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Single-atomic nickel supported on nitrogen-doped porous carbon to boost polysulfide conversion in lithium-sulfur batteries

Ni单原子负载氮掺杂多孔碳促进锂硫电池中的多硫化物转化

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Abstract

Single-atomic catalysts consisting of atomically dispersed metal sites within nitrogen-doped carbon matrix (M SAC@NC) have emerged as high-performance electrocatalytic materials in Li-S batteries due to their maximum atom utilization, unique physicochemical properties, and superior catalytic activity. In the present work, a series of M SAC@NC (M = Ni, Co, Fe) with similar structural and physicochemical properties have been successfully prepared by the combination of physical adsorption and pyrolysis. The combination of the aberration-corrected high-angle annular dark-field scanning transmission electron microscopy and X-ray adsorption spectra indicates the successful formation of single-atomic metal sites. Moreover, the catalytic activity trend toward sulfur redox reaction is observed to be Ni SAC@NC > Co SAC@NC > Fe SAC@NC, and the Ni SAC@NC delivers the highest capacity of 1,280.6 mAh g−1 and long-time stability at a decay rate of 0.07% per cycle for 800 cycles at 0.5 C, demonstrating excellent battery performance.

摘要

由分散在氮掺杂碳载体上的原子级金属位点组成的单原子催化剂(M SAC@NC) 因其具有最大的原子利用率、 独特的物理化学性质和优异的催化活性, 已成为Li-S电池中的高性能电催化材料. 本文采用物理吸附和热解相结合的方法, 成功制备了一系列具有相似结构和理化性质的M SAC@NC (M = Ni, Co, Fe). 双球差校正高角环形暗场扫描透射电子显微镜和X射线吸收光谱表明成功形成了单原子金属位点. 此外, 对硫氧化还原反应的催化活性趋势为Ni SAC@NC > Co SAC@NC > Fe SAC@NC, 其中Ni SAC@NC在0.5 C下表现出1280.6 mAh g−1的最高容量, 循环800次后, 平均每圈容量衰减率仅为0.07%, 具有优异的电池性能.

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Acknowledgements

This work is financially supported by the Key Research and Development Program of Hunan Province, China (2023GK2015) and the Science and Technology Innovation Leader Program of Hunan Province (2022RC3049). Fundamental Research Funds for the Central Universities (202044011), Natural Science Foundation of Changsha (KQ2208259)

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Authors and Affiliations

  1. School of Materials Science and Engineering, Central South University, Changsha, 410083, China

    Leyuan Chen  (陈乐园), Yanyan Sun  (孙焱焱), Zhi Chang  (常智), Simin Chai  (柴思敏), Qiong He  (何琼) & Anqiang Pan  (潘安强)

  2. School of Materials Science and Engineering, Xinjiang University, Urumqi, 830046, China

    Anqiang Pan  (潘安强)

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  1. Leyuan Chen  (陈乐园)
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  2. Yanyan Sun  (孙焱焱)
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  3. Zhi Chang  (常智)
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Contributions

Author contributions Chen L performed the experiments and data analysis and drafted the manuscript. Chang Z, Cai S and He Q provided experimental help and assisted in analyzing the experimental data. Sun Y and Pan A supervised the project and revised the original manuscript. All authors contributed to the general discussion.

Corresponding authors

Correspondence to Yanyan Sun  (孙焱焱) or Anqiang Pan  (潘安强).

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Conflict of interest The authors declare no conflict of interest.

Additional information

Supplementary information Experimental details and supporting data are available in the online version of the paper.

Leyuan Chen is a Master’s candidate at Central South University under the supervision of Prof Anqiang Pan. Her current interest focuses on the effect of transition metal single-atom catalysts on the performance of lithium-sulfur batteries.

Yanyan Sun received her PhD from the Technical University of Berlin in 2018 under the supervision of Professor Peter Strasser who is an expert in electrochemistry, and stayed in the group to continue her postdoctoral research. After that, she joined in the Central South University. Her research focuses on the design of functionalized carbon-based materials for electrocatalysis and electrosynthesis as well as sodium-ion batteries.

Anqiang Pan received his BE (2005) and PhD (2011) degrees in materials physics and chemistry from the Central South University. He joined the faculty of the Central South University in 2012 and was promoted to a Sheng-Hua Professor in 2013. His current interests are controllable synthesis of nanostructured materials and their applications in energy storage and conversion devices, such as LIBs, ZIBs and supercapacitors.

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40843_2024_2934_MOESM1_ESM.pdf

Single-Atomic Nickel Supported on Nitrogen-Doped Porous Carbon to Boost Polysulfide Conversion in Lithium-Sulfur Batteries

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Chen, L., Sun, Y., Chang, Z. et al. Single-atomic nickel supported on nitrogen-doped porous carbon to boost polysulfide conversion in lithium-sulfur batteries. Sci. China Mater. 67, 1938–1946 (2024). https://doi.org/10.1007/s40843-024-2934-9

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