Journal
JOURNAL OF ENERGY CHEMISTRY
Volume 85, Issue -, Pages 267-275Publisher
ELSEVIER
DOI: 10.1016/j.jechem.2023.06.024
Keywords
CO 2 reduction; Methanol oxidation reaction; Formate; Layered double hydroxides; Oxygen vacancies
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Self-supported ultrathin NiCo layered double hydroxides (LDHs) electrodes were fabricated as an anode for methanol electrooxidation to achieve high formate production coupled with CO2 electro-reduction. The total formate faradic efficiency of both anode and cathode can reach up to 188% driven by a low cell potential. This work presents a promising approach for fabricating advanced electrodes towards electrocatalytic reactions.
Electrochemical CO2 reduction into energy-carrying compounds, such as formate, is of great importance for carbon neutrality, which however suffers from high electrical energy input and liquid products crossover. Herein, we fabricated self-supported ultrathin NiCo layered double hydroxides (LDHs) electrodes as anode for methanol electrooxidation to achieve a high formate production rate (5.89 mmol h-1 cm-2) coupled with CO2 electro-reduction at the cathode. A total formate faradic efficiency of both anode for methanol oxidation and cathode for CO2 reduction can reach up to 188% driven by a low cell potential of only 2.06 V at 100 mA cm-2 in membrane-electrode assembly (MEA). Physical characterizations demonstrated that Ni3+ species, formed on the electrochemical oxidation of Ni-containing hydroxide, acted as catalytically active species for the oxidation of methanol to formate. Furthermore, DFT calculations revealed that ultrathin LDHs were beneficial for the formation of Ni3+ in hydroxides and introducing oxygen vacancy in NiCo-LDH could decrease the energy barrier of the rate-determining step for methanol oxidation. This work presents a promising approach for fabricating advanced electrodes towards electrocatalytic reactions.& COPY; 2023 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved.
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