Fe3+ 或 Fe2+ 物种对经铁源改性的 CWK 在 NH3-SCR 反应中的催化性能和反应路径的影响

IF 2.8 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Research on Chemical Intermediates Pub Date : 2024-10-11 DOI:10.1007/s11164-024-05425-z
Ruihua Guo, Zhongxian Song, Xi Chen, Wei Liu, Mengru Zhang, Yehua Fan, Hongrun Gao, Haiyang Li, Xuejun Zhang
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引用次数: 0

摘要

开发用于降低氮氧化物的高性能催化剂是一项重大挑战。采用共沉淀和浸渍法合成了铁源改性的 CWK 催化剂。CWK-F3C 和 CWK-F3S 催化剂在 250-350 ℃ 下具有优异的催化活性和出色的 N2 选择性。CWK-F3C 和 CWK-F3S 催化剂催化活性增强的主要原因可能是较高的 Fe3+ 浓度、更多的表面化学吸附氧物种和更大的 Ce3+ 相对分数。更重要的是,Fe3+ 的掺杂增强了催化剂对 NH3 的吸附和氧化还原能力。DRIFTS 实验结果表明,CWK-F3C 和 CWK-F2C 催化剂遵循 E-R 和 L-H 机理。此外,Fe3+ 的引入产生了更多的表面酸性位点,从而促进了关键中间产物(-NH2)的形成(NH3(ads)+ O(ads)/O2-(ads)→-NH2(ads)+ -OH(ads))。Fe3+ 的存在有利于 NO3- 的形成(NO3- + NO(ads)→NO2(ads)),导致存在快速反应,从而产生了优异的低温催化性能。因此,-NH2 和 NO3- 物种的产生是 CWK-F3C 具有出色催化活性的原因。
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Effect of Fe3+ or Fe2+ species on the catalytic performance and reaction pathway over CWK modified by iron sources in NH3-SCR reaction

Developing high-performance catalysts for NOx reduction was a significant challenge. CWK catalysts modified with iron sources were synthesized using co-precipitation and impregnation methods. The CWK-F3C and CWK-F3S catalysts exhibited the superior catalytic activity at 250–350 ℃ and the excellent N2 selectivity. The key reasons for the enhanced catalytic activity of CWK-F3C and CWK-F3S catalysts could be attributed to the higher Fe3+ concentration, more surface chemisorbed oxygen species and bigger relative fraction of Ce3+. More significantly, the adsorption of NH3 and redox capability were both strengthened by the Fe3+ doping. The DRIFTS experiment results showed that the E-R and L–H mechanism were followed by CWK-F3C and CWK-F2C catalysts. Furthermore, the introduction of Fe3+ generated more surface acidic sites, which could facilitate the formation of key intermediates (-NH2) (NH3(ads) + O(ads)/O2−(ads) → -NH2(ads) + -OH(ads)). The presence of Fe3+ was conducive to NO3 formation (NO3 + NO(ads) → NO2(ads)), resulting in the presence of fast reaction, causing the excellent low temperature catalytic performance. Hence, the production of -NH2 and NO3 species was responsible for the outstanding catalytic activity of CWK-F3C.

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来源期刊
CiteScore
5.70
自引率
18.20%
发文量
229
审稿时长
2.6 months
期刊介绍: Research on Chemical Intermediates publishes current research articles and concise dynamic reviews on the properties, structures and reactivities of intermediate species in all the various domains of chemistry. The journal also contains articles in related disciplines such as spectroscopy, molecular biology and biochemistry, atmospheric and environmental sciences, catalysis, photochemistry and photophysics. In addition, special issues dedicated to specific topics in the field are regularly published.
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