Nitrogen-Doped Ti$_3$C$_2$T$_x$ Coated with a Molecularly Imprinted Polymer as Efficient Cathode Material for Lithium-Sulfur Batteries

Feng Yan; Liqiang Lu; Chongan Ye; Qi Chen; Sumit Kumar; Wenjian Li; Hamoon Hemmatpour; Konstantinos Spyrou; Sytze de Graaf; Marc C. A. Stuart; Bart J. Kooi; Dimitrios P. Gournis; Katja Loos; Yutao Pei; Petra Rudolf

arXiv · 2308.10139

Nitrogen-Doped Ti$_3$C$_2$T$_x$ Coated with a Molecularly Imprinted Polymer as Efficient Cathode Material for Lithium-Sulfur Batteries

Feng Yan·Liqiang Lu·Chongan Ye·Qi Chen·Sumit Kumar·Wenjian Li·Hamoon Hemmatpour·Konstantinos Spyrou·Sytze de Graaf·Marc C. A. Stuart·Bart J. Kooi·Dimitrios P. Gournis·Katja Loos·Yutao Pei·Petra Rudolf

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Abstract

Due to their high energy density (2600 Wh/kg), low cost, and low environmental impact, lithium-sulfur batteries are considered a promising alternative to lithium-ion batteries. However, their commercial viability remains a formidable scientific challenge mainly because of the sluggish reaction kinetics at the cathode and the so-called "shuttling effect" of soluble polysulfides, which results in capacity decay and a shortened lifespan. Herein, molecular imprinting with Li$_2$S$_8$ as a target molecule in combination with a two-dimensional material, MXene, is proposed to overcome these issues. Molecularly imprinted polymer-coated nitrogen-doped Ti-based MXene was successfully synthesized and demonstrated to exhibit an appealing electrochemical performance, namely a high specific capacity of 1095 mAh/g at 0.1 C and an extended cycling stability (300 mAh/g at 1.0 C after 300 cycles). X-ray photoelectron spectroscopy was applied to elucidate the underlying mechanisms and proved that Li$_2$S$_8$-imprinted polymer polyacrylamide serves as a polysulfide trap through strong chemical affinity towards the long-chain lithium polysulfides, while N-doped Ti-based MXene promotes the redox kinetics by accelerating the conversion of lithium polysulfides. This distinct interfacial strategy is expected to result in more effective and stable Li-S batteries.

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Feng Yan, Liqiang Lu, Chongan Ye, Qi Chen, Sumit Kumar, Wenjian Li, Hamoon Hemmatpour, Konstantinos Spyrou, Sytze de Graaf, Marc C. A. Stuart, Bart J. Kooi, Dimitrios P. Gournis, Katja Loos, Yutao Pei, Petra Rudolf. 2023-08-20. Nitrogen-Doped Ti$_3$C$_2$T$_x$ Coated with a Molecularly Imprinted Polymer as Efficient Cathode Material for Lithium-Sulfur Batteries. https://arxiv.org/abs/2308.10139

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