Oxygen evolution reaction over catalytic single-site Co in a well-defined brookite TiO2 nanorod surface

Chang Liu; Jin Qian; Yifan Ye; Hua Zhou; Cheng Jun Sun; Colton Sheehan; Zhiyong Zhang; Gang Wan; Yi Sheng Liu; Jinghua Guo; Shuang Li; Hyeyoung Shin; Sooyeon Hwang; T. Brent Gunnoe; William A. Goddard; Sen Zhang

doi:10.1038/s41929-020-00550-5

Oxygen evolution reaction over catalytic single-site Co in a well-defined brookite TiO₂ nanorod surface

Chang Liu
, Jin Qian
, Yifan Ye
, Hua Zhou
, Cheng Jun Sun
, Colton Sheehan
, Zhiyong Zhang
, Gang Wan
, Yi Sheng Liu
, Jinghua Guo
, Shuang Li
, Hyeyoung Shin
, Sooyeon Hwang
, T. Brent Gunnoe
, William A. Goddard
, Sen Zhang

Surface Chemistry & Catalysis Group

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

262 Scopus citations

Abstract

Efficient electrocatalysts for the oxygen evolution reaction (OER) are paramount to the development of electrochemical devices for clean energy and fuel conversion. However, the structural complexity of heterogeneous electrocatalysts makes it a great challenge to elucidate the surface catalytic sites and OER mechanisms. Here, we report that catalytic single-site Co in a well-defined brookite TiO₂ nanorod (210) surface (Co-TiO₂) presents turnover frequencies that are among the highest for Co-based heterogeneous catalysts reported to date, reaching 6.6 ± 1.2 and 181.4 ± 28 s⁻¹ at 300 and 400 mV overpotentials, respectively. Based on grand canonical quantum mechanics calculations and the single-site Co atomic structure validated by in situ and ex situ spectroscopic probes, we have established a full description of the catalytic reaction kinetics for Co-TiO₂ as a function of applied potential, revealing an adsorbate evolution mechanism for the OER. The computationally predicted Tafel slope and turnover frequencies exhibit exceedingly good agreement with experiment. [Figure not available: see fulltext.]

Original language	English
Pages (from-to)	36-45
Number of pages	10
Journal	Nature Catalysis
Volume	4
Issue number	1
DOIs	https://doi.org/10.1038/s41929-020-00550-5
State	Published - Jan 2021

Funding

This work was supported by the US National Science Foundation (CBET-1805022, CBET-2004808 and CBET-2005250). This research used the resources of the Advanced Photon Source, an Office of Science User Facility operated for the US Department of Energy (DOE) Office of Science by the Argonne National Laboratory, and was supported by the US DOE under contract no. DE-AC02-06CH11357 and the Canadian Light Source and its funding partners. This research used the resources of the Center for Functional Nanomaterials, which is a US DOE Office of Science Facility, at Brookhaven National Laboratory under contract no. DE-SC0012704. This research used the resources of the Advanced Light Source, a US DOE Office of Science User Facility, under contract no. DE-AC02-05CH11231.

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title = "Oxygen evolution reaction over catalytic single-site Co in a well-defined brookite TiO2 nanorod surface",

abstract = "Efficient electrocatalysts for the oxygen evolution reaction (OER) are paramount to the development of electrochemical devices for clean energy and fuel conversion. However, the structural complexity of heterogeneous electrocatalysts makes it a great challenge to elucidate the surface catalytic sites and OER mechanisms. Here, we report that catalytic single-site Co in a well-defined brookite TiO2 nanorod (210) surface (Co-TiO2) presents turnover frequencies that are among the highest for Co-based heterogeneous catalysts reported to date, reaching 6.6 ± 1.2 and 181.4 ± 28 s−1 at 300 and 400 mV overpotentials, respectively. Based on grand canonical quantum mechanics calculations and the single-site Co atomic structure validated by in situ and ex situ spectroscopic probes, we have established a full description of the catalytic reaction kinetics for Co-TiO2 as a function of applied potential, revealing an adsorbate evolution mechanism for the OER. The computationally predicted Tafel slope and turnover frequencies exhibit exceedingly good agreement with experiment. [Figure not available: see fulltext.]",

author = "Chang Liu and Jin Qian and Yifan Ye and Hua Zhou and Sun, \{Cheng Jun\} and Colton Sheehan and Zhiyong Zhang and Gang Wan and Liu, \{Yi Sheng\} and Jinghua Guo and Shuang Li and Hyeyoung Shin and Sooyeon Hwang and Gunnoe, \{T. Brent\} and Goddard, \{William A.\} and Sen Zhang",

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doi = "10.1038/s41929-020-00550-5",

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T1 - Oxygen evolution reaction over catalytic single-site Co in a well-defined brookite TiO2 nanorod surface

AU - Liu, Chang

AU - Qian, Jin

AU - Ye, Yifan

AU - Zhou, Hua

AU - Sun, Cheng Jun

AU - Sheehan, Colton

AU - Zhang, Zhiyong

AU - Wan, Gang

AU - Liu, Yi Sheng

AU - Guo, Jinghua

AU - Li, Shuang

AU - Shin, Hyeyoung

AU - Hwang, Sooyeon

AU - Gunnoe, T. Brent

AU - Goddard, William A.

AU - Zhang, Sen

PY - 2021/1

Y1 - 2021/1

N2 - Efficient electrocatalysts for the oxygen evolution reaction (OER) are paramount to the development of electrochemical devices for clean energy and fuel conversion. However, the structural complexity of heterogeneous electrocatalysts makes it a great challenge to elucidate the surface catalytic sites and OER mechanisms. Here, we report that catalytic single-site Co in a well-defined brookite TiO2 nanorod (210) surface (Co-TiO2) presents turnover frequencies that are among the highest for Co-based heterogeneous catalysts reported to date, reaching 6.6 ± 1.2 and 181.4 ± 28 s−1 at 300 and 400 mV overpotentials, respectively. Based on grand canonical quantum mechanics calculations and the single-site Co atomic structure validated by in situ and ex situ spectroscopic probes, we have established a full description of the catalytic reaction kinetics for Co-TiO2 as a function of applied potential, revealing an adsorbate evolution mechanism for the OER. The computationally predicted Tafel slope and turnover frequencies exhibit exceedingly good agreement with experiment. [Figure not available: see fulltext.]

AB - Efficient electrocatalysts for the oxygen evolution reaction (OER) are paramount to the development of electrochemical devices for clean energy and fuel conversion. However, the structural complexity of heterogeneous electrocatalysts makes it a great challenge to elucidate the surface catalytic sites and OER mechanisms. Here, we report that catalytic single-site Co in a well-defined brookite TiO2 nanorod (210) surface (Co-TiO2) presents turnover frequencies that are among the highest for Co-based heterogeneous catalysts reported to date, reaching 6.6 ± 1.2 and 181.4 ± 28 s−1 at 300 and 400 mV overpotentials, respectively. Based on grand canonical quantum mechanics calculations and the single-site Co atomic structure validated by in situ and ex situ spectroscopic probes, we have established a full description of the catalytic reaction kinetics for Co-TiO2 as a function of applied potential, revealing an adsorbate evolution mechanism for the OER. The computationally predicted Tafel slope and turnover frequencies exhibit exceedingly good agreement with experiment. [Figure not available: see fulltext.]

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Oxygen evolution reaction over catalytic single-site Co in a well-defined brookite TiO₂ nanorod surface

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