School of Chemical Engineering & Advanced Materials, The University of Adelaide, Adelaide, SA 5005, Australia.
School of Chemical Engineering and Technology, Tianjin University, Tianjin, 300350, China.
Angew Chem Int Ed Engl. 2022 Dec 19;61(51):e202213863. doi: 10.1002/anie.202213863. Epub 2022 Nov 22.
Efficient catalyst design is important for lean-electrolyte sulfur reduction in Li-S batteries. However, most of the reported catalysts were focused on catalyst-polysulfide interactions, and generally exhibit high activity only with a large excess of electrolyte. Herein, we proposed a general rule to boost lean-electrolyte sulfur reduction by controlling the catalyst-solvent interactions. As evidenced by synchrotron-based analysis, in situ spectroscopy and theoretical computations, strong catalyst-solvent interaction greatly enhances the lean-electrolyte catalytic activity and battery stability. Benefitting from the strong interaction between solvent and cobalt catalyst, the Li-S battery achieves stable cycling with only 0.22 % capacity decay per cycle with a low electrolyte/sulfur mass ratio of 4.2. The lean-electrolyte battery delivers 79 % capacity retention compared with the battery with flooded electrolyte, which is the highest among the reported lean-electrolyte Li-S batteries.
高效的催化剂设计对于锂硫电池中贫电解质条件下的硫还原反应非常重要。然而，大多数已报道的催化剂都集中在催化剂-多硫化物相互作用上，并且通常只有在大量电解质过剩的情况下才表现出高活性。在此，我们提出了一种通过控制催化剂-溶剂相互作用来提高贫电解质条件下硫还原反应的一般规律。基于同步辐射的分析、原位光谱和理论计算表明，强催化剂-溶剂相互作用极大地提高了贫电解质的催化活性和电池稳定性。得益于溶剂与钴催化剂之间的强相互作用，锂硫电池在低电解质/硫质量比为 4.2 时仅以 0.22%/每循环的容量衰减实现了稳定循环。与充满电解质的电池相比，贫电解质电池的容量保持率达到 79%，这在已报道的贫电解质锂硫电池中是最高的。
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