Rapid Mechanochemical Synthesis of Oxyhalide Superionic Conductor: Time-Resolved Structural Evolution

Denys Butenko; Jo-chi Tseng; Xinyu Zhang; Pencheng Yu; Wen Tang; Jiuwei Lei; Shuoxiao Zhang; Pengfei Wang; Yuhang Li; Ming Liu; Wen Yin; Liping Wang; Songbai Han; Wei Xia; Yusheng Zhao; Jinlong Zhu

doi:10.1002/smtd.202500947

Rapid Mechanochemical Synthesis of Oxyhalide Superionic Conductor: Time-Resolved Structural Evolution

Denys Butenko, Jo-chi Tseng^*, Xinyu Zhang^*, Pencheng Yu, Wen Tang, Jiuwei Lei, Shuoxiao Zhang, Pengfei Wang, Yuhang Li, Ming Liu, Wen Yin, Liping Wang, Songbai Han, Wei Xia^*, Yusheng Zhao, Jinlong Zhu^*

^*Corresponding author for this work

Department of Physics

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

3 Citations (Scopus)

Abstract

The design and synthesis of advanced solid electrolytes (SEs) underlie the development of safety and high-energy density all-solid-state batteries (ASSBs). Mechanochemical synthesis stands as the predominant method, yet it faces criticism due to its energy and time-intensive process (typically spanning several hours to days), presenting a significant obstacle to large-scale industrial production. Furthermore, ambiguity surrounding the formation mechanisms of SEs during mechanochemical reactions has limited optimization efforts. In addressing these challenges, evidence is presented that the efficiency of mechanochemical SE synthesis can achieve remarkable heights through process optimization. Specifically, the rapid synthesis of the state-of-the-art Li-Nb-O-Cl superionic conductor in only a few hours is highlighted, while concurrently demonstrating its superior electrochemical performance. Notably, for the first time, a structural evaluation during the mechanochemical reaction by time-resolved in situ synchrotron X-ray scattering experiments unveils a two-stage process. This expeditious mechanochemical synthesis of SEs establishes a foundational step toward the commercialization of ASSBs. © 2025 The Author(s). Small Methods published by Wiley-VCH GmbH

Original language	English
Article number	e00947
Number of pages	14
Journal	Small Methods
DOIs	https://doi.org/10.1002/smtd.202500947
Publication status	Online published - 6 Oct 2025

Funding

This work was supported by the National Natural Science Foundation of China under Grant No. W2433132, 12204219, 12275119, 51732005, the Shenzhen Science and Technology Program under Grant No. KQTD20200820113047086, the Zhejiang Provincial Natural Science Foundation of China under Grant No. LY23B030003, Natural Science Foundation of Ningbo under Grant No. 2023J200, the Shenzhen Key Laboratory of Solid State Batteries (SYSPG20241211173726011), the Guangdong Provincial Key Laboratory of Energy Materials for Electric Power (2018B030322001), the Guangdong-Hong Kong-Macao Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices (2019B121205001), the Key Laboratory of Energy Conversion and Storage Technologies (Southern University of Science and Technology), the Ministry of Education. The work was also supported by the Laboratory of Electrochemical Energy Storage Technologies, Academy for Advanced Interdisciplinary Studies (SUSTech), the Major Science and Technology Infrastructure Project of Material Genome Big-science Facilities Platform supported by Municipal Development and Reform Commission of Shenzhen, and the Center for Computational Science and Engineering at Southern University of Science and Technology. The synchrotron radiation experiments were performed at BL08W at SPring-8 with the approval of the Japan Synchrotron Radiation Research Institute (JASRI). The proposal numbers are 2021B2006, 2022B1508, and 2023A2341.

Research Keywords

all-solid-state batteries
anion-mixed chemistry
mechanochemistry
oxyhalide

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title = "Rapid Mechanochemical Synthesis of Oxyhalide Superionic Conductor: Time-Resolved Structural Evolution",

