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Abstract MXenes are promising passive components that enable lithium‐sulfur batteries (LSBs) by effectively trapping lithium polysulfides (LiPSs) and facilitating surface‐mediated redox reactions. Despite numerous studies highlighting the potential of MXenes in LSBs, there are no systematic studies of MXenes’ composition influence on polysulfide adsorption, which is foundational to their applications in LSB. Here, a comprehensive investigation of LiPS adsorption on seven MXenes with varying chemistries (Ti2CTx, Ti3C2Tx, Ti3CNTx, Mo2TiC2Tx, V2CTx, Nb2CTx, and Nb4C3Tx), utilizing optical and analytical spectroscopic methods is performed. This work reports on the influence of polysulfide concentration, interaction time, and MXenes’ chemistry (transition metal layer, carbide and carbonitride inner layer, surface terminations and structure) on the amount of adsorbed LiPSs and the adsorption mechanism. These findings reveal the formation of insoluble thiosulfate and polythionate complex species on the surfaces of all tested MXenes. Furthermore, the selective adsorption of lithium and sulfur, and the extent of conversion of the adsorbed species on MXenes varied based on their chemistry. For instance, Ti2CTxexhibits a strong tendency to adsorb lithium ions, while Mo2TiC2Txis effective in trapping sulfur by forming long‐chain polythionates. The latter demonstrates a significant conversion of intermediate polysulfides into low‐order species. This study offers valuable guidance for the informed selection of MXenes in various functional components benefiting the future development of high‐performance LSBs.more » « less
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Vala_Mizrak, Ali; Ehring, Jonathan_C; Shekhirev, Mikhail; Lord, Robert_W; Aküzüm, Bilen; Singh, Pushpendra; Gogotsi, Yury; Kumbur, E_Caglan (, Batteries & Supercaps)Abstract In this work, Ti3C2TxMXene was investigated as a nanofluidic anolyte additive in vanadium redox flow batteries to improve the sluggish kinetics of V2+/V3+redox reaction. Numerous electrochemical tests under flow and static conditions were performed to demonstrate the effectiveness of MXenes for VRFB applications. Pressure drop tests and morphology analysis were also conducted to better understand the hydraulic effects of MXene addition into the anolyte. The nanofluidic anolytes with the concentration of 0.10 and 0.15 wt% showed the best electrochemical performance, although the former induced less aggravated hydraulic effects within a reasonable pressure drop range. At a current density of 200 mA cm−2, the nanofluidic analyte containing 0.10 wt% MXene was able to utilize 67 % of the theoretical capacity. Contrarily, with the pristine anolyte, only 10 % of the theoretical capacity could be utilized due to excessive losses. Moreover, the energy efficiency up to 74 % is observed for the nanofluidic electrolyte, which is an increase of 25 % compared to the pristine anolyte. Primarily, the enhanced battery performance was attributed to the improved electrocatalytic activity towards the anodic V2+/V3+redox reaction. Furthermore, a dynamic, web‐like, flowing electrode network is shown to increase the mass transport capacity of porous carbon felt electrodes by creating additional, abundant, and electrochemically active surfaces within the pores.more » « less
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