Nitrided copper-iron composite oxides derived from layered double hydroxides for enhanced carbon dioxide electroreduction to methane and formic acid

Dian  Song; Jinqing  He; Yiping  Wang; Xuhui  Zhao; Fazhi  Zhang; Xiaodong Lei

doi:10.59400/esc.v2i2.369

Nitrided copper-iron composite oxides derived from layered double hydroxides for enhanced carbon dioxide electroreduction to methane and formic acid

Dian Song State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China
Jinqing He State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China
Yiping Wang State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China; Quzhou Institute for Innovation in Resource Chemical Engineering, Quzhou 324000, Zhejiang Province, China
Xuhui Zhao State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China
Fazhi Zhang State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China
Xiaodong Lei State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China; Quzhou Institute for Innovation in Resource Chemical Engineering, Quzhou 324000, Zhejiang Province, China

Article ID: 369

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DOI: https://doi.org/10.59400/esc.v2i2.369

Keywords: CuFe-LDH; nitrided copper-iron oxides; CO2 electroreduction; electrocatalysis

Abstract

The reduction of carbon dioxide into valuable chemical products is a promising solution to address carbon balance and energy issues. Herein, amorphous nitrided copper-iron oxides are prepared by gas-phase nitriding of CuFe-layered double hydroxide precursors with urea as a nitrogen source. The obtained materials show high activity for CO₂ electroreduction to methane and formic acid, achieving a total Faraday efficiency of 74.7% at −0.7 V vs. RHE and exhibiting continuous 10 h durability in the H-cell. The uniformly distributed Cu+ sites act as active sites by losing electrons to activate CO₂. During the CO₂ electroreduction, CO₂ is converted to *COOH via proton-electron coupling; *COOH combines directly with a proton in solution to produce the HCOOH product; and the other part of *COOH undergoes a protonated dehydration process to form the *CHO intermediate, which dehydrates again to form CH₄. This study provides a new approach for designing CO₂ electroreduction catalysts.

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Published

2024-05-08

How to Cite

Song, D., He, J., Wang, Y., Zhao, X., Zhang, F., & Lei, X. (2024). Nitrided copper-iron composite oxides derived from layered double hydroxides for enhanced carbon dioxide electroreduction to methane and formic acid. Energy Storage and Conversion, 2(2), 369. https://doi.org/10.59400/esc.v2i2.369

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Nitrided Copper-Iron Composite Oxides Derived from Layered Double Hydroxides for Enhanced Carbon Dioxide Electroreduction to Methane and Formic Acid

The reduction of carbon dioxide to valuable chemical products is a promising solution to address carbon balance and energy issues. Herein, amorphous nitrided copper-iron oxides are prepared by gas-phase nitriding of Cu Fe-layered double hydroxide precursor s with urea as nitrogen source. Amorphous materials are more likely to generate defect vacancies during the reaction process, and these vacancies can function as active sites for catalytic reactions. Therefore, the obtained materials show high activity for CO 2 electroreduction to methane and formic acid, achieving a total Faraday efficiency of 74.7% at −0.7 V vs RHE and exhibiting a continuous 10 h durability in the H-cell. The uniformly distributed Cu + sites act as active sites by losing electrons to activate CO 2 . During the CO 2 electroreduction , CO 2 is converted to *COOH via proton-electron coupling, *COOH combines directly with a proton in solution to produce the HCOOH product, and the other part of *COOH undergoes a protonated dehydration process to form the *CHO intermediate which dehydrates again to form CH 4 . This study provides a new approach for designing CO 2 electroreduction catalysts.

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