A Dynamically Stabilized Single‐Nickel Electrocatalyst for Selective Reduction of Oxygen to Hydrogen Peroxide
Abstract
Abstract On‐location electrochemical generation of H 2 O 2 is of great current interest. Herein, selective two‐electron reduction of O 2 to H 2 O 2 by a single [Ni II (H 2 O) 6 ] 2+ cation that is dynamically associated with a negatively charged metal–organic layer (MOL) by hydrogen bonding and coulombic interactions is reported. In contrast, Ni II centers covalently immobilized on the MOL reduce O 2 to H 2 O in a four‐ electron process. Oxygen adsorption by [Ni II (H 2 O) 6 ] 2+ followed by two‐electron reduction generates neutral [Ni II (H 2 O) 4 (OH)(OOH)] 0 , which momentarily disconnects from the negatively charged MOL to avoid the injection of additional electrons. Release of H 2 O 2 from [Ni II (H 2 O) 4 (OH)(OOH)] 0 regenerates [Ni II (H 2 O) 6 ] 2+ , which regains affinity to the MOL. Such dynamically associated Ni II single‐metal electrocatalysts ensure high selectivity and represent a new strategy for generating selective catalysts for electrochemical production of important chemicals.
- Authors:
-
[1];
- Collaborative Innovation Center of Chemistry for Energy Materials State Key Laboratory of Physical Chemistry of Solid Surfaces Department of Chemistry College of Chemistry and Chemical Engineering Xiamen University Xiamen 361005 P. R. China
- Collaborative Innovation Center of Chemistry for Energy Materials State Key Laboratory of Physical Chemistry of Solid Surfaces Department of Chemistry College of Chemistry and Chemical Engineering Xiamen University Xiamen 361005 P. R. China, Department of Chemistry University of Chicago Chicago Illinois 60637 USA
- Department of Chemistry University of Chicago Chicago Illinois 60637 USA
- Publication Date:
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1481440
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Publisher's Accepted Manuscript
- Journal Name:
- Chemistry - A European Journal
- Additional Journal Information:
- Journal Name: Chemistry - A European Journal Journal Volume: 24 Journal Issue: 64; Journal ID: ISSN 0947-6539
- Publisher:
- Wiley Blackwell (John Wiley & Sons)
- Country of Publication:
- Germany
- Language:
- English
Citation Formats
Wang, Tingting, Zeng, Zhongming, Cao, Lingyun, Li, Zhe, Hu, Xuefu, An, Bing, Wang, Cheng, and Lin, Wenbin. A Dynamically Stabilized Single‐Nickel Electrocatalyst for Selective Reduction of Oxygen to Hydrogen Peroxide. Germany: N. p., 2018.
Web. doi:10.1002/chem.201804312.
Wang, Tingting, Zeng, Zhongming, Cao, Lingyun, Li, Zhe, Hu, Xuefu, An, Bing, Wang, Cheng, & Lin, Wenbin. A Dynamically Stabilized Single‐Nickel Electrocatalyst for Selective Reduction of Oxygen to Hydrogen Peroxide. Germany. https://doi.org/10.1002/chem.201804312
Wang, Tingting, Zeng, Zhongming, Cao, Lingyun, Li, Zhe, Hu, Xuefu, An, Bing, Wang, Cheng, and Lin, Wenbin. Fri .
"A Dynamically Stabilized Single‐Nickel Electrocatalyst for Selective Reduction of Oxygen to Hydrogen Peroxide". Germany. https://doi.org/10.1002/chem.201804312.
@article{osti_1481440,
title = {A Dynamically Stabilized Single‐Nickel Electrocatalyst for Selective Reduction of Oxygen to Hydrogen Peroxide},
author = {Wang, Tingting and Zeng, Zhongming and Cao, Lingyun and Li, Zhe and Hu, Xuefu and An, Bing and Wang, Cheng and Lin, Wenbin},
abstractNote = {Abstract On‐location electrochemical generation of H 2 O 2 is of great current interest. Herein, selective two‐electron reduction of O 2 to H 2 O 2 by a single [Ni II (H 2 O) 6 ] 2+ cation that is dynamically associated with a negatively charged metal–organic layer (MOL) by hydrogen bonding and coulombic interactions is reported. In contrast, Ni II centers covalently immobilized on the MOL reduce O 2 to H 2 O in a four‐ electron process. Oxygen adsorption by [Ni II (H 2 O) 6 ] 2+ followed by two‐electron reduction generates neutral [Ni II (H 2 O) 4 (OH)(OOH)] 0 , which momentarily disconnects from the negatively charged MOL to avoid the injection of additional electrons. Release of H 2 O 2 from [Ni II (H 2 O) 4 (OH)(OOH)] 0 regenerates [Ni II (H 2 O) 6 ] 2+ , which regains affinity to the MOL. Such dynamically associated Ni II single‐metal electrocatalysts ensure high selectivity and represent a new strategy for generating selective catalysts for electrochemical production of important chemicals.},
doi = {10.1002/chem.201804312},
journal = {Chemistry - A European Journal},
number = 64,
volume = 24,
place = {Germany},
year = {Fri Nov 09 00:00:00 EST 2018},
month = {Fri Nov 09 00:00:00 EST 2018}
}
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