Diving into the interface-mediated Mars-van Krevelen (M-vK) characteristic of CuOx-supported CeO2 catalysts

被引:26
作者
Tang, Tian [1 ,2 ]
Ye, Lyumeng [3 ]
Chen, Yanrong [1 ,2 ]
Xue, Jingyu [1 ,2 ]
Shen, Xiaoqiang [1 ,2 ]
Chen, Jinfei [1 ,2 ]
Quarcoo, Fiona Hammond [4 ]
Rac, Vladislav [5 ]
Rakic, Vesna [5 ]
Li, Xinbao [6 ]
Du, Xuesen [1 ,2 ]
机构
[1] Chongqing Univ, Key Lab Low Grade Energy Utilizat Technol & Syst, Minist Educ PRC, Chongqing 400044, Peoples R China
[2] Chongqing Univ, Sch Energy & Power Engn, 174 Shazhengjie, Chongqing 400044, Peoples R China
[3] Minist Ecol & Environm PRC, South China Inst Environm Sci, Guangdong Prov Engn Lab Air Pollut Control, Guangzhou 510655, Peoples R China
[4] Nanjing Tech Univ, Coll Chem Engn, State Key Lab Mat Oriented Chem Engn, Nanjing 211816, Peoples R China
[5] Univ Belgrade, Fac Agr, Nemanjina 6, Zemun Belgrade 11080, Serbia
[6] China Jiliang Univ, Coll Metrol & Measurement Engn, Hangzhou 310018, Peoples R China
关键词
Copper-ceria interface; DFT plus U; CO oxidation; Mars-van Krevelen (M-vK); CO OXIDATION; CERIA CATALYSTS; PREFERENTIAL OXIDATION; EXCESS H-2; SURFACE; OXYGEN; IDENTIFICATION; DEPENDENCE; REDUCTION; MECHANISM;
D O I
10.1016/j.apcatb.2023.123368
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
The unique interface synergistic catalytic properties for metal oxide-supported catalysts have long been explored in several critical heterogeneous catalytic processes (e.g., CO oxidation reactions). However, interfacial synergistic catalysis is still a hitherto undescribed mechanism due to the lack of direct evidence at the atomic level. Thereinto, the CuOx-supported CeO2 (CuOx/CeO2) catalyst is a typical case. Herein, a combination study including representative theoretical calculations, in situ DRIFTS spectra and tailored molecular probe experiments supports a new carbonate-interface mediated Mars-van Krevelen (M-vK) mechanism for CO oxidation, i. e., CO molecules form carbonate intermediate species directly between spatial proximity (2.99 angstrom) double lattice oxygen sites with low oxygen vacancies formation energy (EformOv = 0.82 eV/0.83 eV) at the copper-ceria interface. The reaction energy barrier of this process is 0.32 eV, much lower than the 1.23 eV of the conventional M-vK mechanism. Besides, the spatial effect of double oxygen vacancies (Ov) generated by the depletion of intermediate carbonate species promotes the sustained and dynamic activation of O2, hence facilitating the efficient operation of the M-vK mechanism at low temperatures.
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页数:10
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