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Deciphering the dynamic solid-liquid interphase for energetic high-mass-loading energy storage
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DOI：10.1039/d4ee03303e.png)
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摘要
En 中文
Aqueous pseudocapacitive storage has shown promise for future energy applications, but it suffers from a single reaction pathway and mechanism that restrain performance breakthroughs, especially under commercial high-mass-loading conditions. Herein, using MnO2 as a pseudocapacitive storage material, we tailored a reversible pseudocapacitive-type electrode/electrolyte interphase (PEI) by refining the cationic environment, which broke the limitation of MnO2 to unlock an energetic dual-ion storage mechanism. Theoretical calculations demonstrated that the engineered dynamic PEI elevated the removal energy of active Mn species to stabilize dual-cation storage and, more importantly, provided highly available MnO2/PEI heterointerface spaces to accommodate more charges. We unveiled that the exceptional heterointerface region with considerable charge redistribution enabled a significantly reduced ion-migration energy barrier compared with that of the pure MnO2 interlayer, contributing to fast multi-processing storage of dual carriers. As a proof-of-concept, the tailored mechanism enabled robust stability with 92% capacitance retention after 25 000 cycles. Besides, an appealing areal capacitance of 11.1 F cm-2 was demonstrated under a high mass loading of 27.4 mg cm-2. Our findings signify a paradigm shift in aqueous pseudocapacitive chemistry and offer insights into dynamic microenvironment regulation for building advanced energy storage devices.
Keyword:
CHARGE STORAGE
INTERCALATION
BIRNESSITE
STABILITY
CHEMISTRY
期刊
IF:
30.8
论文数:
6.9K
被引数:
12.4W
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