期刊
ADVANCED FUNCTIONAL MATERIALS
卷 32, 期 7, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.202103959
关键词
anion-derived passivation layers; concentrated hybrid aqueous electrolytes; dual-ion batteries; in operando techniques; transmission X-ray microscopy; Zn dendrites; Zn metal anodes
类别
资金
- Ministry of Science and Technology of Taiwan [MOST 110-2639-E-011-001-ASP, 110-3116-F-011-003, 110-3116-F-011-004, 109-2923-E-011-008, 109-2124-M-002-008, 109-2923-E-011-009]
- Ministry of Education of Taiwan [MOE 1080059]
- Academia Sinica [AS-KPQ-106- DDPP]
- National Taiwan University of Science and Technology (NTUST)
- National Center for High-performance Computing (NCHC)
- National Synchrotron Radiation Research Centre (NSRRC)
- NTUST-Kyutech Joint Research Program [NTUST-Kyutech-110-03]
The study introduces a concentrated hybrid aqueous electrolyte as an effective solution to dendrite growth and low coulombic efficiency in zinc anodes. This electrolyte enables dendrite-free zinc plating/stripping with an excellent coulombic efficiency of approximately 100%, surpassing previous values.
Zinc metal is considered a promising anode material for aqueous zinc ion batteries. However, it suffers from dendrite growth, corrosion, and low coulombic efficiency (CE) during plating/stripping. Herein, a concentrated hybrid (4 m Zn(CF3SO3)(2) + 2 m LiClO4) aqueous electrolyte (CHAE) to overcome the challenges facing the Zn anode is reported. The developed electrolyte achieves dendrite-free Zn plating/stripping and obtains an excellent CE of approximate to 100%, surpassing the previously reported values. The combination of synchrotron-based in operando transmission X-ray microscopy, X-ray diffraction, and ex situ X-ray photoelectron spectroscopy analyses indicate that the denser, anion-derived passivation layer formed using the CHAE facilitates homogeneous current distribution and better prevents freshly deposited Zn from directly contacting the electrolyte than the looser, solvent-derived layers formed from a dilute hybrid aqueous electrolyte (DHAE). The beneficial effects of the CHAE on the compact, dense, and stable salt-anion-derived passivation layer can be attributed to its unique solvation structure, which suppresses the water-related side reactions and widens the electrochemical potential window. In the hybrid Zn||LiFePO4 configuration, the CHAE-based cell delivered a stable performance of CE >99% and capacity retention >90% after 285 cycles. In contrast, the DHAE-based cell exhibits capacity retention of <65% after 170 cycles.
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