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Boosting Efficient Ammonia Synthesis over Atomically Dispersed Co-Based Catalyst via the Modulation of Geometric and Electronic Structures

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CCS Chemistry 2022年第5期4卷 1758-1769页

作者： Yanliang Zhou Congying Wang Xuanbei Peng Tianhua Zhang Xiuyun Wang Yafei Jiang Haifeng Qi Lirong Zheng Jianxin Lin Lilong Jiang National Engineering Research Center of Chemical Fertilizer Catalyst Fuzhou UniversityFuzhouFujian 350002 Department of Chemistry Southern University of Science and TechnologyShenzhen 518055 Dalian Institute of Chemical Physics Chinese Academy of SciencesDalian 116023 Institute of High Energy Physics Chinese Academy of SciencesBeijing 100049

Ammonia(NH_(3))synthesis at mild conditions is of great significance,while the significant bottleneck of this process is the activation of N_(2) to realize the desired NH_(3) synthesis performance,which requires deep insight and rational design of active sites at the atomic ***,were synthesized atomically dispersed Co-based catalysts with different Co-N coordination numbers(CNs)to explore the coordination-sensitive NH_(3) synthesis reaction for the first *** studies showed that Co-based catalysts increased the NH_(3) synthesis rate gradually with a decrease in *** Co-N_(2) catalyst exhibited the highest NH_(3) synthesis rate of 85.3 mmol gCo^(−1) h^(−1) at 300℃ and 1 MPa,which outperformed most of the previously reported Co-based *** characterizations and theoretical calculations demonstrated that atomically dispersed Co catalyst with low CN could generate more unoccupied Co 3d charges and tetrahedral cobalt(Ⅱ)*** unoccupied Co 3d charge,in turn,promoted the electron donation from the Co active center to the antibonding π-orbital(π*)of N_(2) and expedites N_(2) ***,the Co-N_(2) catalyst with more tetrahedral cobalt(II)sites could effectively facilitate the desorption of N-containing intermediate species(such as*NH_(3) and*N_(2)H_(4))to obtain a high NH_(3) synthesis rate.

关键词： ammonia synthesis coordination number electron transfer geometric structure intermediate species

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