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硫酸化钛铈氧化物催化剂的抗重金属中毒

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工业烟气中氮氧化物高稳定净化催化剂的开发是实现烟气超低排放的重要需求。目前工业上应用最广的SCR商业V2O5-WO3/TiO2催化剂往往面临重金属中毒失活的难题。采用浸渍法改性CeO2载体,开发了具有优异抗重金属(Pb、Zn、Cd)中毒性能的硫酸化钛铈氧化物催化剂。在气体小时空速(GHSV)360 000 h-1、温度300 ℃条件下,硫酸化钛铈氧化物催化剂Pb、Zn、Cd中毒后NO转化率分别为75%、73%、63%,比商用V2O5-WO3/TiO2催化剂Pb、Zn、Cd中毒后NO转化率分别增加了 28%、36%、43%。Raman表征结果显示,硫酸化钛铈氧化物催化剂Pb中毒后仍然保持了较高的氧空位浓度。XPS和H2-TPR表征结果显示,Pb与SO42-发生相互作用,保护了催化剂表面的Ce活性位点,从而抑制Pb对脱硝活性的影响。NH3-TPD表征结果显示,SO42-的掺杂能使催化剂表面酸量显著增加,且催化剂在Pb中毒后表面酸量基本不变,从而表现出高稳定的脱硝活性。本研究可为抗重金属中毒SCR催化剂的设计提供支撑。
Heavy metal poisoning resistance of sulfate-titanium-cerium-oxide catalyst
The development of highly stable purification catalysts for nitrogen oxides in industrial flue gas is an important requirement for achieving ultra-low emissions of flue gas.At present,the most widely used SCR commercial V2O5-WO3/TiO2 catalyst in industry often faces the problem of heavy metal poisoning deactivation.This paper developed sulfated-titanium-cerium-oxide catalyst with excellent resistance to heavy metal(Pb,Zn,Cd)poisoning by using impregnation method to modify CeO2 carrier.The NO conversion of Pb,Zn,and Cd poisoned sulfated-titanium-cerium-oxide catalysts were 75%,73%,and 63%,which were 28%,36%,and 43%higher than those of Pb,Zn,and Cd poisoned V2O5-WO3/TiO2 catalysts at 300 ℃ under the gas hourly space velocity(GHSV)of 360 000 h-1.The Raman results showed that the sulfated-titanium-cerium-oxide catalyst maintained a high concentration of oxygen vacancies even after Pb poisoning.The XPS and H2-TPR results showed that Pb interacts with SO42,protecting the Ce active sites on the catalyst surface,thereby inhibiting the influence of Pb on denitrification activity.The NH3-TPD results showed that the doping of SO42-can significantly increase the surface acidity of the catalyst,and the surface acidity of the catalyst remains unchanged after Pb poisoning,thus exhibiting high and stable denitrification activity.This study can provide a new way for the design of heavy metal poison-resistant SCR catalysts.

nitrogen oxidesNH3-SCRcerium-based catalystsheavy metalspoison-resistance

郭帅、蒋偲、ISAH Abdulrasheed Gambo、刘宏菊、李想

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北京航空航天大学能源与动力工程学院,北京 100191

北京航空航天大学材料科学与工程学院,北京 100191

北京航空航天大学空间与环境学院,北京 100191

氮氧化物 NH3-SCR 铈基催化剂 重金属 抗中毒

2024

环境工程学报
中国科学院生态环境研究中心

环境工程学报

CSTPCD北大核心
影响因子:0.804
ISSN:1673-9108
年,卷(期):2024.18(3)
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