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Electronic Structure Optimization of PdZn-Graphitic Carbon Nitride Nanocomposites as Electrocatalysts for Selective CO2 to CO Conversion

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Herein, a novel PdZn/g-C3N4 nanocomposite electrocatalyst, PdZnGCN, prepared from a facile hydrothermal reduction procedure for an efficient CO2 to CO conversion has been examined. This composite catalyst reduces CO2 at… Click to show full abstract

Herein, a novel PdZn/g-C3N4 nanocomposite electrocatalyst, PdZnGCN, prepared from a facile hydrothermal reduction procedure for an efficient CO2 to CO conversion has been examined. This composite catalyst reduces CO2 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-C3N4 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.

Keywords: optimization pdzn; structure optimization; electronic structure; co2 conversion; co2

Journal Title: ACS Omega
Year Published: 2022

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