Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 134, Issue 48, Pages 19915-19921Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja310246r
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Funding
- World Premier International Research Center (WPI) initiative on Materials Nanoarchitectonics, MEXT, Japan
- CREST of the Japan Science and Technology Agency (JST)
- JSPS KAKENHI [24310095]
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The topochemical transformation from transition-metal brucite hydroxide (Co1-xFex(OH)(2), Co(OH)(2), Co1-xNix(OH)(2)) to corresponding (Co2+-(Co3+)-Fe3+, Co2+-(Ni2+)-Co3+) LDH under oxidizing halogen agents (iodine, bromine) exhibits different staging phenomena depending on the metallic composition/ratio in starting brucite. A plausible charge hopping mechanism based on valence interchange between redoxable charge center (Fe3+/Co3+) and neighboring divalent sites in the host sheet is proposed to understand the restoration of electron donor sites at the interface between brucite crystallites and halogen agents, which ensures a continual oxidative reaction, and a staged intercalation/diffusion of in situ reduced halide anions into the interlayer gallery commensurate with the host charge propagation. The discussion on the correlation between staging product and metallic composition/ratio offers a general perspective and new insights into M2+/M3+ ratio and cation ordering, host layer charge, and phase evolution in LDH structure.
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