Abstract

Carbon dioxide electroreduction provides a useful source of carbon monoxide, but comparatively few catalysts could be sustained at current densities of industry level. Herein, we construct a high-yield, flexible and self-supported single-atom nickel-decorated porous carbon membrane catalyst. This membrane possesses interconnected nanofibers and hierarchical pores, affording abundant effective nickel single atoms that participate in carbon dioxide reduction. Moreover, the excellent mechanical strength and well-distributed nickel atoms of this membrane combines gas-diffusion and catalyst layers into one architecture. This integrated membrane could be directly used as a gas diffusion electrode to establish an extremely stable three-phase interface for high-performance carbon dioxide electroreduction, producing carbon monoxide with a 308.4 mA cm−2 partial current density and 88% Faradaic efficiency for up to 120 h. We hope this work will provide guidance for the design and application of carbon dioxide electro-catalysts at the potential industrial scale.

Highlights

  • Carbon dioxide electroreduction provides a useful source of carbon monoxide, but comparatively few catalysts could be sustained at current densities of industry level

  • The fabrication method of NiSA/PCFM membrane is described in Fig. 1a, which involves electrospinning process and heated treatment

  • density functional theory (DFT) calculations based on *COOH intermediate provide a molecular understanding of the observed high efficiency on singleatom Ni sites

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Summary

Introduction

Carbon dioxide electroreduction provides a useful source of carbon monoxide, but comparatively few catalysts could be sustained at current densities of industry level. The excellent mechanical strength and well-distributed nickel atoms of this membrane combines gas-diffusion and catalyst layers into one architecture This integrated membrane could be directly used as a gas diffusion electrode to establish an extremely stable three-phase interface for high-performance carbon dioxide electroreduction, producing carbon monoxide with a 308.4 mA cm−2 partial current density and 88% Faradaic efficiency for up to 120 h. CO2 is supplied from the gaseous phase through a gas-diffusion layer to construct a gas–liquid interface adjoined to the solid catalyst layer This unique architecture has the potential to deliver enough CO2 directly onto the catalyst surface and reach very high current densities. This integrated NiSA/PCFM membrane could be immediately utilized as GDE compartment for highperformance CO2 reduction, avoiding the weak connection between the substrate and electro-catalyst

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