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Research Article | Online first | Published: 02 February 2024

Alloy/layer double hydroxide interphasic synergy via nano-heterointerfacing for highly reversible CO2 redox reaction in Li-CO2 batteries

Show Author's Information Tianzhen Jian1,  Wenqing Ma1,3,4( ),  Jiagang Hou2,  Jianping Ma4,  Xianhong Li4,  Haiyang Gao4,  Caixia Xu1( ),  Hong Liu1,3
Institute for Advanced Interdisciplinary Research (iAIR), Collaborative Innovation Center of Technology and Equipment for Biological Diagnosis and Therapy in Universities of Shandong, School of Chemistry and Chemical Engineering, University of Jinan, Jinan 250022, China
Kyiv College at Qilu University of Technology, Qilu University of Technology (Shandong Academy of Sciences), Jinan 250353, China
State Key Laboratory of Crystal Materials, Shandong University, Jinan 250100, China
Shandong Sacred Sun Power Sources Co., Ltd., Qufu 273100, China
Keywords:
interface, dealloying, nanoporous, heterojunction, Li-CO2 battery
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Air batteries
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Jian T, Ma W, Hou J, et al. Alloy/layer double hydroxide interphasic synergy via nano-heterointerfacing for highly reversible CO2 redox reaction in Li-CO2 batteries. Nano Research, 2024, https://doi.org/10.1007/s12274-024-6461-4
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Abstract Full text Electronic supplementary material About this article

Li-CO2 batteries are among the most intriguing techniques for balancing the carbon cycle, but are challenged by the annoyed thermodynamic barrier of the Li2CO3 decomposition reaction. Herein, we demonstrate the electrocatalytic performances of two-dimensional (2D) CoAl-layer double hydroxide (LDH) nanosheets can be significantly improved by trans-dimensional crosslinking with three-dimensional (3D) multilevel nanoporous (MP)-RuCoAl alloy (MP-RuCoAl alloy⊥CoAl-LDH). The MP-RuCoAl alloy⊥CoAl-LDH with multiscale pore channels and abundant nano-heterointerface is directly prepared by controllable etching Al from a Ru-Co-Al master alloy along with simultaneous partial oxidization of Al and Co atoms. The MP-RuCoAl is composed of various intermetallic compounds and Ru with abundant grain boundaries, and forms numerous heterointerface with 2D CoAl-LDH nanosheets. The multiscale porous metallic network benefits mass and electron transportation as well as discharge product storage and enables a rich multiphase reaction interface. In situ differential electrochemical mass spectrometry shows that the mass-to-charge ratio in the charging process is ~ 0.733 which is consistent with the theoretical value of 3/4, stating that the reversible co-decomposition of Li2CO3 and C can be achieved with the MP-RuCoAl alloy⊥CoAl-LDH. The Ketjen black (KB)/MP-RuCoAl⊥CoAl-LDH battery demonstrates a high cyclability for over 2270 h (227 cycles) with a lower voltage gap stabilized at ~ 1.3 V at 200 mA·g−1. Our findings here provide useful guidelines for developing high efficiency transition metal based electrocatalysts by coupling with conductive porous substrate for impelling the development of practical Li-CO2 battery systems.


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Electronic supplementary material
About this article

Alloy/layer double hydroxide interphasic synergy via nano-heterointerfacing for highly reversible CO2 redox reaction in Li-CO2 batteries

Show Author's information Tianzhen Jian1, Wenqing Ma1,3,4( ), Jiagang Hou2, Jianping Ma4, Xianhong Li4, Haiyang Gao4, Caixia Xu1( ), Hong Liu1,3
Institute for Advanced Interdisciplinary Research (iAIR), Collaborative Innovation Center of Technology and Equipment for Biological Diagnosis and Therapy in Universities of Shandong, School of Chemistry and Chemical Engineering, University of Jinan, Jinan 250022, China
Kyiv College at Qilu University of Technology, Qilu University of Technology (Shandong Academy of Sciences), Jinan 250353, China
State Key Laboratory of Crystal Materials, Shandong University, Jinan 250100, China
Shandong Sacred Sun Power Sources Co., Ltd., Qufu 273100, China

Abstract

Li-CO2 batteries are among the most intriguing techniques for balancing the carbon cycle, but are challenged by the annoyed thermodynamic barrier of the Li2CO3 decomposition reaction. Herein, we demonstrate the electrocatalytic performances of two-dimensional (2D) CoAl-layer double hydroxide (LDH) nanosheets can be significantly improved by trans-dimensional crosslinking with three-dimensional (3D) multilevel nanoporous (MP)-RuCoAl alloy (MP-RuCoAl alloy⊥CoAl-LDH). The MP-RuCoAl alloy⊥CoAl-LDH with multiscale pore channels and abundant nano-heterointerface is directly prepared by controllable etching Al from a Ru-Co-Al master alloy along with simultaneous partial oxidization of Al and Co atoms. The MP-RuCoAl is composed of various intermetallic compounds and Ru with abundant grain boundaries, and forms numerous heterointerface with 2D CoAl-LDH nanosheets. The multiscale porous metallic network benefits mass and electron transportation as well as discharge product storage and enables a rich multiphase reaction interface. In situ differential electrochemical mass spectrometry shows that the mass-to-charge ratio in the charging process is ~ 0.733 which is consistent with the theoretical value of 3/4, stating that the reversible co-decomposition of Li2CO3 and C can be achieved with the MP-RuCoAl alloy⊥CoAl-LDH. The Ketjen black (KB)/MP-RuCoAl⊥CoAl-LDH battery demonstrates a high cyclability for over 2270 h (227 cycles) with a lower voltage gap stabilized at ~ 1.3 V at 200 mA·g−1. Our findings here provide useful guidelines for developing high efficiency transition metal based electrocatalysts by coupling with conductive porous substrate for impelling the development of practical Li-CO2 battery systems.

Keywords: interface, dealloying, nanoporous, heterojunction, Li-CO2 battery

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Publication history
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Acknowledgements

Publication history

Received: 06 November 2023
Revised: 14 December 2023
Accepted: 29 December 2023
Published: 02 February 2024

Copyright

© Tsinghua University Press 2024

Acknowledgements

Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (No. 52201254), the Natural Science Foundation of Shandong Province (Nos. ZR2020QE012, ZR2020MB090, ZR2023ME155, and ZR2023ME085), the project of “20 Items of University” of Jinan (No. 202228046), and the Taishan Scholar Project of Shandong Province (No. tsqn202306226). The authors are grateful for the support provided by the Shandong Province Laboratory of Technology and Equipment for Molecular Diagnosis.

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