Atomic ruthenium-riveted metal-organic framework with tunable d-band modulates oxygen redox for lithium-oxygen batteries
Non-aqueous Li-O2 batteries have aroused considerable attention because of their ultrahigh theoretical energy density, but they are severely hindered by slow cathode reaction kinetics and large overvoltages, which are closely associated with the discharge product of Li2O2. Herein, hexagonal conducti...
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sg-ntu-dr.10356-1644842023-01-30T01:55:04Z Atomic ruthenium-riveted metal-organic framework with tunable d-band modulates oxygen redox for lithium-oxygen batteries Lv, Qingliang Zhu, Zhuo Ni, Youxuan Wen, Bo Jiang, Zhuoliang Fang, Hengyi Li, Fujun School of Chemical and Biomedical Engineering Science::Chemistry Catalyst Li-O₂ Non-aqueous Li-O2 batteries have aroused considerable attention because of their ultrahigh theoretical energy density, but they are severely hindered by slow cathode reaction kinetics and large overvoltages, which are closely associated with the discharge product of Li2O2. Herein, hexagonal conductive metal-organic framework nanowire arrays of nickel-hexaiminotriphenylene (Ni-HTP) with quadrilateral Ni-N4 units are synthesized to incorporate Ru atoms into its skeleton for NiRu-HTP. The atomically dispersed Ru-N4 sites manifest strong adsorption for the LiO2 intermediate owing to its tunable d-band center, leading to its high local concentration around NiRu-HTP. This favors the formation of film-like Li2O2 on NiRu-HTP with promoted electron transfer and ion diffusion across the cathode-electrolyte interface, facilitating its reversible decomposition during charge. These allow the Li-O2 battery with NiRu-HTP to deliver a remarkably reduced charge/discharge polarization of 0.76 V and excellent cyclability. This work will enrich the design philosophy of electrocatalysts for regulation of kinetic behaviors of oxygen redox. This work was supported by National Natural Science Foundation of China (52171215), the Tianjin Natural Science Foundation (19JCJQJC62400), and Haihe Laboratory of Sustainable Chemical Transformations. 2023-01-30T01:55:04Z 2023-01-30T01:55:04Z 2022 Journal Article Lv, Q., Zhu, Z., Ni, Y., Wen, B., Jiang, Z., Fang, H. & Li, F. (2022). Atomic ruthenium-riveted metal-organic framework with tunable d-band modulates oxygen redox for lithium-oxygen batteries. Journal of the American Chemical Society, 144(50), 23239-23246. https://dx.doi.org/10.1021/jacs.2c11676 0002-7863 https://hdl.handle.net/10356/164484 10.1021/jacs.2c11676 36474358 2-s2.0-85143867321 50 144 23239 23246 en Journal of the American Chemical Society © 2022 American Chemical Society. All rights reserved. |
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Science::Chemistry Catalyst Li-O₂ Lv, Qingliang Zhu, Zhuo Ni, Youxuan Wen, Bo Jiang, Zhuoliang Fang, Hengyi Li, Fujun Atomic ruthenium-riveted metal-organic framework with tunable d-band modulates oxygen redox for lithium-oxygen batteries |
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Non-aqueous Li-O2 batteries have aroused considerable attention because of their ultrahigh theoretical energy density, but they are severely hindered by slow cathode reaction kinetics and large overvoltages, which are closely associated with the discharge product of Li2O2. Herein, hexagonal conductive metal-organic framework nanowire arrays of nickel-hexaiminotriphenylene (Ni-HTP) with quadrilateral Ni-N4 units are synthesized to incorporate Ru atoms into its skeleton for NiRu-HTP. The atomically dispersed Ru-N4 sites manifest strong adsorption for the LiO2 intermediate owing to its tunable d-band center, leading to its high local concentration around NiRu-HTP. This favors the formation of film-like Li2O2 on NiRu-HTP with promoted electron transfer and ion diffusion across the cathode-electrolyte interface, facilitating its reversible decomposition during charge. These allow the Li-O2 battery with NiRu-HTP to deliver a remarkably reduced charge/discharge polarization of 0.76 V and excellent cyclability. This work will enrich the design philosophy of electrocatalysts for regulation of kinetic behaviors of oxygen redox. |
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School of Chemical and Biomedical Engineering |
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School of Chemical and Biomedical Engineering Lv, Qingliang Zhu, Zhuo Ni, Youxuan Wen, Bo Jiang, Zhuoliang Fang, Hengyi Li, Fujun |
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Article |
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Lv, Qingliang Zhu, Zhuo Ni, Youxuan Wen, Bo Jiang, Zhuoliang Fang, Hengyi Li, Fujun |
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Lv, Qingliang |
title |
Atomic ruthenium-riveted metal-organic framework with tunable d-band modulates oxygen redox for lithium-oxygen batteries |
title_short |
Atomic ruthenium-riveted metal-organic framework with tunable d-band modulates oxygen redox for lithium-oxygen batteries |
title_full |
Atomic ruthenium-riveted metal-organic framework with tunable d-band modulates oxygen redox for lithium-oxygen batteries |
title_fullStr |
Atomic ruthenium-riveted metal-organic framework with tunable d-band modulates oxygen redox for lithium-oxygen batteries |
title_full_unstemmed |
Atomic ruthenium-riveted metal-organic framework with tunable d-band modulates oxygen redox for lithium-oxygen batteries |
title_sort |
atomic ruthenium-riveted metal-organic framework with tunable d-band modulates oxygen redox for lithium-oxygen batteries |
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2023 |
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https://hdl.handle.net/10356/164484 |
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1757048194141782016 |