Enhancing sodium-ion storage performance of MoO2/N-doped carbon through interfacial Mo-N-C bond

通过构筑界面 Mo-N-C 键提高 MoO2/氮掺杂碳复 合材料的钠离子存储性能

Abstract

Na-ion batteries (SIBs) have attracted considerable attention as promising alternatives to commercial Li-ion batteries (LIBs) due to comparable redox potential, and natural abundance of Na. However, it remains challenging to explore suitable anodes for SIBs. Herein, a MoO2/N-doped carbon (MoO2/N-C) composite composed of MoO2 nanocrystals embedded within carbon matrix with a Mo-N-C chemical bond is prepared by a simple yet effective carbonization-induced topochemical transformation route. Na-ion half-cells using MoO2/N-C exhibit excellent cycling stability over 5000 cycles at 5 A g−1 and superior rate capability. Physicochemical characterizations and first principles density functional theory (DFT) simulations reveal that the formation of chemical bond at the interface between MoO2 and N-doped carbon plays an important role in the excellent charge storage properties of MoO2/N-C. More importantly, the interfacial coupling can efficiently promote interface charge transfer. Benefiting from this, Na-ion capacitors (SICs) constructed with the MoO2/N-C anode and activated carbon cathode can deliver an impressive energy density of 15 W h kg−1 at a power density of 1760 W kg−1, together with a capacitance retention of 92.4% over 1000 cycles at 10 A g−1. The proposed strategy in this paper based on interfacial chemical bond may hold pro mises for the design of high-performance electrodes for energy storage devices.

摘要

钠离子电池因具有与锂离子电池接近的工作电压且具有丰 富的钠资源优势而受到广泛关注, 并有望成为商业化锂离子电池 的替代产品. 然而, 开发合适的钠离子电池负极材料仍存在一些挑 战. 本文通过一种简单有效的碳化诱导拓扑化学转化法合成了一 种MoO2/氮掺杂碳复合材料(MoO2/N-C), 其中MoO2纳米晶嵌入在 氮掺杂的碳基质里, 并与之形成Mo–N–C键. 用该MoO2/N-C复合 材料组装的钠离子半电池具有很好的倍率性能和循环稳定性, 可 在5 A g−1的电流密度下循环超5000周. 物理化学表征和基于密度 泛函理论的第一性原理计算表明, MoO2和氮掺杂碳界面上的化学 键合对复合材料电化学性能的提高起了重要作用. 更重要的是, 该 化学键合可有效促进界面上的电荷转移. 基于此, 用该复合材料和 活化碳组装的钠离子电容器在1760 W kg−1功率密度下可提供 15 W h kg−1的能量密度, 同时在10 A g−1的电流密度下循环1000周 后具有92.4%的电容保持率. 本文介绍的界面化学键的构筑有望为 面向储能器件的高性能电极的设计提供参考.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (51804089) and the Guangxi Key Laboratory of Electrochemical and Magneto-chemical Functional Materials (EMFM20181114). Zhao X thanks the support of the research starting foundation of CAEP (PY20200038).

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Contributions

Huang B and Zhao X designed and prepared the samples; Liu S, Li Y, Yang J, Chen Q, Xiao S and Zhang W performed the characterizations and data analysis; Wang HE finished the first-principles calculation; Huang B and Zhao X wrote the paper with support from Cao G; Cao G contributed to the theoretical analysis. All authors contributed to the general discussion.

Corresponding authors

Correspondence to Xu Zhao 赵煦 or Hong-En Wang 王洪恩 or Guozhong Cao 曹国忠.

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The authors declare that they have no conflict of interest.

Supplementary information

Supporting data are available in the online version of the paper.

Bin Huang received his BSc degree (2009) and MSc degree (2012) from the College of Chemistry and Chemical Engineering, Central South University, and received his PhD degree (2016) from the School of Metallurgy and Environment, Central South University. In January 2017, he joined the College of Chemistry and Bioengineering, Guilin University of Technology. His current research focuses on the processing and modification of electrode materials for lithium- & sodium-ion batteries.

Xu Zhao is currently an assistant professor of the Department of Energetic Materials at the Institute of Chemical Materials, China Academy of Engineering Physics (ICM, CAEP). He obtained his PhD degree from Harbin Institute of Technology in 2019. From 2015 to 2017, he was a visiting scholar in Prof. Guozhong Cao’s group at the Materials Science and Engineering, University of Washington. His current research focuses on the design of high-performance energetic materials and advanced electrodes for electrochemical energy storage devices.

Hong-En Wang received his PhD degree from the City University of Hong Kong (2012). Then he worked as an associate professor at Wuhan University of Technology (2012–2019). He joined the College of Physics and Electronics Information of Yunnan Normal University in 2020. His current research interests mainly focus on photovoltaic materials, nanostructured electrode materials for Li/Na-ion and Li-S batteries, etc.

Guozhong Cao is Boeing-Steiner professor of Materials Science and Engineering, professor of Chemical Engineering and adjunct professor of Mechanical Engineering at the University of Washington, Seattle, WA. He is one of the Thomson Reuters Highly Cited Researchers with a total citation of 42,000 and an h-index of 102. His current research focuses on the chemical processing of nanomaterials for solar cells, batteries, and supercapacitors as well as actuators and sensors.

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Huang, B., Liu, S., Zhao, X. et al. Enhancing sodium-ion storage performance of MoO2/N-doped carbon through interfacial Mo-N-C bond. Sci. China Mater. (2020). https://doi.org/10.1007/s40843-020-1370-x

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Keywords

  • topochemical transformation
  • Mo-N chemical bond
  • Na-ion batteries
  • Na-ion capacitor
  • density functional theory simulations