首页|调控Cu/CeO2催化剂形貌增强低温CO氧化的耐水性

调控Cu/CeO2催化剂形貌增强低温CO氧化的耐水性

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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 CuOx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。
Regulating the morphology of Cu/CeO2 catalysts to enhance their water-resistant for low temperature CO oxidation
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 CuOx 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.

water resistanceCO oxidationCu/CeO2 catalyststailorable morphologystructural defects

薛晶、李巧艳、李书宁、梁美生

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太原理工大学环境科学与工程学院,山西太原 030024

耐水性 CO氧化 Cu/CeO2催化剂 形貌调控 结构缺陷

山西省基础研究计划项目山西省基础研究计划项目

20220302121114020210302124131

2024

中国环境科学
中国环境科学学会

中国环境科学

CSTPCDCHSSCD北大核心
影响因子:2.174
ISSN:1000-6923
年,卷(期):2024.44(10)