1. Customizing pyridinic nitrogen coordination in Ni-N-C for electrocatalytic CO 2 reduction towards CO.
- Author
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Ai Y, Zhang K, Li J, Du X, Wang Y, Wu L, and Zhang Z
- Abstract
Nickel anchored N-doped carbon electrocatalysts (Ni-N-C) are rapidly developed for the electrochemical reduction reaction of carbon dioxide (CO
2 RR). However, the high-performanced Ni-N-C analogues design for CO2 RR remains bewilderment, for the reason lacking of definite guidance for its structure-activity relationship. Herein, the correlation between the proportion of nitrogen species derived from various nitrogen sources and the CO2 RR activity of Ni-N-C is investigated. The x-ray photoelectron spectroscopy (XPS) spectrum combined with the CO2 RR performance results show that pyridinic-N content has a positive correlation with CO2 RR activity. Moreover, density functional theory (DFT) demonstrates that pyridinic-N coordinated Ni-N4 sites offers optimized free energy and favorable selectivity towards CO2 RR compared with pyrrolic-N. Accordingly, Ni-Na -C with highest pyridinic-N content (ammonia as nitrogen source) performs superior CO2 RR activity, with the maximum carbon monoxide faradaic efficiency (FECO ) of 99.8% at -0.88 V vs. RHE and the FECO surpassing 95% within potential ranging of -0.88 to -1.38 V vs. RHE. The building of this parameter for CO2 RR activity of Ni-N-C give instructive forecast for low-cost and highly active CO2 RR electrocatalysts., (© 2024 IOP Publishing Ltd.)- Published
- 2024
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