Revisiting the Role of Hydrogen in Lithium-Rich Antiperovskite Solid Electrolytes: New Insight in Lithium Ion and Hydrogen Dynamics

Ling，Sifan1,2; Deng，Bei1,3; Zhao，Ruo4; Lin，Haibin1; Kong，Long5; Zhang，Ruiqin6; Lu，Zhouguang7; Bian，Juncao1; Zhao，Yusheng1,2

2022

10.1002/aenm.202202847

Advanced Energy Materials   Impact Factor & Quartile

1614-6832

1614-6840

LiOHX (X = Cl or Br) with an antiperovskite structure possess the advantages of low melting point, low cost, and ease of scaling-up, which show great promise for applications in all-solid-state Li metal batteries (ASSLMBs). However, Li-ion transport mechanisms in LiOHX are still debated and the influence of H on the electrochemical performance of LiOHX is yet to be explored. Herein, combining the theoretical calculations and experimental measurements, it is found that H affects Li-ion transport, crystal stability, electrochemical stability, and electronic conductivity of LiOHX. Compared with H-free LiOCl, although H helps to generate vacancy-like defects, the electrostatic repulsive force between H and Li-ion leads to an increase in both the activation energy and the diffusion length (space compensation effect), resulting in special Li ion transport trajectories along the Li-O plane. Decreasing H content reduces the electronic conductivity and enhances the reduction-resistant ability of LiOHX, promoting the cycling stability and rate performance of Li∣LiOHX∣Li symmetric cells and the ASSLMBs. This work delivers a new insight into the role of H in antiperovskite LiOHX and can serve as guidance for solid electrolyte design.

Li-ion conduction mechanism Li-rich antiperovskite rotational motion solid electrolytes space compensation

SCI

English

First ; Corresponding

Guangdong Basic and Applied Basic Research Foundation[2021A1515012403] ; Basic Research Project of Science and Technology Innovation Commission of Shenzhen[JSGG20191129111001820] ; Key Program of the National Natural Science Foundation of China[51732005] ; Guangdong Provincial Key Laboratory of Energy Materials for Electric Power[2018B030322001] ; Guangdong-Hong Kong-Macao Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices[2019B121205001] ; National Natural Science Foundation of China["12004214","22005134","U22A20439"] ; China Postdoctoral Science Foundation[2021M702282] ; Shenzhen Science and Technology Program[KQTD20200820113047086]

Chemistry ; Energy & Fuels ; Materials Science ; Physics

Chemistry, Physical ; Energy & Fuels ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter

WOS:000891022200001

WILEY-V C H VERLAG GMBH

2-s2.0-85142850701

Scopus

1.Guangdong Provincial Key Laboratory of Energy Materials for Electric Power & Guangdong-Hong Kong-Macao Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices,Academy for Advanced Interdisciplinary Studies,Southern University of Science and Technology,Shenzhen,518055,China
2.Department of Physics,Southern University of Science and Technology,Shenzhen,518055,China
3.Shenzhen Research Institute,Shandong University,Shenzhen,518057,China
4.Institute for Advanced Study,Shenzhen University,Shenzhen,518055,China
5.Frontiers Science Center for Flexible Electronics and Xi'an Institute of Flexible Electronics (IFE),Northwestern Polytechnical University,Xi'an,710129,China
6.Department of Physics,City University of Hong Kong,Kowloon,Hong Kong
7.Department of Materials Science and Engineering,Southern University of Science and Technology,Shenzhen,518055,China

Ling，Sifan,Deng，Bei,Zhao，Ruo,et al. Revisiting the Role of Hydrogen in Lithium-Rich Antiperovskite Solid Electrolytes: New Insight in Lithium Ion and Hydrogen Dynamics[J]. Advanced Energy Materials,2022.

Ling，Sifan.,Deng，Bei.,Zhao，Ruo.,Lin，Haibin.,Kong，Long.,...&Zhao，Yusheng.(2022).Revisiting the Role of Hydrogen in Lithium-Rich Antiperovskite Solid Electrolytes: New Insight in Lithium Ion and Hydrogen Dynamics.Advanced Energy Materials.

Ling，Sifan,et al."Revisiting the Role of Hydrogen in Lithium-Rich Antiperovskite Solid Electrolytes: New Insight in Lithium Ion and Hydrogen Dynamics".Advanced Energy Materials (2022).