
分子筛	四面体	具有规则、稳定的骨架结构和较高的比表面积,及其较高的热和水热稳定性,确保了活性金属的高度分散,以及反应物和产物的高效扩散,促进反应的迅速进行	Fe基 Cu基	ZSM、SSZ、SAPO等系列	①在通电的条件下,Mn的引入提高了Mn-Cu/ZSM-5催化剂的催化性能；②Cu/ZSM-5在NH₃存在时的产物是NH₄HSO₄,且NH₄HSO₄会与Cu（HSO₄）₂相互转化,控制NH₃的量能提高对Cu/SSZ-13回收效果；③Cu-SSZ-13催化剂显示出优异的NH₃-SCR反应性和较强的SO₂耐受性

Table 5

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脱硝工艺		脱硝率/%		还原/氧化剂	反应温度/℃	催化剂	工艺缺点
干法脱硝	氧化法	光催化氧化	70~75	TiO₂、硫化镉	无	使用	光子产率低、光源单一
		氧化物氧化	70~80	金属氧化物	无	不使用	需处理废弃金属氧化物
		等离子体氧化	60~90	氨水	无	不使用	能耗大,伴随氨逃逸
	分解法	光催化分解	一般	无	无	使用	反应活化能高,所需温度高
	分解法	热催化分解	一般	无	＞500	使用	反应活化能高,所需温度高
	还原法	光催化还原	一般	NH₃或醇类	无	使用	催化还原效果不理想、反应不完全
		SCR	75~90	NH₃或尿素	100~400	使用	无明显缺点
		SNCR	40~70	NH₃或尿素	800~1 300	不使用	氨逃逸
	吸附法（活性炭和活性焦）	50~80		NH₃或尿素	150~200	使用	抗硫性差、脱硝效率低
湿法脱硝	吸收法	溶液吸收	较高	无	＜150	不使用	产生废液、能耗高、酸循环需求量大
		气相氧化吸收		O₂、O₃、ClO₂等			O₃成本高、ClO₂易造成二次污染
		液相氧化吸收		Fenton试剂、含氯氧化剂等			成本高,易造成二次污染
	生物法	70~80		无	无	不使用	脱硝效率低

催化剂类型	制备方法	n（Fe）/n（Ce）	优点	缺点
Fe_0.5Ce_0.5O₂^[12]	共沉淀法	1∶1	工艺简单、固溶体颗粒均匀	催化剂颗粒易聚合、比表面积低
Fe₁Ce_0.35固溶体^[13]	水热合成法	1∶0.35	纯度高、分散性好、污染小、能耗低	设备昂贵、投资高
Fe_0.2Ce_0.8O_2-_δ^[14]	固相法	1∶4	反应温度低、产物颗粒小、粒度分布窄、比表面积大	污染较大、反应时间长
Fe_0.5Ce_0.5O₂^[15]	溶胶-凝胶法	1∶1	工艺简单	容易导致反应不彻底

催化剂	类型	制备方法	最佳活性（NO _x 转化率）	物质的量比	催化剂特点（活性机理）	文献来源
无负载体	Mn-Ce	表面活性剂模板法	100~200 ℃,＞95%	n（Mn）/n（Ce）=1	较高的比表面积,活性中心均匀,易于吸附NH₃和NO _x,抗硫性突出	[27]
	Mn-Ce	共沉淀法	150 ℃,约为95%	n（Mn）/n（Ce）=1	较高的比表面积,活性中心均匀,易于吸附NH₃和NO _x,抗硫性突出	[27]
	La_1-_x Ce _x MnO₃	溶胶-凝胶法	135 ℃,＞90%	n（Mn）/n（La）/n（Ce）= 1∶0.8∶0.2	Ce掺杂增加了La-Mn氧化物的表面Mn⁴⁺含量、化学吸附氧	[28]
有TiO₂负载体	Mn-Ce-Ho/TiO₂	浸渍法	140~220 ℃,＞90% 180 ℃,约为96%	n（Mn）/n（Ce）/n（Ti）/ n（Ho）=0.4∶0.07∶1∶0.1	提高了Mn⁴⁺含量,使化学吸附氧增加	[30]
	Ru-Mn-Ce/TiO₂	浸渍法	120~250 ℃,几乎100%	无	CMRT-X催化剂脱硝活性降低是由于过量的NH₃氧化以及N₂O副产物生成	[31]
	W-Mn-Ce/TiO₂	浸渍法	160 ℃,几乎100%	无	热稳定性增加,增加了NH₃吸附量和反应活性,但抑制NO吸附	[32]
	Mn-Sb/TiO₂	溶胶-凝胶法	100℃,约为95%	n（Mn）/n（Ti）=0.2 n（Sb）/n（Ti）=0.2	生成更多的还原物质、Mn⁴⁺和表面吸附氧	[33]
	Tm-MnO _x /TiO₂	浸渍法	150~270 ℃,几乎100%	n（Mn）/n（Ti）=1∶3 n（Tm）/n（Ti）=0.1∶1	提高了催化剂的表面酸性、还原性、Mn⁴⁺和表面化学吸附氧浓度	[34]
	Sm-Mn/TiO₂	超声波浸渍法	110~250 ℃,大于80%	n（Mn）/n（Sm）=2∶1	改善了MnO _x 在催化剂表面的分散性,增加了比表面积、路易斯酸位点和O _α 的相对浓度	[35]

催化剂种类	制备方法	烟气工况	脱硝效率	参考文献
Ce_0.4Mn/TiO₂	反向共沉淀法	GSHV=44 000 h^-1, 5%H₂O+220 mg/m³ SO₂	200 ℃-99%下降到73%-4 h	[37]
Fe_0.2Co_0.4Mn-Ce/TiO₂	湿式浸渍法	GSHV=12 000 h^-1, 10%H₂O+440 mg/m³ SO₂	200 ℃-98%下降到90%-4 h	[38]
Co₁Mn₄Ce₅O _x	共沉淀法	GSHV=48 000 h^-1, 10%H₂O+330 mg/m³ SO₂	175 ℃-91%下降到73%-6 h	[39]
Ni₁Mn₄Ce₅O _x	共沉淀法	GSHV=48 000 h^-1, 10%H₂O+330 mg/m³ SO₂	175 ℃-91%下降到76%-6 h	[39]
Mn-Eu/TiO₂	溶胶-凝胶法	GSHV=108 000 h^-1,10%H₂O+220 mg/m³ SO₂	150 ℃-85%下降到70%-25 h	[40]
Nb₂O₅-Mn-Ce/AC	湿式浸渍法	GSHV=14 500 h^-1, 350 mg/m³ SO₂	225 ℃-85%下降到70%-3.5 h	[41]

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Research progress on low-temperature denitration catalysts

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