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Double-Exchange-Induced in situ Conductivity in Nickel-Based Oxyhydroxides: An Effective Descriptor for Electrocatalytic Oxygen Evolution

Tian, Bailin and Shin, Hyeyoung and Liu, Shengtang and Fei, Muchun and Mu, Zhangyan and Liu, Cheng and Pan, Yanghang and Sun, Yamei and Goddard, William A., III and Ding, Mengning (2021) Double-Exchange-Induced in situ Conductivity in Nickel-Based Oxyhydroxides: An Effective Descriptor for Electrocatalytic Oxygen Evolution. Angewandte Chemie International Edition, 60 (30). pp. 16448-16456. ISSN 1433-7851. doi:10.1002/anie.202101906. https://resolver.caltech.edu/CaltechAUTHORS:20210517-091659348

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Abstract

Motivated by in silico predictions that Co, Rh, and Ir dopants would lead to low overpotentials to improve OER activity of Ni-based hydroxides, we report here an experimental confirmation on the altered OER activities for a series of metals (Mo, W, Fe, Ru, Co, Rh, Ir) doped into γ-NiOOH. The in situ electrical conductivity for metal doped γ-NiOOH correlates well with the trend in enhanced OER activities. Density functional theory (DFT) calculations were used to rationalize the in situ conductivity of the key intermediate states of metal doped γ-NiOOH during OER. The simultaneous increase of OER activity with intermediate conductivity was later rationalized by their intrinsic connections to the double exchange (DE) interaction between adjacent metal ions with various d orbital occupancies, serving as an indicator for the key metal-oxo radical character, and an effective descriptor for the mechanistic evaluation and theoretical guidance in design and screening of efficient OER catalysts.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1002/anie.202101906DOIArticle
ORCID:
AuthorORCID
Shin, Hyeyoung0000-0001-6694-7895
Goddard, William A., III0000-0003-0097-5716
Additional Information:© 2021 Wiley‐VCH GmbH. Issue Online: 12 July 2021; Version of Record online: 22 June 2021; Accepted manuscript online: 10 May 2021; Manuscript revised: 25 April 2021; Manuscript received: 06 February 2021. B.T. and M.D. acknowledge the support by the Fundamental Research Funds for the Central Universities in China (020514380224), and Natural Science Foundation of Jiangsu Province (BK20180321). H.S. and W.A.G. were supported by the US National Science Foundation (CBET-1805022) and (CBET-2005250). H.S. was also supported by the National Research Foundation of Korea (No.2020R1C1C1008458) and the National Supercomputing Center with supercomputing resources including technical support (KSC-2020-INO-0001). The authors declare no conflict of interest.
Funders:
Funding AgencyGrant Number
Fundamental Research Funds for the Central Universities020514380224
Natural Science Foundation of Jiangsu ProvinceBK20180321
NSFCBET-1805022
NSFCBET-2005250
National Research Foundation of Korea2020R1C1C1008458
National Supercomputing CenterKSC-2020-INO-0001
Subject Keywords:active metal d orbital; double-exchange interaction; in situ intermediates conductivity; Ni-based oxyhydroxides; oxygen evolution reaction
Other Numbering System:
Other Numbering System NameOther Numbering System ID
WAG1429
Issue or Number:30
DOI:10.1002/anie.202101906
Record Number:CaltechAUTHORS:20210517-091659348
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20210517-091659348
Official Citation:Double-Exchange-Induced in situ Conductivity in Nickel-Based Oxyhydroxides: An Effective Descriptor for Electrocatalytic Oxygen Evolution. B. Tian, H. Shin, S. Liu, M. Fei, Z. Mu, C. Liu, Y. Pan, Y. Sun, W. A. Goddard, M. Ding, Angew. Chem. Int. Ed. 2021, 60, 16448; DOI: 10.1002/anie.202101906
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:109143
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:17 May 2021 16:47
Last Modified:12 Jul 2021 22:47

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