Identifying operating mechanism in the electrochemical reduction of CO 2 on thin-film praseodymium-doped ceria electrode

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Identifying operating mechanism in the electrochemical reduction of CO2 on thin-film praseodymium-doped ceria electrodes Neetu Kumari 1 & M. Ali Haider 2 & Uzma Anjum 2 & Suddhasatwa Basu 2 Received: 23 May 2020 / Revised: 5 July 2020 / Accepted: 3 August 2020 # Springer-Verlag GmbH Germany, part of Springer Nature 2020

Abstract Dense thin-film electrodes of Ce0.9Pr0.1O1.95 (PDC) are tested for CO2 reduction in a solid oxide electrolysis cell (SOEC) with yttria-stabilized-zirconia (YSZ) electrolyte and La0.8Sr0.2MnO3-δ (LSM) air electrode. A spray pyrolysis technique is utilized to fabricate thin-film electrodes of PDC with an approximate thickness of 400 nm. Dense microstructure in the thin film is fabricated to understand the relative role and limitations offered by surface reaction and oxygen anion diffusion within the bulk of the PDC electrodes while disallowing any gas phase diffusion. Electrochemical tests are performed in a geometrically well-defined cell to ascertain the operating mechanism. Electrochemical reduction of CO2 is carried out in the SOEC mode on the PDC electrode. Cu is added to the surface of the dense thin film of PDC. Polarization resistance of the thin-film electrode measured at the opencircuit voltage, in an H2/CO2 (8% H2) environment, is observed to reduce by 45% on adding Cu at the surface of the electrode. This suggested that the electrocatalytic activity of the thin-film electrode is limited by sluggish surface activity, which is improved on adding the surface with Cu. Keywords CO2 reduction . Solid oxide electrolysis cell . Electrochemical performance . Thin film . Praseodymium-doped ceria

Introduction Rising CO2 level in the atmosphere is raising awareness about global warming [1]. While the direct impact of CO2 concentration in the atmosphere to the changing climate is rigorously debated, one indirect impact, which is relatively easier to assess, is on the rising acidification of the seawater, leading to ecological imbalance and deaths of corals, that can not be ignored [2]. Sequestration offers an easy way to remove most of the CO2 from the atmosphere [3]. While sequestration techniques are currently being developed, an indirect way of Electronic supplementary material The online version of this article (https://doi.org/10.1007/s11581-020-03731-1) contains supplementary material, which is available to authorized users. * M. Ali Haider [email protected] * Suddhasatwa Basu [email protected] 1

Department of Chemical Engineering, Malaviya National Institute of Technology Jaipur, Jaipur 3012017, India

2

Department of Chemical Engineering, Indian Institute of Technology Delhi, New Delhi 110016, India

shifting the slope of rising CO2 levels in the atmosphere for another 100 years or more could be chemical conversion of CO2 into useful products [4]. Our review on catalytic and electrocatalytic methods available for CO2 reduction offers a detailed overview of routes for chemical conversion [5, 6]. Herein, we are focused on developing a high-temperature solid oxide elect