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Revealing the Synergy of Cation and Anion Vacancies on Improving Overall Water Splitting Kinetics

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Title
Revealing the Synergy of Cation and Anion Vacancies on Improving Overall Water Splitting Kinetics
Author(s)
Yang Liu; Huong T. D. Bui; Amol R. Jadhav; Taehun Yang; Shahid Saqlain; Yongguang Luo; Jianmin Yu; Ashwani Kumar; Hongdan Wang; Lingling Wang; Viet Q. Bui; Min Gyu Kim; Young Dok Kim; Hyoyoung Lee
Publication Date
2021-05
Journal
ADVANCED FUNCTIONAL MATERIALS, v.31, no.21
Publisher
WILEY-V C H VERLAG GMBH
Abstract
The exact understanding for each promotional role of cation and anion vacancies in bifunctional water splitting activity will assist in the development of an efficient activation strategy of inert catalysts. Herein, systematic first-principles computations demonstrate that the synergy of anion-oxygen and cation-manganese vacancies (V-O and V-Mn) in manganese dioxide (MnO2) nanosheets results in abnormal local lattice distortion and electronic modulation. Such alterations enrich the accessible active centers, increase conductivity, enhance the water dissociation step, and favor intermediate adsorption-desorption, consequently promoting HER and OER kinetics. As proof of concept, robust electrocatalysts, MnO2 ultrathin nanosheets doped with dual vacancies (DV-MnO2) are obtained via a maturely chemical strategy. Detailed characterizations confirm the cation vacancies-V-Mn contribute to enhanced conductivity and anion vacancies-V-O enrich the active centers with optimized local electronic configurations, consistent with the simulative predictions. As expected, DV-MnO2 exhibits exceptional bifunctionality with the strong assistance of synergetic dual vacancies which act as abundant "hot spots" for active multiple intermediates. Leading to a lower cell voltage (1.55 V) in alkali electrolyte is required to reach 10 mA cm(-2) for the overall water splitting system. These atomic-level insights on synergetic DV can favor the development of activating strategy from inert electrocatalysts.
URI
https://pr.ibs.re.kr/handle/8788114/9678
DOI
10.1002/adfm.202010718
ISSN
1616-301X
Appears in Collections:
Center for Integrated Nanostructure Physics(나노구조물리 연구단) > 1. Journal Papers (저널논문)
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