Boosting Energy Efficiency and Stability of Li-CO2 Batteries via Synergy between Ru Atom Clusters and Single-Atom Ru-N4 sites in the Electrocatalyst Cathode
© 2022 Wiley-VCH GmbH.
Veröffentlicht in: | Advanced materials (Deerfield Beach, Fla.). - 1998. - 34(2022), 17 vom: 27. Apr., Seite e2200559 |
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1. Verfasser: | |
Weitere Verfasser: | , , , , , , , , |
Format: | Online-Aufsatz |
Sprache: | English |
Veröffentlicht: |
2022
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Zugriff auf das übergeordnete Werk: | Advanced materials (Deerfield Beach, Fla.) |
Schlagworte: | Journal Article Li-CO2 batteries atomic cluster catalysts carbon quantum dots electronic synergy single-atom catalysts |
Zusammenfassung: | © 2022 Wiley-VCH GmbH. The Li-CO2 battery is a novel strategy for CO2 capture and energy-storage applications. However, the sluggish CO2 reduction and evolution reactions cause large overpotential and poor cycling performance. Herein, a new catalyst containing well-defined ruthenium (Ru) atomic clusters (RuAC ) and single-atom Ru-N4 (RuSA ) composite sites on carbon nanobox substrate (RuAC+SA NCB) (NCB = nitrogen-doped carbon nanobox) is fabricated by utilizing the different complexation effects between the Ru cation and the amine group (NH2 ) on carbon quantum dots or nitrogen moieties on NCB. Systematic experimental and theoretical investigations demonstrate the vital role of electronic synergy between RuAC and Ru-N4 in improving the electrocatalytic activity toward the CO2 evolution reaction (CO2 ER) and CO2 reduction reaction (CO2 RR). The electronic properties of the Ru-N4 sites are essentially modulated by the adjacent RuAC species, which optimizes the interactions with key reaction intermediates thereby reducing the energy barriers in the rate-determining steps of the CO2 RR and CO2 ER. Remarkably, the RuAC+SA @NCB-based cell displays unprecedented overpotentials as low as 1.65 and 1.86 V at ultrahigh rates of 1 and 2 A g-1 , and twofold cycling lifespan than the baselines. The findings provide a novel strategy to construct catalysts with composite active sites comprising multiple atom assemblies for high-performance metal-CO2 batteries |
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Beschreibung: | Date Revised 27.04.2022 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
ISSN: | 1521-4095 |
DOI: | 10.1002/adma.202200559 |