Revealing the Crystal Facet Effect of Ceria in Pd/CeO2 Catalysts toward the Selective Oxidation of Benzyl Alcohol

被引:68
作者
Zhang, Leijie [1 ,2 ]
Chen, Runhua [3 ]
Tu, Yi [1 ,2 ]
Gong, Xiaoyu [1 ,2 ]
Cao, Xu [1 ,2 ]
Xu, Qian [1 ,2 ]
Li, Yu [1 ,2 ]
Ye, Bangjiao [3 ]
Ye, Yifan [1 ,2 ]
Zhu, Junfa [1 ,2 ]
机构
[1] Univ Sci & Technol China, Dept Chem Phys, Natl Synchrotron Radiat Lab, Hefei 230029, Peoples R China
[2] Univ Sci & Technol China, Key Lab Surface & Interface Chem Energy Catalysis, Hefei 230029, Peoples R China
[3] Univ Sci & Technol China, State Key Lab Particle Detect & Elect, Hefei 230026, Anhui, Peoples R China
基金
国家重点研发计划; 中国国家自然科学基金;
关键词
ceria; crystal facet effect; supported Pd catalyst; oxygen vacancy; alcohol oxidation; multistep reaction; METAL-SUPPORT INTERACTION; CO OXIDATION; CEO2; NANOCRYSTALS; OXYGEN VACANCIES; MORPHOLOGY; OXIDE; NANORODS; PLANE; PD; PERFORMANCE;
D O I
10.1021/acscatal.2c04252
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Ceria is an excellent catalyst or support for various oxidation reactions due to its abundant oxygen vacancies and strong metal-support interactions. In this study, ceria nanocrystals were hydrothermally prepared with different morphologies (nanorods, nanocubes, and nano-octahedra) and corresponding exposed crystal facets [(110), (100), and (111)]. The Pd/CeO2 catalysts were synthesized through an impregnation method by applying these ceria nanocrystals as supports. Selective oxidation of benzyl alcohol, involving multiple catalytic steps, was employed as a model reaction to explore the crystal facet effect of ceria on the catalytic activity of various Pd/CeO2 catalysts. The Pd/CeO2 nanorod catalyst delivers superior performance in each individual step, resulting in an improved overall catalytic activity. Specifically, the highest oxygen vacancy concentration and the optimum metal-support synergy observed on the CeO2 (110) surface are feasible to dissociate the benzyl alcohol adsorbent, eliminate alpha-H, and activate O2. As a consequence, the Pd/CeO2-nanorod catalysts deliver a much higher benzyl alcohol conversion (74%) than Pd/CeO2-nano-octahedra (35%) and Pd/CeO2-nanocubes (28%). This work provides in-depth insight into the crystal facet-performance relationship of CeO2 in the selective oxidation of benzyl alcohol and sheds light on the catalyst support design strategy for other multistep reactions.
引用
收藏
页码:2202 / 2213
页数:12
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