Lattice Matched Carbide–Phosphide Composites with Superior Electrocatalytic Activity and Stability

Regmi, Yagya N.; Roy, Asa; King, Laurie A.; Cullen, David A.; Meyer, Harry M.; Goenaga, Gabriel A.; Zawodzinski, Thomas A.; Labbé, Nicole; Chmely, Stephen C.

doi:10.1021/acs.chemmater.7b03377

Title: Lattice Matched Carbide–Phosphide Composites with Superior Electrocatalytic Activity and Stability

Journal Article · 19 October 2017 · Chemistry of Materials

DOI: https://doi.org/10.1021/acs.chemmater.7b03377 · OSTI ID:1410911

^[1]; Roy, Asa ^[2];

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^[4]; Goenaga, Gabriel A. ^[5]; Zawodzinski, Thomas A. ^[6];

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Univ. of Tennessee, Knoxville, TN (United States). Center for Renewable Carbon
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States). Bredesen Center for Interdisciplinary Research and Education
Stanford Univ., CA (United States). Dept. of Chemical Engineering
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemical and Biomolecular Engineering
Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemical and Biomolecular Engineering; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States). Bredesen Center for Interdisciplinary Research and Education

Composites of electrocatalytically active transition-metal compounds present an intriguing opportunity toward enhanced activity and stability. Here, to identify potentially scalable pairs of a catalytically active family of compounds, we demonstrate that phosphides of iron, nickel, and cobalt can be deposited on molybdenum carbide to generate nanocrystalline heterostructures. Composites synthesized via solvothermal decomposition of metal acetylacetonate salts in the presence of highly dispersed carbide nanoparticles show hydrogen evolution activities comparable to those of state-of-the-art non-noble metal catalysts. Investigation of the spent catalyst using high resolution microscopy and elemental analysis reveals that formation of carbide–phosphide composite prevents catalyst dissolution in acid electrolyte. Lattice mismatch between the two constituent electrocatalysts can be used to rationally improve electrochemical stability. Among the composites of iron, nickel, and cobalt phosphide, iron phosphide displays the lowest degree of lattice mismatch with molybdenum carbide and shows optimal electrochemical stability. Turnover rates of the composites are higher than that of the carbide substrate and compare favorably to other electrocatalysts based on earth-abundant elements. Lastly, our findings will inspire further investigation into composite nanocrystalline electrocatalysts that use molybdenum carbide as a stable catalyst support.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Nuclear Energy (NE)

Grant/Contract Number:: AC05-00OR22725; NE0000693

OSTI ID:: 1410911

Journal Information:: Chemistry of Materials, Vol. 29, Issue 21; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 19 works

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36 MATERIALS SCIENCE
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Carbide
phosphide
electrocatalysis
hydrogen evolution reaction
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Title: Lattice Matched Carbide–Phosphide Composites with Superior Electrocatalytic Activity and Stability

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