Pulse Plating of Copper onto Gas Diffusion Layers for the Electroreduction of Carbon Dioxide
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MRS Advances © 2017 Materials Research Society DOI: 10.1557/adv.2017.623
Pulse Plating of Copper onto Gas Diffusion Layers for the Electroreduction of Carbon Dioxide Sujat Sen 1, McLain Leonard 1, Rajeswaran Radhakrishnan 2, Stephen Snyder 2, Brian Skinn 2, Dan Wang 2, Timothy Hall 2, E. Jennings Taylor 2 and Fikile R. Brushett 1 1
Department of Chemical Engineering, Massachusetts Institute of Technology, Cambridge, MA, 02139, USA
2
Faraday Technology, Inc., Englewood, OH, 45315, USA
ABSTRACT
This paper discusses a pulse electroplating method for preparing copper (Cu)-coated gas diffusion electrodes (GDEs) for the electrochemical conversion of carbon dioxide (CO2) to hydrocarbons such as ethylene. Ionomer coating and air-plasma surface pre-treatments were explored as means of hydrophilizing the carbon surface to enable adhesion of electrodeposited material. The pulsed-current electrodeposition method used successfully generated copper and copper oxide micro- and nano-particles on the prepared surfaces. Copper(I) species identified on the ionomer-treated GDEs are presumed to be highly active for the selective generation of ethylene as compared to other gaseous byproducts of CO2 reduction. Conversely, copper catalysts deposited onto plasma-treated GDEs were found to have poor activity for hydrocarbon production, likely due to substantial metallic character. Of note, plasma treatment of an ionomer-treated GDE after copper plating yielded further improvements in catalytic activity and durability towards ethylene production.
INTRODUCTION Utilizing carbon dioxide (CO2) as a chemical feedstock has been identified as a means of reducing greenhouse gas emissions and moving towards a carbon neutral energy cycle [1]. A promising approach for CO2 conversion is electrocatalytic reduction to selectively generate hydrocarbons such as ethylene and propylene that are the primary building blocks of the petrochemical industry. The production of these precursors by conventional means from petroleum feedstocks is energy intensive, requiring high temperatures and pressures [1]. Hence, electrochemical methods, which can operate at milder conditions, represent a potentially less expensive and sustainable alternative, provided key performance metrics are realized [2]. Prior reports have demonstrated electroreduction of CO2 to hydrocarbons on copper (Cu)-coated gas diffusion electrodes (GDEs) to obtain ethylene (C2H4). For example, Ma et al. reported a partial current density of 140 mA/cm2 to C2H4 at a potential of -0.8 V versus the reversible hydrogen electrode (RHE) [3]. These studies have typically used Cu nanoparticles (NPs) that are mixed with an ionomer and spray-coated onto a microporous carbon layer (MPL)
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supported by a carbon fiber substrate (CFS), to form a GDE; the composite substrate pr
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