化工学报2024,Vol.75Issue(1) :312-321.DOI:10.11949/0438-1157.20230677

泡沫镍负载CeO2改性CuO催化剂的碳烟燃烧性能研究

Performance of soot combustion over CeO2 modified CuO catalysts supported on nickel foams

张家琳 徐大为 高越 李新刚
化工学报2024,Vol.75Issue(1) :312-321.DOI:10.11949/0438-1157.20230677

泡沫镍负载CeO2改性CuO催化剂的碳烟燃烧性能研究

Performance of soot combustion over CeO2 modified CuO catalysts supported on nickel foams

张家琳 1徐大为 1高越 1李新刚1
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作者信息

  • 1. 天津大学化工学院,天津市应用催化科学与工程重点实验室,天津化学化工协同创新中心,化学工程联合国家重点实验室,天津 300354
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摘要

通过在泡沫镍基底上预沉积CeO2晶核,采用水热法成功合成出泡沫镍负载CeO2改性CuO催化剂(x CeO2-CuO/NF),同未加入CeO2的催化剂(CuO/NF)相比,其碳烟氧化活性显著提高.随着催化剂中CeO2含量的增加,Ce/Cu质量比不断增大直至趋于平稳,催化剂的催化活性随之提高直至基本不变.其中,6.5CeO2-CuO/NF的催化活性最好,T50(383℃)最低,比CuO/NF催化剂低32℃.研究结果表明,预沉积CeO2晶核一方面可促进CuO微纳结构的生长,提高碳烟颗粒与催化剂活性位点的接触效率;另一方面,x CeO2-CuO/NF中形成的CuxCe1-xO固溶体增强了铜铈之间的相互作用,通过Ce3+/Ce4+和Cu2+/Cu+之间氧化还原耦合循环促使活性氧物种的生成,并提升了其本征活性,从而极大地提高了其催化碳烟氧化的能力.

Abstract

CeO2-modified CuO catalyst(x CeO2-CuO/NF)was successfully synthesized by hydrothermal method through pre-deposition of CeO2 crystal nuclei on nickel foam substrate.The soot oxidation activity of x CeO2-CuO/NF was significantly higher than that of the catalyst without addition of CeO2(CuO/NF).With the increase of CeO2 content,the Ce/Cu mass ratio and the intrinsic catalytic activity of the catalyst gradually increased,and finally both of them reached stable.Among them,the catalytic activity of 6.5CeO2-CuO/NF was the best with the lowest T50(383℃),which was 32℃lower than that of the CuO/NF catalyst.The results indicate that the pre-deposition of CeO2 crystal nuclei can promote the growth of CuO into a nanostructure,which improves the contact efficiency between soot particles and active sites of the catalyst,on the other hand,the formation of CuxCe1-xO solid solution on x CeO2-CuO/NF enhances the interaction between Ce and Cu cations.The interaction generates a redox coupling cycle between Ce3+/Ce4+ and Cu2+/Cu+,prompting the generation and intrinsic activity of active oxygen species.All of these merits greatly improve the catalytic performance of soot oxidation over our as-synthesized catalysts.

关键词

催化剂/固溶体/纳米结构/多相反应/活性氧物种

Key words

catalyst/solid solution/nanostructure/multiphase reaction/active oxygen species

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基金项目

国家自然科学基金项目(21878213)

出版年

2024
化工学报
中国化工学会 化学工业出版社

化工学报

CSTPCDCSCD北大核心
影响因子:1.26
ISSN:0438-1157
参考文献量42
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