Efficient electron transfer across hydrogen bond interfaces by proton-coupled and -uncoupled pathways

Tao Cheng, Dong Xue Shen, Miao Meng, Suman Mallick, Lijiu Cao, Nathan J. Patmore, Hong Li Zhang, Shan Feng Zou, Huo Wen Chen, Yi Qin, Yi Yang Wu and Chun Y. Liu ()
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Tao Cheng: Jinan University
Dong Xue Shen: Jinan University
Miao Meng: Jinan University
Suman Mallick: Jinan University
Lijiu Cao: Jinan University
Nathan J. Patmore: University of Huddersfield, Queensgate
Hong Li Zhang: Jinan University
Shan Feng Zou: Jinan University
Huo Wen Chen: Jinan University
Yi Qin: Jinan University
Yi Yang Wu: Jinan University
Chun Y. Liu: Jinan University

Nature Communications, 2019, vol. 10, issue 1, 1-10

Abstract: Abstract Thermal electron transfer through hydrogen bonds remains largely unexplored. Here we report the study of electron transfer through amide-amide hydrogen bonded interfaces in mixed-valence complexes with covalently bonded Mo2 units as the electron donor and acceptor. The rate constants for electron transfer through the dual hydrogen bonds across a distance of 12.5 Å are on the order of ∼ 1010 s−1, as determined by optical analysis based on Marcus–Hush theory and simulation of ν(NH) vibrational band broadening, with the electron transfer efficiencies comparable to that of π conjugated bridges. This work demonstrates that electron transfer across a hydrogen bond may proceed via the known proton-coupled pathway, as well as an overlooked proton-uncoupled pathway that does not involve proton transfer. A mechanistic switch between the two pathways can be achieved by manipulation of the strengths of electronic coupling and hydrogen bonding. The knowledge of the non-proton coupled pathway has shed light on charge and energy transport in biological systems.

Date: 2019
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DOI: 10.1038/s41467-019-09392-7

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