%0 Journal Article %A Lujie Jia %A Jian Wang %A Shuaiyang Ren %A Guoxi Ren %A Xiang Jin %A Licheng Kao %A Xuefei Feng %A Feipeng Yang %A Qi Wang %A Ludi Pan %A Qingtian Li %A Yi‐sheng Liu %A Yang Wu %A Gao Liu %A Jun Feng %A Shoushan Fan %A Yifan Ye %A Jinghua Guo %A Yuegang Zhang %B ENERGY & ENVIRONMENTAL MATERIALS %D 2021 %G eng %N 2 %P 222 - 228 %R 10.1002/eem2.v4.210.1002/eem2.12152 %T Unraveling Shuttle Effect and Suppression Strategy in Lithium/Sulfur Cells by In Situ/Operando X‐ray Absorption Spectroscopic Characterization %V 4 %8 01/2021 %! Energy Environ. Mater. %X

The polysulfides shuttle effect represents a great challenge in achieving high capacity and long lifespan of lithium/sulfur (Li/S) cells. A comprehensive understanding of the shuttle-related sulfur speciation and diffusion process is vital for addressing this issue. Herein, we employed in situ/operando X-ray absorption spectroscopy (XAS) to trace the migration of polysulfides across the Li/S cells by precisely monitoring the sulfur chemical speciation at the cathodic electrolyte-separator and electrolyte-anode interfaces, respectively, in a real-time condition. After we adopted a shuttle-suppressing strategy by introducing an electrocatalytic layer of twinborn bismuth sulfide/bismuth oxide nanoclusters in a carbon matrix (BSOC), we found the Li/S cell showed greatly improved sulfur utilization and longer life span. The operando S K-edge XAS results revealed that the BSOC modification was bi-functional: trapping polysulfides and catalyzing conversion of sulfur species simultaneously. We elucidated that the polysulfide trapping-and-catalyzing effect of the BSOC electrocatalytic layer resulted in an effective lithium anode protection. Our results could offer potential stratagem for designing more advanced Li/S cells.