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Abstract
Transition metal oxide electrocatalysts (TMOEs) are poised to revive grid-scale all-vanadium redox flow batteries (VRFBs) due to their low-cost and unique electronic properties, while often inescapably harboring surface vacancies. The role of local vacancy-induced physicochemical properties on vanadium-redox electrochemistry (VRE), encompassing kinetics, and stability, remains profoundly unveiled. Herein, for the first time, it is revealed that vacancies induce atomic-scale polarization in TMOEs and elucidate its mechanism in VRE. Attributable to local polarization, particularly by cation vacancy, the activated nearest-coordinated Mn sites prominently augment the adsorption competence of the V2+/V3+ couple and expedite its round-tripping by forming an intermediate *Mn–O–V bridge. It is also affirmed that the anion vacancies are vulnerable to microstructure reconfiguration by feeble hydroxyl adsorption and thus performance degradation over long-term cycling, in contrast to cation vacancies. Accordingly, the VRFB employing cation-vacancy-functionalized electrode delivers an energy efficiency of 80.8% and a reliable 1000-cycle lifespan with a negligible decay of 0.57% per cycle at 300 mA cm−2, outclassing others. The findings shed light on the fundamental rules governing the utility and evolution of vacancies in TMOEs, thereby moving a step closer toward their deployment in a wide range of sustainable energy storage schemes.
© 2025 Wiley-VCH GmbH
© 2025 Wiley-VCH GmbH
Original language | English |
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Article number | 2420510 |
Journal | Advanced Materials |
Volume | 37 |
Issue number | 13 |
Online published | 29 Jan 2025 |
DOIs | |
Publication status | Published - 2 Apr 2025 |
Funding
X.Z., K.A., J.S., and X.Y. These authors contributed equally. The study wassupported by the Research Grants Council of Hong Kong, General Re-search Fund (Grant no. 11306021).
Research Keywords
- atomic-scale polarization
- nearest-coordinated Mn
- transition metaloxide-based electrocatalysts
- vanadium-redox electrochemistry
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GRF: Understanding Ion Transport in Hydrogel Electrolyte and Charge Transfer on Electrode-Hydrogel Interfaces for Wearable Zinc-Ion Battery
DAOUD, W. (Principal Investigator / Project Coordinator)
1/01/22 → …
Project: Research