CIESC Journal ›› 2024, Vol. 75 ›› Issue (1): 312-321.DOI: 10.11949/0438-1157.20230677

• Catalysis, kinetics and reactors • Previous Articles     Next Articles

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

Jialin ZHANG(), Dawei XU, Yue GAO, Xingang LI()   

  1. State Key Laboratory of Chemical Engineering, Collaborative Innovation Center of Chemical Science and Engineering, Tianjin Key Laboratory of Applied Catalysis Science and Engineering, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300354, China
  • Received:2023-07-03 Revised:2023-09-26 Online:2024-03-11 Published:2024-01-25
  • Contact: Xingang LI

泡沫镍负载CeO2改性CuO催化剂的碳烟燃烧性能研究

张家琳(), 徐大为, 高越, 李新刚()   

  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
  • 通讯作者: 李新刚
  • 作者简介:张家琳(1999—),女,硕士研究生,zjl_3010@tju.edu.cn
  • 基金资助:
    国家自然科学基金项目(21878213)

Abstract:

CeO2-modified CuO catalyst (xCeO2-CuO/NF) was successfully synthesized by hydrothermal method through pre-deposition of CeO2 crystal nuclei on nickel foam substrate. The soot oxidation activity of xCeO2-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 Cu x Ce1-x O solid solution on xCeO2-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.

Key words: catalyst, solid solution, nanostructure, multiphase reaction, active oxygen species

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(xCeO2-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,xCeO2-CuO/NF中形成的Cu x Ce1-x O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。

关键词: 催化剂, 固溶体, 纳米结构, 多相反应, 活性氧物种

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