Title: Polymer-supported CuPd nanoalloy as a synergistic catalyst for electrocatalytic reduction of carbon dioxide to methane

Abstract

Developing sustainable energy strategies based on CO₂ reduction is an increasingly important issue given the world’s continued reliance on hydrocarbon fuels and the rise in CO₂ concentrations in the atmosphere. An important option is electrochemical or photoelectrochemical CO₂ reduction to carbon fuels. We describe here an electrodeposition strategy for preparing highly dispersed, ultrafine metal nanoparticle catalysts on an electroactive polymeric film including nanoalloys of Cu and Pd. Compared with nanoCu catalysts, which are state-of-the-art catalysts for CO₂ reduction to hydrocarbons, the bimetallic CuPd nanoalloy catalyst exhibits a greater than twofold enhancement in Faradaic efficiency for CO₂ reduction to methane. The origin of the enhancement is suggested to arise from a synergistic reactivity interplay between Pd–H sites and Cu–CO sites during electrochemical CO₂ reduction. The polymer substrate also appears to provide a basis for the local concentration of CO₂ resulting in the enhancement of catalytic current densities by threefold. In conclusion, the procedure for preparation of the nanoalloy catalyst is straightforward and appears to be generally applicable to the preparation of catalytic electrodes for incorporation into electrolysis devices.

Authors:

Zhang, Sheng ^[1]; Kang, Peng ^[1]; Bakir, Mohammed ^[2]; Lapides, Alexander M. ^[1]; Dares, Christopher J. ^[1]; Meyer, Thomas J. ^[1]

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+ Show Author Affiliations

1. Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, NC 27599,
2. Department of Chemistry, University of the West Indies, Mona, Kingston 7, Jamaica

Publication Date:

Mon Dec 14 00:00:00 EST 2015

Research Org.:

Energy Frontier Research Centers (EFRC) (United States). Center for Solar Fuels (UNC EFRC)

Sponsoring Org.:

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

OSTI Identifier:

1235505

Alternate Identifier(s):

OSTI ID: 1370858

Grant/Contract Number:  

SC0001011

Resource Type:

Published Article

Journal Name:

Proceedings of the National Academy of Sciences of the United States of America

Additional Journal Information:

Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 112 Journal Issue: 52; Journal ID: ISSN 0027-8424

Publisher:

Proceedings of the National Academy of Sciences

Country of Publication:

United States

Language:

English

Subject:

36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; catalysis (homogeneous); catalysis (heterogeneous); solar (photovoltaic); solar (fuels); photosynthesis (natural and artificial); hydrogen and fuel cells; electrodes - solar; charge transport; materials and chemistry by design; synthesis (novel materials); synthesis (self-assembly); solar energy; carbon dioxide reduction; CuPd nanoalloy; electropolymerized film; hydrocarbon