Stability and Activity of Cobalt Antimonate for Oxygen Reduction in Strong Acid

Lan Zhou; Hao Li; Yungchieh Lai; Matthias Richter; Kevin Kan; Joel A. Haber; Sara Kelly; Zhenbin Wang; Yubing Lu; R. Soyoung Kim; Xiang Li; Junko Yano; Jens K. Nørskov; John M. Gregoire

doi:10.1021/acsenergylett.1c02673

Stability and Activity of Cobalt Antimonate for Oxygen Reduction in Strong Acid

Lan Zhou, Hao Li, Yungchieh Lai, Matthias Richter, Kevin Kan, Joel A. Haber, Sara Kelly, Zhenbin Wang, Yubing Lu, R. Soyoung Kim, Xiang Li, Junko Yano, Jens K. Nørskov, John M. Gregoire

Research output: Contribution to journal › Article › peer-review

12 Citations (Scopus)

Abstract

Guided by computational Pourbaix screening and high-throughput experiments aimed at the development of precious-metal-free fuel cells, we investigate rutile CoSb₂O₆ as an electrocatalyst for oxygen reduction in 1 M sulfuric acid. Following 4 h of catalyst conditioning at 0.7 V vs RHE, operation at this potential for 20 h yielded an average current density of −0.17 mA cm^-2 with corrosion at a rate of 0.04 nm hour^-1 that is stoichiometric with catalyst composition. Surface Pourbaix analysis of the (111) surface identified partial H coverage under operating conditions. The Sb active site has an HO* binding free energy of 0.49 eV, which is near the peak of the kinetic 4e^- ORR volcano for transition-metal oxides in acidic conditions. The experimental demonstration of operational stability and computational identification of a reaction pathway with favorable energetics place rutile CoSb₂O₆ among the most promising precious-metal-free electrocatalysts for oxygen reduction in acidic media.

Original language	English
Pages (from-to)	993-1000
Number of pages	8
Journal	ACS Energy Letters
Volume	7
Issue number	3
DOIs	https://doi.org/10.1021/acsenergylett.1c02673
Publication status	Published - 2022 Mar 11
Externally published	Yes

ASJC Scopus subject areas

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

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10.1021/acsenergylett.1c02673

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title = "Stability and Activity of Cobalt Antimonate for Oxygen Reduction in Strong Acid",

abstract = "Guided by computational Pourbaix screening and high-throughput experiments aimed at the development of precious-metal-free fuel cells, we investigate rutile CoSb2O6 as an electrocatalyst for oxygen reduction in 1 M sulfuric acid. Following 4 h of catalyst conditioning at 0.7 V vs RHE, operation at this potential for 20 h yielded an average current density of −0.17 mA cm-2 with corrosion at a rate of 0.04 nm hour-1 that is stoichiometric with catalyst composition. Surface Pourbaix analysis of the (111) surface identified partial H coverage under operating conditions. The Sb active site has an HO* binding free energy of 0.49 eV, which is near the peak of the kinetic 4e- ORR volcano for transition-metal oxides in acidic conditions. The experimental demonstration of operational stability and computational identification of a reaction pathway with favorable energetics place rutile CoSb2O6 among the most promising precious-metal-free electrocatalysts for oxygen reduction in acidic media.",

author = "Lan Zhou and Hao Li and Yungchieh Lai and Matthias Richter and Kevin Kan and Haber, {Joel A.} and Sara Kelly and Zhenbin Wang and Yubing Lu and Kim, {R. Soyoung} and Xiang Li and Junko Yano and N{\o}rskov, {Jens K.} and Gregoire, {John M.}",

note = "Funding Information: This work was supported by Toyota Research Institute. Use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515. Publisher Copyright: {\textcopyright} 2022 American Chemical Society",

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day = "11",

doi = "10.1021/acsenergylett.1c02673",

language = "English",

volume = "7",

pages = "993--1000",

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T1 - Stability and Activity of Cobalt Antimonate for Oxygen Reduction in Strong Acid

AU - Zhou, Lan

AU - Li, Hao

AU - Lai, Yungchieh

AU - Richter, Matthias

AU - Kan, Kevin

AU - Haber, Joel A.

AU - Kelly, Sara

AU - Wang, Zhenbin

AU - Lu, Yubing

AU - Kim, R. Soyoung

AU - Li, Xiang

AU - Yano, Junko

AU - Nørskov, Jens K.

AU - Gregoire, John M.

N1 - Funding Information: This work was supported by Toyota Research Institute. Use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515. Publisher Copyright: © 2022 American Chemical Society

PY - 2022/3/11

Y1 - 2022/3/11

N2 - Guided by computational Pourbaix screening and high-throughput experiments aimed at the development of precious-metal-free fuel cells, we investigate rutile CoSb2O6 as an electrocatalyst for oxygen reduction in 1 M sulfuric acid. Following 4 h of catalyst conditioning at 0.7 V vs RHE, operation at this potential for 20 h yielded an average current density of −0.17 mA cm-2 with corrosion at a rate of 0.04 nm hour-1 that is stoichiometric with catalyst composition. Surface Pourbaix analysis of the (111) surface identified partial H coverage under operating conditions. The Sb active site has an HO* binding free energy of 0.49 eV, which is near the peak of the kinetic 4e- ORR volcano for transition-metal oxides in acidic conditions. The experimental demonstration of operational stability and computational identification of a reaction pathway with favorable energetics place rutile CoSb2O6 among the most promising precious-metal-free electrocatalysts for oxygen reduction in acidic media.

AB - Guided by computational Pourbaix screening and high-throughput experiments aimed at the development of precious-metal-free fuel cells, we investigate rutile CoSb2O6 as an electrocatalyst for oxygen reduction in 1 M sulfuric acid. Following 4 h of catalyst conditioning at 0.7 V vs RHE, operation at this potential for 20 h yielded an average current density of −0.17 mA cm-2 with corrosion at a rate of 0.04 nm hour-1 that is stoichiometric with catalyst composition. Surface Pourbaix analysis of the (111) surface identified partial H coverage under operating conditions. The Sb active site has an HO* binding free energy of 0.49 eV, which is near the peak of the kinetic 4e- ORR volcano for transition-metal oxides in acidic conditions. The experimental demonstration of operational stability and computational identification of a reaction pathway with favorable energetics place rutile CoSb2O6 among the most promising precious-metal-free electrocatalysts for oxygen reduction in acidic media.

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Stability and Activity of Cobalt Antimonate for Oxygen Reduction in Strong Acid

Abstract

ASJC Scopus subject areas

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