The photo‐assisted strategy is regarded as a crucial approach to enhance the conversion kinetics of polysulfides in lithium–sulfur (Li–S) batteries. However, the development of photo‐assisted Li–S batteries still faces important challenges, such as the rapid recombination of photogenerated electron−holes on cathode and more severe shuttle effect. Herein, a breakthrough in overcoming the challenges has been made by constructing a promising photo‐assisted Li−S battery based on semiconducted metal−organic frameworks. During the discharging progress, the photoexcited electrons generated by H2BPDC ligand based on ligand‐to‐metal charge transfer (LMCT) effect, are injected into the Ti‐oxo clusters in Ti‐MOF, thereby facilitating the sulfur reduction to Li2S. And photoexcited holes are capable of promoting the decomposition kinetics of Li2S during charging. More importantly, the stronger chemical interaction between Ti‐BPDC‐d and polysulfides under light inhibits the polysulfides dissolution and shuttling, which fundamentally addresses the issue of light‐accelerated shuttling. As a result, the photo‐assisted Li–S batteries deliver a reversible capability of 1090.21 mAh g−1 at 0.2 C with a capacity retention of 82.91% over 150 cycles, and a superior rate capability of 673.58 mAh g−1 at 5 C. The findings are promising in advancing the design principles for photo‐rechargeable Li−S batteries.

中文翻译：

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金属有机框架中配位缺陷诱导的路易斯对增强了双功能光辅助锂硫电池的硫动力学

光辅助策略被认为是增强锂硫（Li-S）电池中多硫化物转化动力学的关键方法。然而，光辅助锂硫电池的发展仍然面临着重要的挑战，例如光生电子空穴在阴极上的快速复合和更严重的穿梭效应。在此，通过构建一种基于半导体金属有机框架的有前景的光辅助锂硫电池，在克服这些挑战方面取得了突破。在放电过程中，H产生的光生电子2基于配体到金属电荷转移（LMCT）效应的BPDC配体被注入Ti-MOF中的Ti-oxo簇中，从而促进硫还原为Li2S.并且光生空穴能够促进Li的分解动力学2充电期间。更重要的是，Ti-BPDC-d与多硫化物在光作用下更强的化学相互作用抑制了多硫化物的溶解和穿梭，从根本上解决了光加速穿梭的问题。因此，光辅助Li-S电池的可逆容量为1090.21 mAh g−10.2 C 下 150 次循环容量保持率为 82.91%，倍率性能高达 673.58 mAh g−15 C。这些发现对于推进光充电锂硫电池的设计原理很有希望。