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The Predominance of Hydrogen Evolution on Transition Metal Sulfides and Phosphides under CO_2 Reduction Conditions: An Experimental and Theoretical Study

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. (2018) The Predominance of Hydrogen Evolution on Transition Metal Sulfides and Phosphides under CO_2 Reduction Conditions: An Experimental and Theoretical Study. ACS Energy Letters, 3 (6). pp. 1450-1457. ISSN 2380-8195. https://resolver.caltech.edu/CaltechAUTHORS:20180601-080239556

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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 CO_2 reduction (CO_2R) on transition metal phosphide and transition metal sulfide catalysts. Although multifunctional active sites in these materials could potentially improve their CO_2R activity relative to pure transition metal electrocatalysts, under aqueous testing conditions, these materials showed a high selectivity for the HER relative to CO_2R. Computational results supported these findings, indicating that a limitation of the metal phosphide catalysts is that the HER is favored thermodynamically over CO_2R. On Ni-MoS_2, a limitation is the kinetic barrier for the proton–electron transfer to *CO. These theoretical and experimental results demonstrate that selective CO_2R requires electrocatalysts that possess both favorable thermodynamic pathways and surmountable kinetic barriers.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1021/acsenergylett.8b00237DOIArticle
https://pubs.acs.org/doi/suppl/10.1021/acsenergylett.8b00237PublisherSupporting Information
ORCID:
AuthorORCID
Torelli, Daniel A.0000-0002-6222-817X
Xiao, Jianping0000-0003-1779-6140
Kibsgaard, Jakob0000-0002-9219-816X
Lewis, Nathan S.0000-0001-5245-0538
Chan, Karen0000-0002-6897-1108
Hahn, Christopher0000-0002-2772-6341
Jaramillo, Thomas F.0000-0001-9900-0622
Alternate Title:The Predominance of Hydrogen Evolution on Transition Metal Sulfides and Phosphides under CO2 Reduction Conditions: An Experimental and Theoretical Study
Additional Information:© 2018 American Chemical Society. Received: February 9, 2018; Accepted: April 20, 2018; Publication Date (Web): May 31, 2018. This material is based, in part, on work performed by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the U.S. Department of Energy, under Award No. DE-SC0004993. This research used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy (under Contract No. DE-AC02-05CH11231). Part of this work was performed at the Stanford Nano Shared Facilities (SNSF) and the Stanford Nanofabrication Facility (SNF), supported by the National Science Foundation under Award ECCS-1542152. We also acknowledge assistance from the Stanford NMR Facility. M.F. and D.A.T. acknowledge a graduate fellowship through the National Science Foundation. S.A.F. acknowledges the Resnick Sustainability Institute at Caltech for a postdoctoral fellowship. The authors also thank J. Chance Crompton for assistance in synthesizing the nanoparticle electrocatalysts. The authors declare no competing financial interest.
Group:JCAP, Resnick Sustainability Institute
Funders:
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0004993
Department of Energy (DOE)DE-AC02-05CH11231
NSFECCS-1542152
NSF Graduate Research FellowshipUNSPECIFIED
Resnick Sustainability InstituteUNSPECIFIED
Issue or Number:6
Record Number:CaltechAUTHORS:20180601-080239556
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20180601-080239556
Official Citation: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, and Thomas F. Jaramillo. ACS Energy Letters 2018 3 (6), 1450-1457. DOI: 10.1021/acsenergylett.8b00237
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:86732
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:01 Jun 2018 16:15
Last Modified:03 Oct 2019 19:47

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