Electronic Structure Optimization of PdZn-Graphitic Carbon Nitride Nanocomposites as Electrocatalysts for Selective CO(2) to CO Conversion

钯锌-石墨氮化碳纳米复合材料的电子结构优化及其作为选择性CO₂转化为CO电催化剂的应用

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Abstract

Herein, a novel PdZn/g-C(3)N(4) nanocomposite electrocatalyst, PdZnGCN, prepared from a facile hydrothermal reduction procedure for an efficient CO(2) to CO conversion has been examined. This composite catalyst reduces CO(2) at a thermodynamic overpotential of 0.79 V versus RHE with a 93.6% CO Faradaic efficiency and a CO partial current density of 4.4 mA cm(-2). Moreover, the turnover frequency for PdZnGCN reaches 20 974 h(-1) with an average selectivity of 95.4% for CO after 1 h and an energy efficiency approaching 59%, which is superior to most reported noble metals and metal alloys as electrocatalysts. The enhanced catalytic activity of this nanocomposite is due to synergistic interactions between PdZn and g-C(3)N(4) as evidenced by optimum work function, zeta potential, CO desorption rate, and downshifted d-band center. Furthermore, suppressed grain growth during the formation of nanocomposites also results in faster reaction kinetics, as demonstrated by a lower Tafel slope (93.6 mV/dec) and a larger electrochemically active surface, consequently enhancing the overall performance.

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