Enhanced carbon dioxide electrolysis at redox manipulated interfaces

Wenyuan Wang,Kui Xie,John P Lemmon,Lizhen Gan,Fanglin Chen,John T S Irvine

doi:10.1038/s41467-019-09568-1

Abstract

Utilization of carbon dioxide from industrial waste streams offers significant reductions in global carbon dioxide emissions. Solid oxide electrolysis is a highly efficient, high temperature approach that reduces polarization losses and best utilizes process heat; however, the technology is relatively unrefined for currently carbon dioxide electrolysis. In most electrochemical systems, the interface between active components are usually of great importance in determining the performance and lifetime of any energy materials application. Here we report a generic approach of interface engineering to achieve active interfaces at nanoscale by a synergistic control of materials functions and interface architectures. We show that the redox-manipulated interfaces facilitate the atomic oxygen transfer from adsorbed carbon dioxide molecules to the cathode lattice that determines carbon dioxide electrolysis at elevated temperatures. The composite cathodes with in situ grown interfaces demonstrate significantly enhanced carbon dioxide electrolysis and improved durability.

Highlights

Utilization of carbon dioxide from industrial waste streams offers significant reductions in global carbon dioxide emissions
We develop new generic approaches of manipulation of active metal–oxide interfaces considering cathodes ranging from metallic nickel to Ni–YSZ cermet, CeO2−δ, and Nb1.33(Ti0.8M0.2)0.67O4 (M = Mn,Cr) ceramic compositions, through control of phase decomposition during reduction
Nickel element is exclusively present as Ni2+ while manganese is present in the form of Mn2+, Mn3+, and Mn4+ in the sample, as shown in X-ray photoelectron spectroscopy (XPS) in Supplementary Fig. 118

Summary

Introduction

Utilization of carbon dioxide from industrial waste streams offers significant reductions in global carbon dioxide emissions. We show that the redox-manipulated interfaces facilitate the atomic oxygen transfer from adsorbed carbon dioxide molecules to the cathode lattice that determines carbon dioxide electrolysis at elevated temperatures. The active interface for metallic cathodes where CO2 splitting reactions proceed is normally located on the electrolyte surface with intimate contact with porous metal phase. Loading of metal or oxide nanoparticles in porous nickel, Ni–YSZ scaffold and titanate electrode to ex situ assemble interfaces, all have demonstrated the successful manipulation of nanostructures at interfaces aiming at electrode activity enhancement. In situ exsolved metal/oxide interfaces with strong interactions would provide the possibility to facilitate atomic oxygen transfer process These exsolved metal–oxide interface through phase decomposition has been demonstrated to be effective to enhance CO2 electrolysis

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Results

Conclusion