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
![]() |
PDF
- Accepted Version
See Usage Policy. 2MB |
![]() |
PDF
- Supplemental Material
See Usage Policy. 6MB |
Use this Persistent URL to link to this item: https://resolver.caltech.edu/CaltechAUTHORS:20210517-091659348
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: |
| ||||||||||||||
ORCID: |
| ||||||||||||||
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: |
| ||||||||||||||
Subject Keywords: | active metal d orbital; double-exchange interaction; in situ intermediates conductivity; Ni-based oxyhydroxides; oxygen evolution reaction | ||||||||||||||
Other Numbering System: |
| ||||||||||||||
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 |
Repository Staff Only: item control page