Photochemical H2 activation by an Zn–Fe heterometallic: a mechanistic investigation

文献情報

出版日 2023-12-14

DOI 10.1039/D3SC05966A

インパクトファクター 9.825

著者

Marina Perez-Jimenez, Mark R. Crimmin

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要旨

Addition of H2 to a Zn–Fe complex was observed to occur under photochemical conditions (390 or 428 nm LED) and leads to the formation of a heterometallic dihydride complex. The reaction does not occur under thermal conditions and DFT calculations suggest this is an endergonic, light driven process. Through a combined experimental and computational approach, the plausible mechanisms for H2 activation were investigated. Inhibition experiments, double-label cross-over experiments, radical trapping experiments, EPR spectroscopy and DFT calculations were used to gain insight into this system. The combined data are consistent with two plausible mechanisms, the first involving ligand dissociation followed by oxidative addition of H2 at the Fe centre, the second involving homolytic fragmentation of the Zn–Fe heterometallic and formation of radical intermediates.

掲載誌

Chemical Science

CiteScore: 14.4

自己引用率: 3.9%

年間論文数: 1413

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Photochemical H2 activation by an Zn–Fe heterometallic: a mechanistic investigation

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