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      d-Orbital steered active sites through ligand editing on heterometal imidazole frameworks for rechargeable zinc-air battery

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          Abstract

          The implementation of pristine metal-organic frameworks as air electrode may spark fresh vitality to rechargeable zinc-air batteries, but successful employment is rare due to the challenges in regulating their electronic states and structural porosity. Here we conquer these issues by incorporating ligand vacancies and hierarchical pores into cobalt-zinc heterometal imidazole frameworks. Systematic characterization and theoretical modeling disclose that the ligand editing eases surmountable energy barrier for *OH deprotonation by its efficacy to steer metal d-orbital electron occupancy. As a stride forward, the selected cobalt-zinc heterometallic alliance lifts the energy level of unsaturated d-orbitals and optimizes their adsorption/desorption process with oxygenated intermediates. With these merits, cobalt-zinc heterometal imidazole frameworks, as a conceptually unique electrode, empowers zinc-air battery with a discharge-charge voltage gap of 0.8 V and a cyclability of 1250 h at 15 mA cm –2, outperforming the noble-metal benchmarks.

          Abstract

          Low intrinsic activity and accessibility of active sites limit the application of metal-organic framework as catalyst for Zn-air battery. Here, authors present a cation substitution strategy to regulate the electronic state of metal sites and modify its porosity, which enables battery operation.

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          Most cited references56

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          Metal-Air Batteries with High Energy Density: Li-Air versus Zn-Air

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            Batteries and fuel cells for emerging electric vehicle markets

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              Electrically Rechargeable Zinc-Air Batteries: Progress, Challenges, and Perspectives

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                Author and article information

                Contributors
                zhwchen@uwaterloo.ca
                Journal
                Nat Commun
                Nat Commun
                Nature Communications
                Nature Publishing Group UK (London )
                2041-1723
                17 November 2020
                17 November 2020
                2020
                : 11
                : 5858
                Affiliations
                [1 ]GRID grid.46078.3d, ISNI 0000 0000 8644 1405, Department of Chemical Engineering, Waterloo Institute for Nanotechnology, , University of Waterloo, ; Waterloo, ON N2L 3G1 Canada
                [2 ]GRID grid.24516.34, ISNI 0000000123704535, School of Materials Science and Engineering, , Tongji University Shanghai, ; 201804 Shanghai, China
                [3 ]GRID grid.462338.8, ISNI 0000 0004 0605 6769, School of Chemistry and Chemical Engineering, , Henan Normal University, ; 453007 Xinxiang, China
                [4 ]GRID grid.25152.31, ISNI 0000 0001 2154 235X, Canadian Light Source, , University of Saskatchewan, ; Saskatoon, SK S7N 0X4 Canada
                Author information
                http://orcid.org/0000-0001-9289-888X
                http://orcid.org/0000-0003-3463-5509
                Article
                19709
                10.1038/s41467-020-19709-6
                7673988
                33203863
                793b98c7-7085-4daf-be61-342a223436f6
                © The Author(s) 2020

                Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.

                History
                : 8 June 2020
                : 9 October 2020
                Funding
                Funded by: FundRef https://doi.org/10.13039/501100000038, Gouvernement du Canada | Natural Sciences and Engineering Research Council of Canada (Conseil de Recherches en Sciences Naturelles et en Génie du Canada);
                Categories
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                © The Author(s) 2020

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                batteries
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                batteries

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