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Electrochemical synthesis based on electron as reagents provide a broad prospect for commodity chemical manufacturing. A direct one-step route from amino C-N bonds electrooxidation to nitrile C≡N bonds offer an alternative pathway for nitriles producting. However, this promising topic has not been fully explored whether the chemical bond reforming process or the performance optimization. Here we proposed a model of vacancies-rich Ni(OH)2 atomic layer to understand performance relationship with structure. By theory calculations, the vaca