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

Research output: Contribution to journalArticle

11 Citations (Scopus)

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

Fingerprint

Sulfides
Transition metals
Hydrogen
Electrocatalysts
Catalysts
Kinetics
Carbon Monoxide
Protons
Metals
Thermodynamics
Electrons
Testing
Experiments

ASJC Scopus subject areas

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

Cite this

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

In: ACS Energy Letters, Vol. 3, No. 6, 08.06.2018, p. 1450-1457.

Research output: Contribution to journalArticle

Landers, AT, Fields, M, Torelli, DA, Xiao, J, Hellstern, TR, Francis, SA, Tsai, C, Kibsgaard, J, Lewis, NS, Chan, K, Hahn, C & Jaramillo, TF 2018, 'The Predominance of Hydrogen Evolution on Transition Metal Sulfides and Phosphides under CO2 Reduction Conditions: An Experimental and Theoretical Study', ACS Energy Letters, vol. 3, no. 6, pp. 1450-1457. https://doi.org/10.1021/acsenergylett.8b00237
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. In: ACS Energy Letters. 2018 ; Vol. 3, No. 6. pp. 1450-1457.
@article{214c17908633480298bbf598592ffd95,
title = "The Predominance of Hydrogen Evolution on Transition Metal Sulfides and Phosphides under CO2 Reduction Conditions: An Experimental and Theoretical Study",
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.",
author = "Landers, {Alan T.} and Meredith Fields and Torelli, {Daniel A.} and Jianping Xiao and Hellstern, {Thomas R.} and Francis, {Sonja A.} and Charlie Tsai and Jakob Kibsgaard and Lewis, {Nathan S} and Karen Chan and Christopher Hahn and Jaramillo, {Thomas F.}",
year = "2018",
month = "6",
day = "8",
doi = "10.1021/acsenergylett.8b00237",
language = "English",
volume = "3",
pages = "1450--1457",
journal = "ACS Energy Letters",
issn = "2380-8195",
publisher = "American Chemical Society",
number = "6",

}

TY - JOUR

T1 - The Predominance of Hydrogen Evolution on Transition Metal Sulfides and Phosphides under CO2 Reduction Conditions

T2 - An Experimental and Theoretical Study

AU - Landers, Alan T.

AU - Fields, Meredith

AU - Torelli, Daniel A.

AU - Xiao, Jianping

AU - Hellstern, Thomas R.

AU - Francis, Sonja A.

AU - Tsai, Charlie

AU - Kibsgaard, Jakob

AU - Lewis, Nathan S

AU - Chan, Karen

AU - Hahn, Christopher

AU - Jaramillo, Thomas F.

PY - 2018/6/8

Y1 - 2018/6/8

N2 - 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.

AB - 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.

UR - http://www.scopus.com/inward/record.url?scp=85048508876&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85048508876&partnerID=8YFLogxK

U2 - 10.1021/acsenergylett.8b00237

DO - 10.1021/acsenergylett.8b00237

M3 - Article

VL - 3

SP - 1450

EP - 1457

JO - ACS Energy Letters

JF - ACS Energy Letters

SN - 2380-8195

IS - 6

ER -