Solvated metal complexes for balancing stability and activity of sulfur free radicals

IF 42.9 Q1 ELECTROCHEMISTRY
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Abstract

Free radicals can improve the reaction rate, but most of them are unstable due to unpaired electrons. Simultaneously maintaining their stability and activity is challenging. Herein, taking sulfur (S) radicals as an example, we propose a strategy in which solvated metal complexes constructed by Al(acetylacetonate)3 and different solvents can stabilize high concentrations of S radicals with good activity through ion–dipole interactions. Based on this strategy, it is first demonstrated that S4· is selectively stabilized by controlling the configurations of the solvated complexes. As a result, the reaction rate of S↔Li2S is increased by 8 times, and the energy efficiency and rate capability of the Li–S batteries are significantly improved, especially the 5-fold increase in cell capacities at a low electrolyte/sulfur ratio. This work provides an important strategy in which solvated metal complexes balance the activity and stability of free radicals to accelerate reactions and their application in various fields.

Abstract Image

Abstract Image

用于平衡硫自由基稳定性和活性的溶解金属复合物
自由基可以提高反应速度,但由于其电子不配对,大多数自由基都不稳定。同时保持自由基的稳定性和活性具有挑战性。在此,我们以硫(S)自由基为例,提出了一种策略,即由乙酰丙酮铝(Al(acetylacetonate)3)和不同溶剂构建的溶解金属配合物可以通过离子-偶极子相互作用稳定高浓度的 S 自由基,并使其具有良好的活性。基于这种策略,研究人员首次证明,通过控制溶解络合物的构型,可以选择性地稳定 S4--。因此,S↔Li2S 的反应速率提高了 8 倍,锂-S 电池的能量效率和速率能力得到显著提高,尤其是在低电解质/硫比条件下,电池容量提高了 5 倍。这项工作提供了一种重要的策略,即溶解金属复合物可以平衡自由基的活性和稳定性,从而加速反应并将其应用于各个领域。
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来源期刊
CiteScore
33.70
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