LiZn/LiAlO2/Li2O‐Derived Chemical Confinement Enabling Hierarchical and Oriented Li Plating/Stripping

ABSTRACT ZnO with good lithiophilicity has widely been employed to modify the lithiophobic substrates and facilitate uniform lithium (Li) deposition. The overpotential of ZnO‐derived Li anode during cycling depends on the lithiophilicity of both LiZn and Li2O products upon lithiation of ZnO. However...

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Main Authors: Huaming Qian, Xifei Li, Qinchuan Chen, Jingjing Wang, Xiaohua Pu, Wei Xiao, Yanyan Cao, Mengxin Bai, Wenbin Li, Zhengdong Ma, Guiqiang Cao, Ruixian Duan, Gaini Zhang, Kaihua Xu, Kun Zhang, Wei Yan, Jiujun Zhang
Format: Article
Language:English
Published: Wiley 2025-05-01
Series:Carbon Energy
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Online Access:https://doi.org/10.1002/cey2.714
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author Huaming Qian
Xifei Li
Qinchuan Chen
Jingjing Wang
Xiaohua Pu
Wei Xiao
Yanyan Cao
Mengxin Bai
Wenbin Li
Zhengdong Ma
Guiqiang Cao
Ruixian Duan
Gaini Zhang
Kaihua Xu
Kun Zhang
Wei Yan
Jiujun Zhang
author_facet Huaming Qian
Xifei Li
Qinchuan Chen
Jingjing Wang
Xiaohua Pu
Wei Xiao
Yanyan Cao
Mengxin Bai
Wenbin Li
Zhengdong Ma
Guiqiang Cao
Ruixian Duan
Gaini Zhang
Kaihua Xu
Kun Zhang
Wei Yan
Jiujun Zhang
author_sort Huaming Qian
collection DOAJ
description ABSTRACT ZnO with good lithiophilicity has widely been employed to modify the lithiophobic substrates and facilitate uniform lithium (Li) deposition. The overpotential of ZnO‐derived Li anode during cycling depends on the lithiophilicity of both LiZn and Li2O products upon lithiation of ZnO. However, the striking differences in the lithiophilicity between Li2O and LiZn would result in a high overpotential during cycling. In this research, the Al2O3/nZnO (n ≥ 1) hybrid layers were precisely fabricated by atomic layer deposition (ALD) to regulate the lithiophilicity of ZnO phase and Li2O/LiZn configuration—determining the actual Li loading amount and Li plating/stripping processes. Theoretically, the Li adsorption energy (Ea) values of LiZn and Li2O in the LiZn/Li2O configuration are separately predicted as −2.789 and −3.447 eV. In comparison, the Ea values of LiZn, LiAlO2, and Li2O in the LiZn/LiAlO2/Li2O configuration upon lithiation of Al2O3/8ZnO layer are calculated as −2.899, −3.089, and −3.208 eV, respectively. Importantly, a novel introduction of LiAlO2 into the LiZn/Li2O configuration could enable the hierarchical Li plating/stripping and reduce the overpotentials during cycling. Consequently, the Al2O3/8ZnO‐derived hybrid Li‐metal anode could exhibit electrochemical performances superior to these of ZnO‐derived Li anode in both symmetrical and full cells paired with a LiNi0.6Co0.2Mn0.2O2 (NCM622) cathode.
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spelling doaj-art-879f4e42272f43ef9b5f8c7b1453af4f2025-08-20T03:22:19ZengWileyCarbon Energy2637-93682025-05-0175n/an/a10.1002/cey2.714LiZn/LiAlO2/Li2O‐Derived Chemical Confinement Enabling Hierarchical and Oriented Li Plating/StrippingHuaming Qian0Xifei Li1Qinchuan Chen2Jingjing Wang3Xiaohua Pu4Wei Xiao5Yanyan Cao6Mengxin Bai7Wenbin Li8Zhengdong Ma9Guiqiang Cao10Ruixian Duan11Gaini Zhang12Kaihua Xu13Kun Zhang14Wei Yan15Jiujun Zhang16Key Materials & Components of Electrical Vehicles for Overseas Expertise Introduction Center for Discipline Innovation, School of Materials Science and Engineering, Institute of Advanced Electrochemical Energy Xi'an University of Technology Xi'an Shaanxi ChinaKey Materials & Components of Electrical Vehicles for Overseas Expertise Introduction Center for Discipline Innovation, School of Materials Science and Engineering, Institute of Advanced Electrochemical Energy Xi'an University of Technology Xi'an Shaanxi ChinaKey Materials & Components of Electrical Vehicles for Overseas Expertise Introduction Center for Discipline Innovation, School of Materials Science and Engineering, Institute of Advanced Electrochemical Energy Xi'an University of Technology Xi'an Shaanxi ChinaKey Materials & Components of Electrical Vehicles for Overseas Expertise Introduction Center for Discipline Innovation, School of Materials Science and Engineering, Institute of Advanced Electrochemical Energy Xi'an University of Technology Xi'an Shaanxi ChinaKey Materials & Components of Electrical Vehicles for Overseas Expertise Introduction Center for Discipline Innovation, School of Materials Science and Engineering, Institute of Advanced Electrochemical Energy Xi'an University of Technology Xi'an Shaanxi ChinaKey Materials & Components of Electrical Vehicles for Overseas Expertise Introduction Center for Discipline Innovation, School of Materials Science and Engineering, Institute of Advanced Electrochemical Energy Xi'an University of Technology Xi'an Shaanxi ChinaKey Materials & Components of Electrical Vehicles for Overseas Expertise Introduction Center for Discipline Innovation, School