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首页> 外文期刊>Advanced functional materials >Pyrrolic N-Stabilized Monovalent Ni Single-Atom Electrocatalyst for Efficient CO_2 Reduction: Identifying the Role of Pyrrolic–N and Synergistic Electrocatalysis
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Pyrrolic N-Stabilized Monovalent Ni Single-Atom Electrocatalyst for Efficient CO_2 Reduction: Identifying the Role of Pyrrolic–N and Synergistic Electrocatalysis

机译：Pyrrolic N-Stabilized Monovalent Ni Single-Atom Electrocatalyst for Efficient CO_2 Reduction: Identifying the Role of Pyrrolic–N and Synergistic Electrocatalysis

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Engineering the electronic structure of metal, N-doped carbon catalysts is apotential strategy for increasing the activity and selectivity of CO_2 electroreductionreaction (CO_2RR). However, establishing a definitive link betweenstructure and performance is extremely difficult due to constrained synthesisapproaches that lack the ability to precisely control the specific local environmentof M-N-C catalysts. Herein, a soft-template aided technique is developedfor the first time to synthesize pyrrolic N_4-Ni sites coupled with varyingN-type defects to synergistically enhance the CO_2RR performance. Theoptimal catalyst helps attain a CO Faradaic efficiency of 94% at a low potentialof ?0.6 V and CO partial current density of 59.6 mA cm~(?2) at ?1 V. Resultsof controlled experimental investigations indicate that the synergy betweenNi-N_4 and metal free defect sites can effectively promote the CO_2RR activity.Theoretical calculations revealed that the pyrrolic N coordinated Ni-N_4 sitesand C atoms next to pyrrolic N (pyrrolic N-C) have a lower energy barrier forthe formation of COOH* intermediate and optimum CO* binding energy. Thepyrrolic N regulate the electronic structure of the catalyst, resulting in lowerCO_2 adsorption energy and higher intrinsic catalytic activity.

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