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Electrocatalytic reduction of protons to hydrogen by a copper complex of the pentadentate ligand Dmphen-DPA in a nonaqueous electrolyte

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Abstract

A copper complex based on the pentadentate aminopyridine ligand [(9-methyl-1,10-phenanthrolin-2-yl)methyl]bis-(pyridin-2-ylmethyl)amine (Dmphen-DPA), namely [Cu(Dmphen-DPA)](ClO4)2 (1), was synthesized and characterized by elemental analysis, HR-MS spectroscopy and X-ray single crystal diffraction. The complex has five-coordinated solid-state structures, but has an open coordination site in acetonitrile. The electrochemical studies reveal that complex 1 has an electrocatalytic proton reduction activity in acetonitrile, when using acetic acid as a proton source with icat/ip ∼ 2.5. DFT calculations suggest that the parent copper complex undergoes two successive reductions to generate the radical species [Cu(I)(Dmphen-DPA˙)]0, which is protonated at the low-valence copper center to afford a reactive CuII–H intermediate. The CuII–H species combines bimolecularly and generates H2 via reductive elimination.

Graphical abstract: Electrocatalytic reduction of protons to hydrogen by a copper complex of the pentadentate ligand Dmphen-DPA in a nonaqueous electrolyte

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Publication details

The article was received on 18 Aug 2019, accepted on 21 Oct 2019 and first published on 21 Oct 2019


Article type: Paper
DOI: 10.1039/C9NJ04275J
New J. Chem., 2019, Advance Article

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    Electrocatalytic reduction of protons to hydrogen by a copper complex of the pentadentate ligand Dmphen-DPA in a nonaqueous electrolyte

    Y. Gao, Y. Zhao, X. Song, R. Huang, Y. Meng, J. Wang, W. Wang and C. Chen, New J. Chem., 2019, Advance Article , DOI: 10.1039/C9NJ04275J

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