Proton-Driven Intercalation and Ion Substitution Utilizing Solid-State Electrochemical Reaction

Masaya Fujioka, Chuanbao Wu, Naoki Kubo, Gaoyang Zhao, Atsushi Inoishi, Shigeto Okada, Satoshi Demura, Hideaki Sakata, Manabu Ishimaru, Hideo Kaiju, Junji Nishii

Research output: Contribution to journalArticlepeer-review

13 Citations (Scopus)


The development of an unconventional synthesis method has a large potential to drastically advance materials science. In this research, a new synthesis method based on a solid-state electrochemical reaction was demonstrated, which can be made available for intercalation and ion substitution. It was referred to as proton-driven ion introduction (PDII). The protons generated by the electrolytic dissociation of hydrogen drive other monovalent cations along a high electric field in the solid state. Utilizing this mechanism, Li+, Na+, K+, Cu+, and Ag+ were intercalated into a layered TaS2 single crystal while maintaining high crystallinity. This liquid-free process of ion introduction allows the application of high voltage around several kilovolts to the sample. Such a high electric field strongly accelerates ion substitution. Actually, compared to conventional solid-state reaction, PDII introduced 15 times the amount of K into Na super ionic conductor (NASICON)-structured Na3-xKxV2(PO4)3. The obtained materials exhibited a thermodynamically metastable phase, which has not been reported so far. This concept and idea for ion introduction is expected to form new functional compounds and/or phases.

Original languageEnglish
Pages (from-to)17987-17993
Number of pages7
JournalJournal of the American Chemical Society
Issue number49
Publication statusPublished - 13 Dec 2017
Externally publishedYes


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