Catalytic role of assembled Ce Lewis acid sites over ceria for electrocatalytic conversion of dinitrogen to ammonia
Catalytic role of assembled Ce Lewis acid sites over ceria for electrocatalytic conversion of dinitrogen to ammonia
复制标题
DOI：
10.1016/j.jechem.2021.01.016
复制
发表时间：
2021-02-09
影响因子：
13.1
通讯作者：
Lin, Sen
中科院分区：
文献类型：
--
作者：
Qi, Jiamin;Zhou, Shulan;Lin, Sen
CeO2-based catalysts are emerging as novel candidates for catalyzing nitrogen reduction reaction (NRR). However, despite the increasing amount of experimental and theoretical research, the design of more efficient ceria catalysts for NRR remains a challenge due to the poor knowledge of the catalytic mechanism, particularly the nature of the active sites and how they catalyze NRR. Here, using first-principle calculations, we investigated the NRR catalysis process involving adjacent Ce Lewis acid clusters formed on (111), (110), and (100) facets of CeO2 as active sites. Our results revealed that the assembled structures of the Ce Lewis acid as active centers after the oxygen vacancies (Ovs) were opened. The exposed Ce sites on CeO2(111), CeO2(110), and CeO2(100) can cause N-2 to be adsorbed in a manner, which facilitates the N-2 activation and thus leads to much higher NRR activity. Furthermore, from the perspective of electronic structure, we establish two useful descriptors for assessing the NRR activity on ceria with O(v)s: The N-N bond strength of the adsorbed N-2 and the adsorption energy of the *N2H intermediate. This work thus provides direct guidance for the design of more-effective oxide catalysts without the use of scarce metals. (c) 2021 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved.
