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E02-JEM ARM 300CF	General synthesis and definitive structural identification of MN4C4 single-atom catalysts with tunable electrocatalytic activities Huilong Fei , Juncai Dong , Yexin Feng , Christopher Allen , Chengzhang Wan , Boris Volosskiy , Mufan Li , Zipeng Zhao , Yiliu Wang , Hongtao Sun , Pengfei An , Wenxing Chen , Zhiying Guo , Chain Lee , Dongliang Chen , Imran Shakir , Mingjie Liu , Tiandou Hu , Yadong Li , Angus I. Kirkland , Xiangfeng Duan , Yu Huang Nature Catalysis 1, 63 - 72 DOI: 10.1038/s41929-017-0008-y Diamond Proposal Number(s): [16967] Show Abstract ▼ Abstract: Single-atom catalysts (SACs) have recently attracted broad research interest as they combine the merits of both homogeneous and heterogeneous catalysts. Rational design and synthesis of SACs are of immense significance but have so far been plagued by the lack of a definitive correlation between structure and catalytic properties. Here, we report a general approach to a series of monodispersed atomic transition metals (for example, Fe, Co, Ni) embedded in nitrogen-doped graphene with a common MN4C4 moiety, identified by systematic X-ray absorption fine structure analyses and direct transmission electron microscopy imaging. The unambiguous structure determination allows density functional theoretical prediction of MN4C4 moieties as efficient oxygen evolution catalysts with activities following the trend Ni > Co > Fe, which is confirmed by electrochemical measurements. Determination of atomistic structure and its correlation with catalytic properties represents a critical step towards the rational design and synthesis of precious or nonprecious SACs with exceptional atom utilization efficiency and catalytic activities.	Jan 2018

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E02-JEM ARM 300CF

General synthesis and definitive structural identification of MN4C4 single-atom catalysts with tunable electrocatalytic activities