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1.
Small ; : e2402862, 2024 Jun 18.
Artigo em Inglês | MEDLINE | ID: mdl-38888118

RESUMO

Lithium-sulfur (Li-S) batteries are expected to be the next-generation energy storage system due to the ultrahigh theoretical energy density and low cost. However, the notorious shuttle effect of higher-order polysulfides and the uncontrollable lithium dendrite growth are the two biggest challenges for commercially viable Li-S batteries. Herein, these two main challenges are solved by in situ polymerization of bi-functional gel polymer electrolyte (GPE). The initiator (SiCl4) not only drives the polymerization of 1,3-dioxolane (DOL) but also induces the construction of a hybrid solid electrolyte interphase (SEI) with inorganic-rich compositions on the Li anode. In addition, diatomaceous earth (DE) is added and anchored in the GPE to obtain PDOL-SiCl4-DE electrolyte through in situ polymerization. Combined with density functional theory (DFT) calculations, the hybrid SEI provides abundant adsorption sites for the deposition of Li+, inhibiting the growth of lithium dendrites. Meanwhile, the shuttle effect is greatly alleviated due to the strong adsorption capacity of DE toward lithium polysulfides. Therefore, the Li/Li symmetric cell and Li-S full cell assembled with PDOL-SiCl4-DE exhibit excellent cycling stability. This study offers a valuable reference for the development of high performance and safe Li-S batteries.

2.
ChemSusChem ; 17(17): e202400159, 2024 Sep 09.
Artigo em Inglês | MEDLINE | ID: mdl-38581393

RESUMO

Uneven lithium (Li) metal deposition typically results in uncontrollable dendrite growth, which renders an unsatisfactory cycling stability and coulombic efficiency (CE) of Li metal batteries (LMBs), preventing their practical application. Herein, a novel carbon cloth with the modification of ZnO nanosheets (ZnO@CC) is fabricated for LMBs. The as-prepared ZnO@CC with a cross-linked network significantly reduces the local current density, and the design of ZnO nanosheets can promote the uniform deposition of Li metal as lithiophilic sites. As a result, the Li metal anodes (LMAs) based on ZnO@CC (ZnO@CC@Li) enables a long cycle life over 640 hours with a low overpotential of 65 mV at a current density of 4 mA cm-2 with a capacity of 1 mAh cm-2 in the symmetric cell. Moreover, when coupling the ZnO@CC@Li with a LiFePO4 cathode, the assembled full cell exhibits excellent long cycle and rate performance, highlighting its promising practical application prospect.

3.
ACS Appl Mater Interfaces ; 15(14): 17986-17993, 2023 Apr 12.
Artigo em Inglês | MEDLINE | ID: mdl-36988389

RESUMO

The Si/C anode is one of the most promising candidate materials for the next-generation lithium-ion batteries (LIBs). Herein, a silicon/carbon nanotubes/carbon (Si/CNTs/C) composite is in situ synthesized by a one-step reaction of magnesium silicide, calcium carbonate, and ferrocene. Transmission electron microscopy reveals that the growth of CNTs is attributed to the catalysis of iron atoms derived from the decomposition of ferrocene. In comparison to a Si/C composite, the cycle stability of the Si/CNTs/C composite can obviously be improved as an anode for LIBs. The enhanced performance is mainly attributed to the following factors: (i) the perfect combination of Si nanoparticles and in situ grown CNTs achieves high mechanical integrity and good electrical contact; (ii) Si nanoparticles are entangled in the CNT cage, effectively reducing the volume expansion upon cycling; and (iii) in situ grown CNTs can improve the conductivity of composites and provide lithium ion transport channels. Moreover, the full cell constructed by a LiFePO4 cathode and Si/CNTs/C anode exhibits excellent cycling stability (137 mAh g-1 after 300 cycles at 0.5 C with a capacity retention rate of 91.2%). This work provides a new way for the synthesis of a Si/C anode for high-performance LIBs.

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