In operando X-ray absorption fine structure studies of polyoxometalate molecular cluster batteries: polyoxometalates as electron sponges

Journal of the American Chemical Society
Heng WangKunio Awaga

Abstract

We carried out in operando Mo K-edge X-ray absorption fine structure measurements on the rechargeable molecular cluster batteries (MCBs) of polyoxometalates (POMs), in which a Keggin-type POM, [PMo(12)O(40)](3-), is utilized as a cathode active material with a lithium metal anode. The POM-MCBs exhibit a large capacity of ca. 270 (A h)/kg in a voltage range between V = 4.0 V and V = 1.5 V. X-ray absorption near-edge structure analyses demonstrate that all 12 Mo(6+) ions in [PMo(12)O(40)](3-) are reduced to Mo(4+) in the discharging process. This means the formation of a super-reduced state of the POM, namely, [PMo(12)O(40)](27-), which stores 24 electrons, and this electron number can explain the large capacity of the POM-MCBs. Furthermore, extended X-ray absorption fine structure analyses reveal the molecular structure of [PMo(12)O(40)](27-), which is slightly reduced in size compared to the original [PMo(12)O(40)](3-) and involves Mo(4+) metal-metal-bonded triangles. Density functional theory calculations suggest that these triangles are formed because of the large number of additional electrons in the super-reduced state.

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Citations

Nov 9, 2016·Proceedings of the National Academy of Sciences of the United States of America·Venkateshkumar PrabhakaranJulia Laskin
Jan 17, 2017·Physical Chemistry Chemical Physics : PCCP·Han-Yi ChenUlrich Stimming
Mar 20, 2015·Dalton Transactions : an International Journal of Inorganic Chemistry·Sven HerrmannCarsten Streb
Mar 27, 2018·Dalton Transactions : an International Journal of Inorganic Chemistry·Shubiao XiaHong Guo
Mar 5, 2015·Physical Chemistry Chemical Physics : PCCP·Magda Pascual-BorràsJosep M Poblet
Feb 6, 2015·Dalton Transactions : an International Journal of Inorganic Chemistry·Rao Naumaan Nasim KhanYongge Wei
Jun 28, 2018·Physical Chemistry Chemical Physics : PCCP·Lijin GeorgeManu Jaiswal
Aug 11, 2018·Chemical Communications : Chem Comm·Tom HomewoodNuria Garcia-Araez
Apr 30, 2019·Dalton Transactions : an International Journal of Inorganic Chemistry·Benlong Luo, Li Xu
Jun 28, 2019·Chemistry, an Asian Journal·Yuyin WangHuan Pang
Jan 24, 2020·Chemistry : a European Journal·Xueying JiaYu-Fei Song
Jun 22, 2012·Dalton Transactions : an International Journal of Inorganic Chemistry·Heng WangKunio Awaga
May 25, 2013·Chemical Communications : Chem Comm·Wei-Peng ChenLi Xu
Sep 24, 2020·Chemical Communications : Chem Comm·Dongyang ShenBingan Lu
Jul 12, 2012·Chemical Society Reviews·Anna ProustGuillaume Izzet
Aug 4, 2012·Chemical Society Reviews·Haralampos N MirasLeroy Cronin
Aug 31, 2018·Frontiers in Chemistry·Aleksandar Kondinski, Tatjana N Parac-Vogt
Aug 7, 2012·Dalton Transactions : an International Journal of Inorganic Chemistry·Wei-Qiu KanJian-Fang Ma
May 9, 2013·Physical Chemistry Chemical Physics : PCCP·Shizheng WenGuanhua Chen

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