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Asymmetricalπback-donation of hetero-dicationic Mo^(4+)-Mo^(6+)pairs for enhanced electrochemical nitrogen reduction

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Nano Research 2022年第4期15卷 3010-3016页

作者： Hao Tan Qianqian Ji Chao Wang Hengli Duan Yuan Kong Yao Wang Sihua Feng Liyang Lv Fengchun Hu Wenhua Zhang Wangsheng Chu Zhihu Sun Wensheng Yan National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230029China Hefei National Laboratory for Physical Sciences at the Microscale and Department of Chemical Physics and Synergetic Innovation Center of Quantum Information and Quantum PhysicsUniversity of Science and Technology of ChinaHefei 230029China

The breaking of nonpolar N≡N bond of dinitrogen is the biggest dilemma for electrocatalytic nitrogen reduction reaction(NRR)application,driving electron migration between catalysts and N≡N bond(termed“πback-donation”process)is crucial for attenuating interfacial energy barrier but still remains ***,using density functional theory calculations,we revealed that constructing a unique hetero-dicationic Mo^(4+)-Mo^(6+)pair could effectively activate N≡N bond with a lying-down chemisorption configuration by an asymmetrical“πback-donation”*** a proof-of-concept demonstration,we synthesized MoO_(2)@MoO_(3)heterostructure with double Mo sites(Mo^(4+)-Mo^(6+)),which are embedded in graphite,for electrochemical nitrogen ***,this hetero-dicationic Mo^(4+)-Mo^(6+)pair catalysts display more excellent catalytic performance with a high NH_(3)yield(60.9μg·h^(-1)·mg^(-1))and Faradic efficiency(23.8%)as NRR catalysts under ambient conditions than pristine MoO_(2)and MoO_(3).operando characterizations using synchrotron-based spectroscopic techniques identified the emergence of a key^(*)N_(2)Hy intermediate on Mo sites during NRR,which indicates that the Mo sites are active sites and the NRR process tends to follow an associative *** novel type of hetero-dicationic catalyst has tremendous potential as a new class of transition metal-based catalysts with promising applications in electrocatalysis and catalysts for energy conversion and storage.

关键词： asymmetrical"πback-donation"process hetero-dicationic Mo^(4+)–Mo^(6+)pairs nitrogen reduction reaction operando experimental characterizations

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