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活性炭负载MnO基催化剂低温CH-SCR的稳定性机制

Stability Mechanism of Low Temperature CH-SCR with Activated-Carbon-Supported MnO -Based Catalyst.

作者信息

Liu Fang, Zhao Jiangyuan, He Shengbao, Liu Qing, Liu Guangli, Yang Li

机构信息

School Of Low-Carbon Energy And Power Engineering, China University of Mining and Technology, Xuzhou 221116, Jiangsu, China.

Petrochemical Research Institute of PetroChina, Beijing 102206, China.

出版信息

ACS Omega. 2022 Mar 24;7(14):12004-12014. doi: 10.1021/acsomega.2c00202. eCollection 2022 Apr 12.

Abstract

Manganese-based catalysts have shown great potential for use as a hydrocarbon reductant for NO reduction (HC-SCR) at low temperatures if their catalytic stability could be further maintained. The effect of CeO as a promoter and catalyst stability agent for activated carbon supported MnO was investigated during low temperature deNO based on a CH reductant. The modern characterization technology could provide a clear understanding of the activity observed during the deNO tests. When reaction temperatures were greater than 180 °C and with ceria concentrations more than 5%, the overall NO conversion became stable near 70% during long duration testing. In situ DRIFTS shows that CH is adsorbed on the MnCe/NAC catalysts to generate hydrocarbon activated intermediates, R-COOH, and the reaction mechanism followed the E-R mechanism. The stability and the analytical data pointed to the formation of stable oxygen vacancies within Ce/Ce redox couplets that prevented the reduction of MnO to crystalline MnO and promoted the chemisorption of oxygen on the surface of MnO -CeO structures. Based on the data, a synergetic mechanism model of the deNO activity is proposed for the MnO -CeO catalysts.

摘要

如果能够进一步保持催化稳定性,锰基催化剂在低温下作为烃类还原剂用于氮氧化物还原(HC-SCR)显示出巨大潜力。基于甲烷还原剂,研究了CeO作为活性炭负载MnO的促进剂和催化剂稳定剂在低温脱硝过程中的作用。现代表征技术能够清晰地理解脱硝试验中观察到的活性。当反应温度高于180℃且二氧化铈浓度超过5%时,在长时间测试中,总体氮氧化物转化率在70%左右趋于稳定。原位漫反射红外傅里叶变换光谱表明,甲烷吸附在MnCe/NAC催化剂上生成烃类活性中间体R-COOH,反应机理遵循E-R机理。稳定性和分析数据表明,在Ce/Ce氧化还原偶中形成了稳定的氧空位,这阻止了MnO还原为结晶态MnO,并促进了氧在MnO-CeO结构表面的化学吸附。基于这些数据,提出了MnO-CeO催化剂脱硝活性的协同机理模型。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5dcd/9016832/f45f94fbde69/ao2c00202_0001.jpg

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