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

Abstract

Here, 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.

Authors:
 [1];  [2]; ORCiD logo [3]; ORCiD logo [2];  [2];  [3];  [2]; ORCiD logo [4]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2]
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  1. Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., Stanford, CA (United States)
  3. California Inst. of Technology (CalTech), Pasadena, CA (United States)
  4. SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., Stanford, CA (United States); Technical Univ. of Denmark, Lyngby (Denmark)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1469213
Grant/Contract Number:  
AC02-76SF00515; SC0004993
Resource Type:
Accepted Manuscript
Journal Name:
ACS Energy Letters
Additional Journal Information:
Journal Volume: 3; Journal Issue: 6; Journal ID: ISSN 2380-8195
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Landers, Alan T., Fields, Meredith, Torelli, Daniel A., Xiao, Jianping, Hellstern, Thomas R., Francis, Sonja A., Tsai, Charlie, Kibsgaard, Jakob, Lewis, Nathan S., Chan, Karen, Hahn, Christopher, and Jaramillo, Thomas F. The Predominance of Hydrogen Evolution on Transition Metal Sulfides and Phosphides under CO2 Reduction Conditions: An Experimental and Theoretical Study. United States: N. p., 2018. Web. doi:10.1021/acsenergylett.8b00237.
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Landers, Alan T., Fields, Meredith, Torelli, Daniel A., Xiao, Jianping, Hellstern, Thomas R., Francis, Sonja A., Tsai, Charlie, Kibsgaard, Jakob, Lewis, Nathan S., Chan, Karen, Hahn, Christopher, & Jaramillo, Thomas F. The Predominance of Hydrogen Evolution on Transition Metal Sulfides and Phosphides under CO2 Reduction Conditions: An Experimental and Theoretical Study. United States. doi:10.1021/acsenergylett.8b00237.
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Landers, Alan T., Fields, Meredith, Torelli, Daniel A., Xiao, Jianping, Hellstern, Thomas R., Francis, Sonja A., Tsai, Charlie, Kibsgaard, Jakob, Lewis, Nathan S., Chan, Karen, Hahn, Christopher, and Jaramillo, Thomas F. Thu . "The Predominance of Hydrogen Evolution on Transition Metal Sulfides and Phosphides under CO2 Reduction Conditions: An Experimental and Theoretical Study". United States. doi:10.1021/acsenergylett.8b00237. https://www.osti.gov/servlets/purl/1469213.
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@article{osti_1469213,
title = {The Predominance of Hydrogen Evolution on Transition Metal Sulfides and Phosphides under CO2 Reduction Conditions: An Experimental and Theoretical Study},
author = {Landers, Alan T. and Fields, Meredith and Torelli, Daniel A. and Xiao, Jianping and Hellstern, Thomas R. and Francis, Sonja A. and Tsai, Charlie and Kibsgaard, Jakob and Lewis, Nathan S. and Chan, Karen and Hahn, Christopher and Jaramillo, Thomas F.},
abstractNote = {Here, 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.},
doi = {10.1021/acsenergylett.8b00237},
journal = {ACS Energy Letters},
number = 6,
volume = 3,
place = {United States},
year = {2018},
month = {5}
}
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Journal Article:
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DOI:  10.1021/acsenergylett.8b00237
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Figures / Tables:

Figure 1 Figure 1: Faradaic efficiency for H2 production under CO2R conditions for representative transition metal phosphide and sulfide materials. Less than 3.5 percent of the current density went towards CO2 reduction products on these materials. Square symbols denote thin film catalysts while asterisk symbols denote nanoparticle catalysts. The color of themore » symbol corresponds to the material composition.« less
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  • Liu, Jingwei; Yu, Guangtao; Zhang, Ran
  • Physical Chemistry Chemical Physics, Vol. 21, Issue 10
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