Structure Sensitivity of Formic Acid Electrooxidation on Transition Metal Surfaces: A First-Principles Study

Elnabawy, Ahmed O.; Herron, Jeffrey A.; Scaranto, Jessica; Mavrikakis, Manos

doi:10.1149/2.0161815jes

Structure Sensitivity of Formic Acid Electrooxidation on Transition Metal Surfaces: A First-Principles Study

Journal Article · Sat Sep 22 00:00:00 EDT 2018 · Journal of the Electrochemical Society

DOI:https://doi.org/10.1149/2.0161815jes· OSTI ID:1494744

^[1]; Herron, Jeffrey A. ^[2]; Scaranto, Jessica ^[2]; ^[2]

Univ. of Wisconsin, Madison, WI (United States). Dept. of Chemical and Biological Engineering; University of Wisconsin-Madison Department of Chemical and Biological Engineering
Univ. of Wisconsin, Madison, WI (United States). Dept. of Chemical and Biological Engineering

Formic acid presents several advantages for use as a fuel in fuel cells. We present a first-principles based analysis of electrooxidation trends for formic acid on the close-packed facets of eight fcc metals: Au, Ag, Cu, Pt, Pd, Ni, Ir, and Rh, and four hcp metals: Co, Os, Ru, and Re. To explore the structure sensitivity of this reaction on the fcc metals, we also studied the open (100) facet of these eight metals. We find that the open facets of Au, Ag, Cu, Pt, and Pd are more energy-efficient (i.e. require less overpotential) for formic acid electrooxidation when compared to their close-packed facets. The opposite is true for the stronger-binding metals: Ni, Ir, and Rh. Using the free energy of adsorbed CO* and OH* as reactivity descriptors, we cast the thermochemistry of the reaction network into phase diagrams showing regions of rate-determining steps, together with their calculated free energies. This allows the identification of bimetallic alloys, potentially possessing improved electrocatalysis for formic acid electrooxidation, compared to Pt or Pd. We discuss the need for anode catalysts for direct formic acid fuel cells (DFAFCs) to diminish CO* poisoning, by promoting the formation of formate instead of carboxyl intermediate.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Wisconsin, Madison, WI (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)

Grant/Contract Number:: FG02-05ER15731; AC02-06CH11357; AC02-05CH11231

OSTI ID:: 1494744

Journal Information:: Journal of the Electrochemical Society, Journal Name: Journal of the Electrochemical Society Journal Issue: 15 Vol. 165; ISSN 0013-4651

Publisher:: The Electrochemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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