Abstract

Co-electrolysis of carbon dioxide and steam has been shown to be an efficient way to produce syngas, however further optimisation requires detailed understanding of the complex reactions, transport processes and degradation mechanisms occurring in the solid oxide cell (SOC) during operation. Whilst electrochemical measurements are currently conducted in situ, many analytical techniques can only be used ex situ and may even be destructive to the cell (e.g. SEM imaging of the microstructure). In order to fully understand and characterise co-electrolysis, in situ monitoring of the reactants, products and SOC is necessary. Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS) is ideal for in situ monitoring of co-electrolysis as both gaseous and adsorbed CO and CO2 species can be detected, however it has previously not been used for this purpose. The challenges of designing an experimental rig which allows optical access alongside electrochemical measurements at high temperature and operates in a dual atmosphere are discussed. The rig developed has thus far been used for symmetric cell testing at temperatures from 450 °C to 600 °C. Under a CO atmosphere, significant changes in spectra were observed even over a simple Au|10Sc1CeSZ|Au SOC. The changes relate to a combination of CO oxidation, the water gas shift reaction, carbonate formation and decomposition processes, with the dominant process being both potential and temperature dependent.

Highlights

  • Electrochemical devices based on solid-state ceramic electrolytes have a wide range of applications from sensors to membrane reactors; batteries to fuel cells

  • In this paper we report the development of a modi ed commercial Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS) unit for the study of solid oxide cells (SOC) under operating conditions

  • DRIFTS data recorded at 450 C show distinct peaks at 3245, 2360 and 1320–1896 cmÀ1

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Summary

Introduction

Electrochemical devices based on solid-state ceramic electrolytes have a wide range of applications from sensors to membrane reactors; batteries to fuel cells. One of the attractive features of these devices is their exibility and efficiency when operated at high temperature. It was recognised very early on that solid oxide cells (SOC) were capable of reverse operation in electrolysis mode, for example the pioneering work of Doenitz et al.[1,2] on steam electrolysis. Recent research interest has focused on the co-electrolysis of steam and carbon dioxide for the single-step production of syngas. This process is attractive because it represents an efficient route to producing synthetic liquid hydrocarbon fuels with all of the associated bene ts of high energy density, transport infrastructure and ease of handling. The efficient conversion of electricity into an energydense chemical offers the possibility for commercially viable large-scale energy storage

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