abstract = "The design and synthesis of advanced solid electrolytes (SEs) underlie the development of safety and high-energy density all-solid-state batteries (ASSBs). Mechanochemical synthesis stands as the predominant method, yet it faces criticism due to its energy and time-intensive process (typically spanning several hours to days), presenting a significant obstacle to large-scale industrial production. Furthermore, ambiguity surrounding the formation mechanisms of SEs during mechanochemical reactions has limited optimization efforts. In addressing these challenges, evidence is presented that the efficiency of mechanochemical SE synthesis can achieve remarkable heights through process optimization. Specifically, the rapid synthesis of the state-of-the-art Li-Nb-O-Cl superionic conductor in only a few hours is highlighted, while concurrently demonstrating its superior electrochemical performance. Notably, for the first time, a structural evaluation during the mechanochemical reaction by time-resolved in situ synchrotron X-ray scattering experiments unveils a two-stage process. This expeditious mechanochemical synthesis of SEs establishes a foundational step toward the commercialization of ASSBs. {\textcopyright} 2025 The Author(s). Small Methods published by Wiley-VCH GmbH",

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author = "Denys Butenko and Jo-chi Tseng and Xinyu Zhang and Pencheng Yu and Wen Tang and Jiuwei Lei and Shuoxiao Zhang and Pengfei Wang and Yuhang Li and Ming Liu and Wen Yin and Liping Wang and Songbai Han and Wei Xia and Yusheng Zhao and Jinlong Zhu",

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TY - JOUR

T1 - Rapid Mechanochemical Synthesis of Oxyhalide Superionic Conductor

T2 - Time-Resolved Structural Evolution

AU - Butenko, Denys

AU - Tseng, Jo-chi

AU - Zhang, Xinyu

AU - Yu, Pencheng

AU - Tang, Wen

AU - Lei, Jiuwei

AU - Zhang, Shuoxiao

AU - Wang, Pengfei

AU - Li, Yuhang

AU - Liu, Ming

AU - Yin, Wen

AU - Wang, Liping

AU - Han, Songbai

AU - Xia, Wei

AU - Zhao, Yusheng

AU - Zhu, Jinlong

PY - 2025/10/6

Y1 - 2025/10/6

N2 - The design and synthesis of advanced solid electrolytes (SEs) underlie the development of safety and high-energy density all-solid-state batteries (ASSBs). Mechanochemical synthesis stands as the predominant method, yet it faces criticism due to its energy and time-intensive process (typically spanning several hours to days), presenting a significant obstacle to large-scale industrial production. Furthermore, ambiguity surrounding the formation mechanisms of SEs during mechanochemical reactions has limited optimization efforts. In addressing these challenges, evidence is presented that the efficiency of mechanochemical SE synthesis can achieve remarkable heights through process optimization. Specifically, the rapid synthesis of the state-of-the-art Li-Nb-O-Cl superionic conductor in only a few hours is highlighted, while concurrently demonstrating its superior electrochemical performance. Notably, for the first time, a structural evaluation during the mechanochemical reaction by time-resolved in situ synchrotron X-ray scattering experiments unveils a two-stage process. This expeditious mechanochemical synthesis of SEs establishes a foundational step toward the commercialization of ASSBs. © 2025 The Author(s). Small Methods published by Wiley-VCH GmbH

AB - The design and synthesis of advanced solid electrolytes (SEs) underlie the development of safety and high-energy density all-solid-state batteries (ASSBs). Mechanochemical synthesis stands as the predominant method, yet it faces criticism due to its energy and time-intensive process (typically spanning several hours to days), presenting a significant obstacle to large-scale industrial production. Furthermore, ambiguity surrounding the formation mechanisms of SEs during mechanochemical reactions has limited optimization efforts. In addressing these challenges, evidence is presented that the efficiency of mechanochemical SE synthesis can achieve remarkable heights through process optimization. Specifically, the rapid synthesis of the state-of-the-art Li-Nb-O-Cl superionic conductor in only a few hours is highlighted, while concurrently demonstrating its superior electrochemical performance. Notably, for the first time, a structural evaluation during the mechanochemical reaction by time-resolved in situ synchrotron X-ray scattering experiments unveils a two-stage process. This expeditious mechanochemical synthesis of SEs establishes a foundational step toward the commercialization of ASSBs. © 2025 The Author(s). Small Methods published by Wiley-VCH GmbH

KW - all-solid-state batteries

KW - anion-mixed chemistry

KW - mechanochemistry

KW - oxyhalide

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DO - 10.1002/smtd.202500947

M3 - RGC 21 - Publication in refereed journal

SN - 2366-9608

JO - Small Methods

JF - Small Methods

M1 - e00947

ER -

Rapid Mechanochemical Synthesis of Oxyhalide Superionic Conductor: Time-Resolved Structural Evolution

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