Electrocatalytic Reduction of CO2 at Au Nanoparticle Electrodes: Effects of Interfacial Chemistry on Reduction Behavior

Andrews, Evan; Katla, Sai; Kumar, Challa; Patterson, Matthew; Sprunger, Phillip; Flake, John

doi:10.1149/2.0541512jes

Title: Electrocatalytic Reduction of CO₂ at Au Nanoparticle Electrodes: Effects of Interfacial Chemistry on Reduction Behavior

Journal Article · Sat Sep 12 00:00:00 EDT 2015 · Journal of the Electrochemical Society

DOI:https://doi.org/10.1149/2.0541512jes· OSTI ID:1369704

Andrews, Evan ^[1]; Katla, Sai ^[1]; Kumar, Challa ^[1]; Patterson, Matthew ^[1]; Sprunger, Phillip ^[1]; Flake, John ^[1]

Louisiana State Univ., Baton Rouge, LA (United States)

Nanoscale Au electrocatalysts demonstrate the extraordinary ability to reduce CO₂ at low overpotentials with high selectivity to CO. Here, we investigate the role of surface chemistry on CO₂ reduction behavior using Au₂₅ and 5 nm Au nanoparticles. Onset potentials for CO₂ reduction at Au₂₅ nanoparticles in Nafion binders are shifted anodically by 190 mV while the hydrogen evolution reaction is shifted cathodically by 300 mV relative to Au foil. The net effect of this beneficial separation in onset potentials is relatively high Faradayic efficiencies for CO (90% at 0.8 V versus RHE) at high current densities. Experimental results show Faradayic efficiencies for CO are greatest using electrodes made with Nafion-immobilized Au₂₅ nanoparticles. Likewise, CO₂ reduction onset potential shifts are greater for smaller nanoparticles and when Nafion binders are used instead of (sulfonate-free) polyvinylidene fluoride. X-ray photoelectron spectroscopy analysis reveals Au nanoparticles may react with the sulfonates of Nafion binders. Here, the results suggest sulfonate interfaces may alter the binding energies of key species or lead to favorable reconstructions, either of which ultimately results in remarkable improvements in Faradayic efficiencies relative to Au foil electrodes.

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Research Organization:: Energy Frontier Research Centers (EFRC), Washington, D.C. (United States). Center for Atomic-Level Catalyst Design (CALCD)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0001058

OSTI ID:: 1369704

Journal Information:: Journal of the Electrochemical Society, Vol. 162, Issue 12; Related Information: CALCD partners with Louisiana State University (lead); Clemson University; University of Florida; Georgia Institute of Technology; Grambling State University; Oak Ridge National Laboratory; Ohio State University; Pennsylvania State; Texas A&M University; Vienna University of Technology, Austria; University of Utrecht, Netherlands; ISSN 0013-4651

Publisher:: The Electrochemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 42 works

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
carbon dioxide
electrocatalyst
gold
Nafion
reduction

Title: Electrocatalytic Reduction of CO2 at Au Nanoparticle Electrodes: Effects of Interfacial Chemistry on Reduction Behavior

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