从头开始理解形貌依赖的CuOx-CeO2相互作用

doi:10.1016/S1872-2067(19)63503-5

催化学报 ›› 2020, Vol. 41 ›› Issue (6): 1006-1016.DOI: 10.1016/S1872-2067(19)63503-5

从头开始理解形貌依赖的CuO_x-CeO₂相互作用

高玉仙^a, 张振华^b, 李兆瑞^a, 黄伟新^a

a 中国科学技术大学化学物理系, 中国科学院能量转换材料重点实验室, 安徽省教育厅表界面化学与能源催化重点实验室, 合肥微尺度物质科学国家研究中心, 安徽合肥 230026;
b 浙江师范大学物理化学研究所, 先进催化材料教育部重点实验室, 浙江金华 321004

收稿日期:2019-10-20 修回日期:2019-11-29 出版日期:2020-06-18 发布日期:2020-01-21
通讯作者: 黄伟新
基金资助:
国家自然科学基金（21525313，21761132005）；中国科学院和教育部长江学者奖励计划.

Understanding morphology-dependent CuO_x-CeO₂ interactions from the very beginning

Yuxian Gao^a, Zhenhua Zhang^b, Zhaorui Li^a, Weixin Huang^a

a Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, CAS Key Laboratory of Materials for Energy Conversion and Department of Chemical Physics, University of Science and Technology of China, Hefei 230026, Anhui, China;
b Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, Institute of Physical Chemistry, Zhejiang Normal University, Jinhua 321004, Zhejiang, China

Received:2019-10-20 Revised:2019-11-29 Online:2020-06-18 Published:2020-01-21
Contact: S1872-2067(19)63503-5
Supported by:
This work was supported by the National Natural Science Foundation of China (21525313, 21761132005), the Chinese academy of Sciences, and the Changjiang Scholars Program of Ministry of Education of China.

摘要/Abstract

摘要： CuO_x/CeO₂催化剂在CO氧化反应中表现出高催化活性和显著结构敏感性.文献报道中CuO_x/CeO₂催化剂体系的合成条件差异较大，从而导致观察到的CuO_x-CeO₂相互作用存在较大争议.因此，系统研究并阐明CuO_x/CeO₂催化剂中CuO_x-CeO₂相互作用对于理解复杂的CuO_x-CeO₂界面催化作用具有重要的研究意义.近期发现，氧化物纳米晶的形貌可作为一种新的结构参数，在不改变氧化物催化剂组成的条件下实现其结构和性能的调控.本文以不同形貌CeO₂纳米晶为载体，包括优先暴露{110}+{100}晶面的CeO₂纳米棒、优先暴露{100}晶面的CeO₂纳米立方体和优先暴露{111}晶面的CeO₂纳米多面体，采用等体积浸渍方法合成了Cu担载量为0.025%~5%的CuO_x/CeO₂纳米晶催化剂，结合谱学和电镜表征方法，以及CO吸附原位红外光谱，系统研究了CuO_x物种在不同形貌CeO₂纳米晶上的结构演化及其催化CO氧化的构-效关系.
结构表征结果表明，CuO_x物种结构不仅依赖于Cu的担载量，也依赖于载体CeO₂的形貌.随着Cu担载量的增加，CuO_x物种优先沉积在CeO₂的表面缺陷位，然后聚集和长大；同时伴随着CuO_x物种从孤立Cu离子到与载体强/弱相互作用的CuO_x团簇，高分散CuO颗粒和大尺寸CuO颗粒.孤立Cu⁺离子和与载体弱相互作用CuO_x团簇主要形成于CeO₂纳米立方体的表面，这可能与CeO₂纳米立方体暴露的氧终止CeO₂{100}晶面相关.CO吸附原位红外结果表明，CuO_x团簇与不同CeO₂表面相互作用的强度顺序为：CeO₂纳米棒暴露的{110}面 > CeO₂纳米多面体暴露的{111}面 > CeO₂纳米立方体暴露的{100}面.CeO₂纳米立方体与Cu²⁺离子间相互作用弱于与Cu⁺之间的，因此CeO₂纳米立方体负载的CuO_x物种在CO还原过程中容易停留在稳定的Cu⁺中间物种；而CeO₂纳米棒与Cu²⁺离子之间的相互作用强于与Cu⁺之间的相互作用，因此CeO₂纳米棒负载的CuO_x物种在CO还原过程中容易形成金属铜.因此CO吸附原位红外光谱观察到CeO₂纳米立方体负载CuO_x催化剂中吸附在Cu⁺的CO物种远远多于CeO₂纳米棒负载CuO_x催化剂.
CO氧化反应结果表明，CuO_x/CeO₂催化剂表现出同时依赖于CuO_x物种结构和CeO₂形貌的结构敏感性.CuO_x/CeO₂催化剂活性表现出与CuO_x/CeO₂催化剂的CO还原性能的正相关性，说明中CuO_x/CeO₂催化CO氧化反应遵循MvK反应机理.这些结果系统地关联了CeO₂形貌，CuO_x-CeO₂相互作用，CuO_x物种结构和CeO₂还原性能，CuO_x/CeO₂催化CO氧化反应活性.

关键词: CeO₂纳米晶, CuO_x/CeO₂催化剂, 金属-载体相互作用, CO氧化反应, 形貌效应

Abstract: Elucidation of the CuO_x-CeO₂ interactions is of great interest and importance in understanding complex CuO_x-CeO₂ interfacial catalysis in various reactions. In the present work, we have investigated structures and catalytic activity in CO oxidation of CuO_x species on CeO₂ rods, cubes and polyhedra predominantly exposing {110}+{100}, {100} and {111} facets by the incipient wetness impregnation method with the lowest Cu loading of 0.025%. The structural evolution of CuO_x species was found to depend on both the Cu loading and the CeO₂ morphology. As the Cu loading increases, CuO_x species are deposited preferentially on the surface defect of CeO₂ and then aggregate and grow, accompanied by the formation of isolated Cu ions, CuO_x clusters strongly/weakly interacting with the CeO₂, highly dispersed CuO nanoparticles, and large CuO nanoparticles. The isolated Cu⁺ species and CuO_x clusters weakly interacting with the CeO₂ were observed mainly on the O-terminated CeO₂{100} facets. Meanwhile, more Cu(I) species are stabilized during CO reduction processes in CuO_x/c-CeO₂ catalysts than in CuO_x/r-CeO₂ and CuO_x/p-CeO₂ catalysts. The catalytic activities of various CuO_x/CeO₂ catalysts in CO oxidation vary with both the CuO_x species and the CeO₂ morphology. These results comprehensively elucidate the CuO_x-CeO₂ interactions and exemplify their morphology-dependence.

Key words: CeO₂ nanocrystals, CuO_x/CeO₂ catalysts, Metal-support interactions, CO oxidation, Morphology effect

高玉仙, 张振华, 李兆瑞, 黄伟新. 从头开始理解形貌依赖的CuO_x-CeO₂相互作用[J]. 催化学报, 2020, 41(6): 1006-1016.

Yuxian Gao, Zhenhua Zhang, Zhaorui Li, Weixin Huang. Understanding morphology-dependent CuO_x-CeO₂ interactions from the very beginning[J]. Chinese Journal of Catalysis, 2020, 41(6): 1006-1016.

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从头开始理解形貌依赖的CuO_x-CeO₂相互作用

Understanding morphology-dependent CuO_x-CeO₂ interactions from the very beginning

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