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Nano Research 2023, 16(8): 11473-11485 https://doi.org/10.1007/s12274-023-5795-7
Research Article | Issue | Published: 03 June 2023

Single-atomic Zn-(C/N/O) lithiophilic sites induced stable lithium plating/stripping in anode-free lithium metal battery

Show Author's Information Shifei Huang1,2,  Sirong Lu3,  Yao Lv1,4,  Nanrui Li1,2,  Zhenwei Wu5,  Geng Zhong1,2,  Xiaolong Ren1,2,  Yufeng Wang1,2,  Bo Sun1,2,  Yuxiong Huang2,6,  Feiyu Kang1,2( ),  Yidan Cao1,2( )
Institute of Materials Research, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen 518055, China
Tsinghua-Berkeley Shenzhen Institute, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen 518055, China
Shenzhen Institute for Quantum Science and Engineering, Southern University of Science and Technology, Shenzhen 518055, China
College of Sciences and Institute for Sustainable Energy, Shanghai University, Shanghai 200444, China
Shell Catalysts & Technologies, Shell Technology Center Houston, Houston TX 77082-3101, USA
Institute of Environment and Ecology, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen 518055, China
Keywords:
carbon, lithium dendrite, lithiophilic sites, anode-free, single atomic zinc
Topics:
Anodes
Cite this article:
Huang S, Lu S, Lv Y, et al. Single-atomic Zn-(C/N/O) lithiophilic sites induced stable lithium plating/stripping in anode-free lithium metal battery. Nano Research, 2023, 16(8): 11473-11485. https://doi.org/10.1007/s12274-023-5795-7
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Abstract Full text Electronic supplementary material About this article

For anode-free lithium metal battery, lithiophilic surface modification on the current collector can effectively reduce the lithium nucleation barrier, so as to regulate the electrodeposition of lithium. Here, atomically dispersed Zn-(C/N/O) lithiophilic sites in the amorphous carbon medium were introduced onto Cu by an in-situ induced ion coordination chemistry strategy to get the modified Zn@NC@RGO@Cu current collector. X-ray absorption spectroscopy (XAS) combined with scanning transmission electron microscopy in high angle annular dark field (STEM-HAADF) analysis proved the single atomic state of the zinc sites surrounded by C, N, and O with a coordination number of ~ 3. According to the electrochemical tests and first principle calculations, the ultra-uniformly dispersed Zn-(C/N/O) sites at the atomic level can effectively improve the lithium affinity, reduce the energy barrier for lithium nucleation, homogenize the lithium nucleation, and enhance an inorganic lithium compounds rich solid electrolyte interphase layer. As a result, the nucleation overpotential of lithium on the modified current collector was reduced to 7.7 mV, which was 5.4 times lower than that on bare Cu. Uniform lithium nucleation and deposition enabled stable Li plating/stripping and elevated Coulombic efficiency of 98.95% in Li||Cu cell after > 850 cycles. Capacity retention of 89.7% was successfully achieved in the anode-free lithium metal battery after 100 cycles.


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Abstract
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Electronic supplementary material
About this article

Single-atomic Zn-(C/N/O) lithiophilic sites induced stable lithium plating/stripping in anode-free lithium metal battery

Show Author's information Shifei Huang1,2, Sirong Lu3, Yao Lv1,4, Nanrui Li1,2, Zhenwei Wu5, Geng Zhong1,2, Xiaolong Ren1,2, Yufeng Wang1,2, Bo Sun1,2, Yuxiong Huang2,6, Feiyu Kang1,2( ), Yidan Cao1,2( )
Institute of Materials Research, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen 518055, China
Tsinghua-Berkeley Shenzhen Institute, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen 518055, China
Shenzhen Institute for Quantum Science and Engineering, Southern University of Science and Technology, Shenzhen 518055, China
College of Sciences and Institute for Sustainable Energy, Shanghai University, Shanghai 200444, China
Shell Catalysts & Technologies, Shell Technology Center Houston, Houston TX 77082-3101, USA
Institute of Environment and Ecology, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen 518055, China

Abstract

For anode-free lithium metal battery, lithiophilic surface modification on the current collector can effectively reduce the lithium nucleation barrier, so as to regulate the electrodeposition of lithium. Here, atomically dispersed Zn-(C/N/O) lithiophilic sites in the amorphous carbon medium were introduced onto Cu by an in-situ induced ion coordination chemistry strategy to get the modified Zn@NC@RGO@Cu current collector. X-ray absorption spectroscopy (XAS) combined with scanning transmission electron microscopy in high angle annular dark field (STEM-HAADF) analysis proved the single atomic state of the zinc sites surrounded by C, N, and O with a coordination number of ~ 3. According to the electrochemical tests and first principle calculations, the ultra-uniformly dispersed Zn-(C/N/O) sites at the atomic level can effectively improve the lithium affinity, reduce the energy barrier for lithium nucleation, homogenize the lithium nucleation, and enhance an inorganic lithium compounds rich solid electrolyte interphase layer. As a result, the nucleation overpotential of lithium on the modified current collector was reduced to 7.7 mV, which was 5.4 times lower than that on bare Cu. Uniform lithium nucleation and deposition enabled stable Li plating/stripping and elevated Coulombic efficiency of 98.95% in Li||Cu cell after > 850 cycles. Capacity retention of 89.7% was successfully achieved in the anode-free lithium metal battery after 100 cycles.

Keywords: carbon, lithium dendrite, lithiophilic sites, anode-free, single atomic zinc

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Publication history

Received: 23 March 2023
Revised: 29 April 2023
Accepted: 01 May 2023
Published: 03 June 2023
Issue date: August 2023

Copyright

© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

This work was supported by Department of Science and Technology of Guangdong Province (No. 211233812024), Guangdong Basic and Applied Basic Research Foundation (No. 2021A1515110871), Shenzhen Science and Technology Program (Nos. JCYJ20220818101007016 and JCYJ20210324140804013), and Tsinghua Shenzhen International Graduate School (No. QD2021005N).

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