H2activation by hydrogenase-inspired NiFe catalyst using frustrated Lewis pair: effect of buffer and halide ion in the heterolytic H-H bond cleavage

研究成果: Contribution to journalArticle査読

1 被引用数 (Scopus)

抄録

Hydrogen is a clean fuel alternative to fossil fuels, and it is vital to develop catalysts for its efficient activation and production. We investigate the reaction mechanism of H2activation in an aqueous solution by the recently developed NiFe complex (Ogoet al. Sci. Adv. 2020,6, eaaz8181) using density functional theory (DFT) calculation. Our computational results showed that H2is activated using frustrated Lewis pair. That is, H2binds to the Fe site of the NiFe complex, acting as a Lewis acid, while the added buffer, acting as Lewis base, abstracts protons to form a hydride complex. Furthermore, the higher basicity in the proton abstraction reaction characterises reaction more exergonic and lowers the reaction barrier. In addition, in the proton abstraction by the water molecule, the reaction barrier was lowered when anion such as Clis in the vicinity of the water. Understanding the chemical species that contribute to the catalytic process in cooperation with the metal catalyst at the atomic level should help to maximise the function of the catalyst.

本文言語英語
ページ(範囲)28420-28432
ページ数13
ジャーナルRSC Advances
11
45
DOI
出版ステータス出版済み - 8 17 2021

All Science Journal Classification (ASJC) codes

  • 化学 (全般)
  • 化学工学(全般)

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