调控Cu/CeO<sub>2</sub>催化剂形貌增强低温CO氧化的耐水性

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摘要合成了管状、棒状和颗粒状的Cu/CeO₂的催化剂,探讨了其在潮湿条件下氧化CO的结构-性能相关性.结果表明,管状催化剂(CuCe-NT)具有优异的低温活性和抗H₂O稳定性.根据表征,CuCe-NT与纳米棒状(CuCe-NR)和纳米颗粒状(CuCe-NP)催化剂相比,结晶度更低、表面积更大且结构缺陷更多,从而增强了CuO_x与CeO₂间的相互作用,加强了Ce⁴⁺/Ce³⁺和Cu²⁺/Cu⁺的氧化还原循环,使表面富集大量Ce³⁺和Cu⁺,进一步促进了CO的吸附和氧化.此外,中空结构的CuCe-NT具有较大的孔径,可有效抑制H₂O的缔合吸附,从而抑制氧空位上惰性OH的生成,在潮湿条件下保持较高的氧化性.In-situ DRIFTS表明,相比于CuCe-NP,中空结构的CuCe-NT可以缓解H₂O与CO的竞争性吸附,抑制桥式碳酸盐的形成,确保在潮湿环境下氧化CO.本研究从吸附H₂O的类型和反应机理方面证明了催化剂结构对耐H₂O性的影响,为设计耐H₂O性CO氧化催化剂提供了一种策略.

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	薛晶
	李巧艳
	李书宁
	梁美生

关键词 ：耐水性, CO氧化, Cu/CeO₂催化剂, 形貌调控, 结构缺陷

Abstract：Herein, tube-, rod- and particle-like Cu/CeO₂ catalysts were synthesized and their structure-performance relationship for CO oxidation in moist conditions was explored. The results revealed that the tube-like catalysts (CuCe-NT) exhibited excellent low-temperature activity and superior H₂O resistance stability. The characterization results indicated that CuCe-NT catalyst had a lower crystallinity, larger surface area and more structural defects in comparation with rod-like (CuCe-NR) and particle-like (CuCe-NP) samples, which greatly strengthened the interactions between CuO_x and CeO₂, thus boosting the redox of Ce⁴⁺/Ce³⁺ and Cu²⁺/Cu⁺, and the surface enrichment of Ce³⁺ and Cu⁺, further facilitating the CO adsorption and oxidation. Moreover, the hollow structure of CuCe-NT catalyst with a large pore size effectively inhibited the associatively adsorption of H₂O, suppressing the generation of inert OH groups on oxygen vacancies, and thus maintaining its higher oxidization in the presence of water. In situ-DRIFTS showed that compared to CuCe-NP catalyst, the nanotube structure of CuCe-NT catalyst alleviated the competitive adsorption of H₂O with CO, and inhibited the formation of bridged carbonates, thus ensuring the CO oxidation under humid atmosphere. This study revealed the effect of catalyst structure on its resistance of H₂O in terms of H₂O adsorption type and reaction mechanism, thus providing an ingenious strategy for the design of H₂O-resistant CO oxidation catalysts.

Key words： water resistance CO oxidation Cu/CeO₂ catalysts tailorable morphology structural defects

收稿日期: 2024-02-29

PACS:

X511

基金资助:山西省基础研究计划项目(202203021211140,20210302124131)

通讯作者: 梁美生,教授,liangmeisheng@tyut.edu.cn E-mail: liangmeisheng@tyut.edu.cn

作者简介: 薛晶(1999-),女,山西运城人,太原理工大学硕士研究生,主要从事大气污染控制CO催化氧化方向研究.1169680131@qq.com.

引用本文:

薛晶, 李巧艳, 李书宁, 梁美生. 调控Cu/CeO₂催化剂形貌增强低温CO氧化的耐水性[J]. 中国环境科学, 2024, 44(10): 5415-5425. XUE Jing, LI Qiao-yan, LI Shu-ning, LIANG Mei-sheng. Regulating the morphology of Cu/CeO₂ catalysts to enhance their water-resistant for low temperature CO oxidation. CHINA ENVIRONMENTAL SCIENCECE, 2024, 44(10): 5415-5425.

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http://www.zghjkx.com.cn/CN/ 或 http://www.zghjkx.com.cn/CN/Y2024/V44/I10/5415

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