期刊
ADVANCED MATERIALS
卷 32, 期 17, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202000151
关键词
heterostructures; interfacial and electronic properties; lithiation; delithiation pathways; lithium-ion batteries; MXenes
类别
资金
- China Postdoctoral Science Foundation [2016M601431, 2018T110308] Funding Source: Medline
- Heilongjiang Province Postdoctoral Science Foundation [LBH-Z16056, LBH-TZ1707] Funding Source: Medline
- National Natural Science Foundation of China [51604089, 51874110] Funding Source: Medline
- Natural Science Foundation of Heilongjiang Province [JJ20180042] Funding Source: Medline
Structural modulation endows electrochemical hybrids with promising energy storage properties owing to their adjustable interfacial and/or electronic characteristics. For MXene-based materials, however, the facile but effective strategies for tuning their structural properties at nanoscale are still lacking. Herein, 3D crumpled S-functionalized Ti3C2Tx substrate is rationally integrated with Fe3O4/FeS heterostructures via coprecipitation and subsequent partial sulfurization to induce a highly active and stable electrode architecture. The unique heterostructures with tuned electronic properties can induce improved kinetics and structural stability. The surface engineering by S terminations on the MXene further unlocks extra (pseudo)capacitive lithium storage. Serving as anode for lithium storage, the optimized electrode delivers an excellent long-term cycling stability (913.9 mAh g(-1) after 1000 cycles at 1 A g(-1)) and superior rate capability (490.4 mAh g(-1) at 10 A g(-1)). Moreover, the (de)lithiation pathways associated with energy storage mechanisms are further revealed by operando X-ray diffraction, in situ electroanalytical techniques, and first-principles calculations. The hybrid electrode is proved to undergo stepwise phase transformations during discharging but a relatively uniform reconversion during charging, suggesting an asymmetric conversion mechanism. This work provides a novel strategy for designing high-performance hybrids and paves the way for in-depth understanding of complex lithium intercalation and conversion reactions.
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