Protonation/Deprotonation of Rutile TiO2 in Acid Aqueous Electrolytes

脱质子化 质子化 锐钛矿 无机化学 化学 金红石 电解质 水溶液 电化学 质子 质子输运 电极 离子 物理化学 有机化学 催化作用 光催化 物理 量子力学 生物化学
作者
Masahiro Shimizu,D. Nishida,Ayaka Kikuchi,Susumu Arai
出处
期刊:Journal of Physical Chemistry C [American Chemical Society]
卷期号:127 (36): 17677-17684 被引量:2
标识
DOI:10.1021/acs.jpcc.3c05069
摘要

The diversity of carrier ions in electrochemical devices has attracted much attention with regard to the use of protons. If the fast proton conduction originating from the Grötthuss mechanism can be utilized, the development of water-based rechargeable batteries that combine safety and rapid charge–discharge performance is expected. However, the narrow potential window of acid-based aqueous solutions limits the operation of active materials. In this work, the effect of the crystal structure on electrochemical protonation/deprotonation of TiO2 as a negative electrode material was systematically investigated using slurry-based composite electrodes. In the galvanostatic charge–discharge tests using a buffer electrolyte consisting of 1 M citric acid and 1 M trisodium citrate, the protonation of the rutile TiO2 proceeded at a higher potential than those of the anatase and brookite TiO2, resulting in reversible capacities of 102 and 87 mA h g–1 at the first cycle and 50th cycle, respectively, due to the decrease in irreversible hydrogen evolution. X-ray diffraction revealed that the protonation occurred inside the bulk, although the changes in the a and c axes during protonation/deprotonation were much smaller than those of Li+ and Na+ insertion. On the other hand, in particle sizes larger than 100 nm, the hydrogen evolution was dominant and the deprotonation was less in the anatase TiO2, and neither charging/discharging nor even the hydrogen generation occurred in the larger rutile TiO2. This is presumably due to the slow proton diffusion in the solid phases, which stalls the proton storage and induces the reduction of protons at the electrode–electrolyte interface. These obstacles should be overcome by nanosizing the particles and optimizing electrolyte compositions.
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