Abstract
Constructing SiOx-based composite materials with fast reaction kinetics and high stability is crucial but challenging for high-performance lithium-ion batteries. Herein, we developed the N-doped Ti3C2Tx MXene ultrathin sheet (NTS)-coupled SiOx nanoparticles using a melamine-assisted ball milling and annealing procedure. The principle of melamine in exfoliating MXene was demonstrated by contrast experiments and theoretical calculations. The strong interfacial interactions between SiOx and the NTS (Si−O−Ti bond) can effectively enhance the electron transfer and ensure electrode stability. Moreover, the NTS with rich surface groups endowed the composite with a pseudocapacitive behavior, beneficial for fast lithium storage. As a result, the composite delivered a long lifespan (∼700 mA h g−1 over 800 cycles at 1.0 A g−1) and a superior rate performance (596.4 mA h g−1 at 5 A g−1). More importantly, the composite in half and full cells exhibited high areal capacity and good cycling stability at high mass loadings, revealing a promising application prospect.
摘要
构建具有快速反应动力学和优异循环稳定性的SiOx基负极材料是获取高性能锂离子电池的关键和挑战. 本文中, 我们利用三聚氰胺辅助的球磨和退火方法, 合成了氮掺杂的Ti3C2Tx MXene超薄片层(NTS)包覆的SiOx复合材料. 通过对比实验和理论计算, 我们论证了三聚氰胺剥离MXene的作用机理. SiOx与NTS之间强烈的界面相互作用(Si−O−Ti键)可以有效地增强电子转移, 确保电极的稳定性. 此外, 具有丰富表面基团的NTS使复合材料具有赝电容性能, 有利于快速储锂. 因此, 该复合材料展现出了长循环寿命(在1.0 A g−1的电流密度下, 循环800次后比容量保持为∼700 mA h g−1)和优越的倍率性能(在5 A g−1的电流密度下, 比容量为596.4 mA h g−1). 更重要的是, 在高负载量下, 该复合材料在半电池和全电池中均表现出较高的面积比容量和良好的循环稳定性, 展现出了良好的应用潜力.
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Acknowledgements
This work was supported by the National Natural Science Foundation of China (21971146 and 52171182), Taishan Scholarship in Shandong Province (ts201511004), the Key Research and Development Program of Shandong Province (2021ZLGX01), and the HPC Cloud Platform of Shandong University. The authors thank the equipment support from Shandong University Structural Constituent and Physical Property Research Facilities for the high-energy ball-milling machine (Fritsch Pulverisette 7, Germany) and AFM (Bruker Bioscope Resolve, Germany).
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Zhang K conceived the idea, performed the experiments and data analysis, and wrote the original draft. Zhao D performed the calculation. Qian Z guided the calculation process. Gu X, Yang J, and Qian Y guided the idea and finalized the manuscript. All authors read and approved the final manuscript.
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Kaiyuan Zhang received his PhD degree in inorganic chemistry from Shandong University in 2021. Then, he works at the School of Chemistry and Chemical Engineering, Linyi University. His research focuses on developing Si/SiOx-based anode materials for lithium-ion batteries.
Xin Gu received his PhD degree in inorganic chemistry from Shandong University in 2014. After his postdoctoral research at the College of Science, China University of Petroleum (East China), he joined the College of New Energy, China University of Petroleum (East China). He is currently an associate professor. His work mainly focuses on the exploration of electrode materials for rechargeable batteries.
Zhao Qian received his PhD degree from KTH Royal Institute of Technology (Sweden) in 2013. After his postdoctoral research at Uppsala University (Sweden), he joined Shandong University (China). He is currently a full-time professor in materials science and engineering and mainly conducts research on computational materials science (DFT, First-principles, etc.) and electronic structure calculations/explorations.
Jian Yang received his BSc and PhD degrees from the University of Science and Technology of China. He joined the School of Chemistry and Chemical Engineering, Shandong University in 2011. His research interests focus on the development of new electrode materials for Na/Zn ion batteries, unraveling the underlying electrochemical reactions, and designing electrolyte additives/polymers for advanced batteries.
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Zhang, K., Zhao, D., Qian, Z. et al. N-doped Ti3C2Tx MXene sheet-coated SiOx to boost lithium storage for lithium-ion batteries. Sci. China Mater. 66, 51–60 (2023). https://doi.org/10.1007/s40843-022-2142-1
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DOI: https://doi.org/10.1007/s40843-022-2142-1