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Proton-Driven Intercalation and Ion Substitution Utilizing Solid-State Electrochemical Reaction
Journal of the American Chemical Society ( IF 15.0 ) Pub Date : 2017-11-16 , DOI: 10.1021/jacs.7b09328
Masaya Fujioka 1 , Chuanbao Wu 2 , Naoki Kubo 1 , Gaoyang Zhao 2 , Atsushi Inoishi 3 , Shigeto Okada 3 , Satoshi Demura 4 , Hideaki Sakata 4 , Manabu Ishimaru 5 , Hideo Kaiju 1 , Junji Nishii 1
Affiliation  

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.

中文翻译:

利用固态电化学反应的质子驱动插层和离子取代

非常规合成方法的发展具有极大地推动材料科学发展的潜力。在这项研究中,展示了一种基于固态电化学反应的新合成方法,可用于嵌入和离子取代。它被称为质子驱动的离子引入(PDII)。氢的电解解离产生的质子在固态下沿着高电场驱动其他单价阳离子。利用这种机制,Li+、Na+、K+、Cu+ 和Ag+ 被嵌入层状TaS2 单晶中,同时保持高结晶度。这种无液体的离子引入过程允许向样品施加大约几千伏的高压。如此高的电场强烈地加速了离子置换。实际上,与传统的固态反应相比,PDII 向 Na 超离子导体 (NASICON) 结构的 Na3-xKxV2(PO4)3 中引入了 15 倍的 K。获得的材料表现出热力学亚稳态相,迄今为止尚未报道。这种离子引入的概念和想法有望形成新的功能化合物和/或相。
更新日期:2017-11-16
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