of Materials Science and Engineering, Institute of Advanced Electrochemical Energy Xi'an University of Technology Xi'an Shaanxi ChinaKey Materials & Components of Electrical Vehicles for Overseas Expertise Introduction Center for Discipline Innovation, School of Materials Science and Engineering, Institute of Advanced Electrochemical Energy Xi'an University of Technology Xi'an Shaanxi ChinaKey Materials & Components of Electrical Vehicles for Overseas Expertise Introduction Center for Discipline Innovation, School of Materials Science and Engineering, Institute of Advanced Electrochemical Energy Xi'an University of Technology Xi'an Shaanxi ChinaKey Materials & Components of Electrical Vehicles for Overseas Expertise Introduction Center for Discipline Innovation, School of Materials Science and Engineering, Institute of Advanced Electrochemical Energy Xi'an University of Technology Xi'an Shaanxi ChinaKey Materials & Components of Electrical Vehicles for Overseas Expertise Introduction Center for Discipline Innovation, School of Materials Science and Engineering, Institute of Advanced Electrochemical Energy Xi'an University of Technology Xi'an Shaanxi ChinaKey Materials & Components of Electrical Vehicles for Overseas Expertise Introduction Center for Discipline Innovation, School of Materials Science and Engineering, Institute of Advanced Electrochemical Energy Xi'an University of Technology Xi'an Shaanxi ChinaKey Materials & Components of Electrical Vehicles for Overseas Expertise Introduction Center for Discipline Innovation, School of Materials Science and Engineering, Institute of Advanced Electrochemical Energy Xi'an University of Technology Xi'an Shaanxi ChinaGEM Co. Ltd. Shenzhen Guangdong ChinaGEM Co. Ltd. Shenzhen Guangdong ChinaCollege of Materials Science and Engineering Fuzhou University Fuzhou Fujian ChinaCollege of Materials Science and Engineering Fuzhou University Fuzhou Fujian ChinaABSTRACT ZnO with good lithiophilicity has widely been employed to modify the lithiophobic substrates and facilitate uniform lithium (Li) deposition. The overpotential of ZnO‐derived Li anode during cycling depends on the lithiophilicity of both LiZn and Li2O products upon lithiation of ZnO. However, the striking differences in the lithiophilicity between Li2O and LiZn would result in a high overpotential during cycling. In this research, the Al2O3/nZnO (n ≥ 1) hybrid layers were precisely fabricated by atomic layer deposition (ALD) to regulate the lithiophilicity of ZnO phase and Li2O/LiZn configuration—determining the actual Li loading amount and Li plating/stripping processes. Theoretically, the Li adsorption energy (Ea) values of LiZn and Li2O in the LiZn/Li2O configuration are separately predicted as −2.789 and −3.447 eV. In comparison, the Ea values of LiZn, LiAlO2, and Li2O in the LiZn/LiAlO2/Li2O configuration upon lithiation of Al2O3/8ZnO layer are calculated as −2.899, −3.089, and −3.208 eV, respectively. Importantly, a novel introduction of LiAlO2 into the LiZn/Li2O configuration could enable the hierarchical Li plating/stripping and reduce the overpotentials during cycling. Consequently, the Al2O3/8ZnO‐derived hybrid Li‐metal anode could exhibit electrochemical performances superior to these of ZnO‐derived Li anode in both symmetrical and full cells paired with a LiNi0.6Co0.2Mn0.2O2 (NCM622) cathode.https://doi.org/10.1002/cey2.714atomic layer depositionhierarchical Li plating/strippinghybrid LiZn/LiAlO2/Li2O configurationLi‐metal anodelithiophilicity regulationoverpotential regulation
spellingShingle Huaming Qian
Xifei Li
Qinchuan Chen
Jingjing Wang
Xiaohua Pu
Wei Xiao
Yanyan Cao
Mengxin Bai
Wenbin Li
Zhengdong Ma
Guiqiang Cao
Ruixian Duan
Gaini Zhang
Kaihua Xu
Kun Zhang
Wei Yan
Jiujun Zhang
LiZn/LiAlO2/Li2O‐Derived Chemical Confinement Enabling Hierarchical and Oriented Li Plating/Stripping
Carbon Energy
atomic layer deposition
hierarchical Li plating/stripping
hybrid LiZn/LiAlO2/Li2O configuration
Li‐metal anode
lithiophilicity regulation
overpotential regulation
title LiZn/LiAlO2/Li2O‐Derived Chemical Confinement Enabling Hierarchical and Oriented Li Plating/Stripping
title_full LiZn/LiAlO2/Li2O‐Derived Chemical Confinement Enabling Hierarchical and Oriented Li Plating/Stripping
title_fullStr LiZn/LiAlO2/Li2O‐Derived Chemical Confinement Enabling Hierarchical and Oriented Li Plating/Stripping
title_full_unstemmed LiZn/LiAlO2/Li2O‐Derived Chemical Confinement Enabling Hierarchical and Oriented Li Plating/Stripping
title_short LiZn/LiAlO2/Li2O‐Derived Chemical Confinement Enabling Hierarchical and Oriented Li Plating/Stripping
title_sort lizn lialo2 li2o derived chemical confinement enabling hierarchical and oriented li plating stripping
topic atomic layer deposition
hierarchical Li plating/stripping
hybrid LiZn/LiAlO2/Li2O configuration
Li‐metal anode
lithiophilicity regulation
overpotential regulation
url https://doi.org/10.1002/cey2.714
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