Designing tailored multifunctional catalysts that enhance lean-electrolyte sulfur redox kinetics is crucial for achieving high-energy-density lithium-sulfur batteries;however,it still remains challenge.Motivated by th...Designing tailored multifunctional catalysts that enhance lean-electrolyte sulfur redox kinetics is crucial for achieving high-energy-density lithium-sulfur batteries;however,it still remains challenge.Motivated by the structural protection of active sites in natural enzymes,we implant natural glutathione(GSH)within the metal-organic framework MIL-47(V)cavity for GSH@MIL-47(V)biomimetic catalysts,thereby stabilizing and activating its thiol functionality.Quantification using 5,5’-dithiobis(2-nitrobenzoic acid)(DTNB)as a probe confirmed successful GSH incorporation,revealing that GSH@MIL-47(V)enables a continuous and stable catalytic reaction cycle.Moreover,in-situ and ex-situ spectroscopies indicate thiol-driven S-S bond breakage that lowers the reaction energy barrier and concurrently promotes lithium bis(trifluoromethanesulfonyl)imide(LiTFSI)decomposition.As a result,GSH@MIL-47(V)cells,at 6 C rate,deliver a discharge capacity of 733.1 mAh·g^(−1) and maintain 573.0 mAh·g^(−1) after 750 cycles.Even under an electrolyte-to-sulfur ratio of 5.5μL·mg^(−1) ,it maintains 867.2 mAh·g^(−1) at a highrate of 0.5 C.This strategy highlights the potential of enzyme-inspired catalysts for enhancing lithium-sulfur batteries.展开更多
基金supported by the National Natural Science Foundation of China(Nos.22309136 and 22309135)the Natural Science Foundation of Zhejiang Province(No.LQ22B030003)+2 种基金Wenzhou Major Science and Technology Project(No.ZG2023055)the Doctoral Innovation Foundation of Wenzhou University(No.3162023001002)Zhejiang Xinmiao Talents Program(No.2024R429B042).
文摘Designing tailored multifunctional catalysts that enhance lean-electrolyte sulfur redox kinetics is crucial for achieving high-energy-density lithium-sulfur batteries;however,it still remains challenge.Motivated by the structural protection of active sites in natural enzymes,we implant natural glutathione(GSH)within the metal-organic framework MIL-47(V)cavity for GSH@MIL-47(V)biomimetic catalysts,thereby stabilizing and activating its thiol functionality.Quantification using 5,5’-dithiobis(2-nitrobenzoic acid)(DTNB)as a probe confirmed successful GSH incorporation,revealing that GSH@MIL-47(V)enables a continuous and stable catalytic reaction cycle.Moreover,in-situ and ex-situ spectroscopies indicate thiol-driven S-S bond breakage that lowers the reaction energy barrier and concurrently promotes lithium bis(trifluoromethanesulfonyl)imide(LiTFSI)decomposition.As a result,GSH@MIL-47(V)cells,at 6 C rate,deliver a discharge capacity of 733.1 mAh·g^(−1) and maintain 573.0 mAh·g^(−1) after 750 cycles.Even under an electrolyte-to-sulfur ratio of 5.5μL·mg^(−1) ,it maintains 867.2 mAh·g^(−1) at a highrate of 0.5 C.This strategy highlights the potential of enzyme-inspired catalysts for enhancing lithium-sulfur batteries.
