The Predominance of Hydrogen Evolution on Transition Metal Sulfides and Phosphides under CO2 Reduction Conditions: An Experimental and Theoretical Study

Alan T. Landers, Meredith Fields, Daniel A. Torelli, Jianping Xiao, Thomas R. Hellstern, Sonja A. Francis, Charlie Tsai, Jakob Kibsgaard, Nathan S. Lewis, Karen Chan, Christopher Hahn, Thomas F. Jaramillo

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Abstract

A combination of experiment and theory has been used to understand the relationship between the hydrogen evolution reaction (HER) and CO2 reduction (CO2R) on transition metal phosphide and transition metal sulfide catalysts. Although multifunctional active sites in these materials could potentially improve their CO2R activity relative to pure transition metal electrocatalysts, under aqueous testing conditions, these materials showed a high selectivity for the HER relative to CO2R. Computational results supported these findings, indicating that a limitation of the metal phosphide catalysts is that the HER is favored thermodynamically over CO2R. On Ni-MoS2, a limitation is the kinetic barrier for the proton-electron transfer to CO. These theoretical and experimental results demonstrate that selective CO2R requires electrocatalysts that possess both favorable thermodynamic pathways and surmountable kinetic barriers.

Original languageEnglish
Pages (from-to)1450-1457
Number of pages8
JournalACS Energy Letters
Volume3
Issue number6
DOIs
Publication statusPublished - Jun 8 2018

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ASJC Scopus subject areas

  • Chemistry (miscellaneous)
  • Renewable Energy, Sustainability and the Environment
  • Fuel Technology
  • Energy Engineering and Power Technology
  • Materials Chemistry

Cite this

Landers, A. T., Fields, M., Torelli, D. A., Xiao, J., Hellstern, T. R., Francis, S. A., Tsai, C., Kibsgaard, J., Lewis, N. S., Chan, K., Hahn, C., & Jaramillo, T. F. (2018). The Predominance of Hydrogen Evolution on Transition Metal Sulfides and Phosphides under CO2 Reduction Conditions: An Experimental and Theoretical Study. ACS Energy Letters, 3(6), 1450-1457. https://doi.org/10.1021/acsenergylett.8b00237