Resolving nanostructure and chemistry of solid-electrolyte interphase on lithium anodes by depth-sensitive plasmon-enhanced Raman spectroscopy.
Yu Gu, En-Ming You, Jian-De Lin, Jun-Hao Wang, Si-Heng Luo, Ru-Yu Zhou, Chen-Jie Zhang, Jian-Lin Yao, Hui-Yang Li, Gen Li, Wei-Wei Wang, Yu Qiao, Jia-Wei Yan, De-Yin Wu, Guo-Kun Liu, Li Zhang, Jian-Feng Li, Rong Xu, Zhong-Qun Tian, Yi Cui, Bing-Wei Mao
Author Information
Yu Gu: State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, China. ORCID
En-Ming You: State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, China. ORCID
Jian-De Lin: State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, China.
Jun-Hao Wang: State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, China.
Si-Heng Luo: State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, China.
Ru-Yu Zhou: State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, China.
Chen-Jie Zhang: College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou, China.
Jian-Lin Yao: College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou, China.
Hui-Yang Li: State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, China.
Gen Li: State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, China. ORCID
Wei-Wei Wang: State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, China.
Yu Qiao: State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, China. ORCID
Jia-Wei Yan: State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, China. ORCID
De-Yin Wu: State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, China. ORCID
Guo-Kun Liu: State Key Laboratory of Marine Environmental Science, College of the Environment and Ecology, Xiamen University, Xiamen, China.
Li Zhang: State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, China.
Jian-Feng Li: State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, China. ORCID
Rong Xu: Department of Materials Science and Engineering, Stanford University, Stanford, CA, USA.
Zhong-Qun Tian: State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, China. zqtian@xmu.edu.cn. ORCID
Yi Cui: Department of Materials Science and Engineering, Stanford University, Stanford, CA, USA. yicui@stanford.edu. ORCID
Bing-Wei Mao: State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, China. bwmao@xmu.edu.cn.
The solid-electrolyte interphase (SEI) plays crucial roles for the reversible operation of lithium metal batteries. However, fundamental understanding of the mechanisms of SEI formation and evolution is still limited. Herein, we develop a depth-sensitive plasmon-enhanced Raman spectroscopy (DS-PERS) method to enable in-situ and nondestructive characterization of the nanostructure and chemistry of SEI, based on synergistic enhancements of localized surface plasmons from nanostructured Cu, shell-isolated Au nanoparticles and Li deposits at different depths. We monitor the sequential formation of SEI in both ether-based and carbonate-based dual-salt electrolytes on a Cu current collector and then on freshly deposited Li, with dramatic chemical reconstruction. The molecular-level insights from the DS-PERS study unravel the profound influences of Li in modifying SEI formation and in turn the roles of SEI in regulating the Li-ion desolvation and the subsequent Li deposition at SEI-coupled interfaces. Last, we develop a cycling protocol that promotes a favorable direct SEI formation route, which significantly enhances the performance of anode-free Li metal batteries.
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