Electrocatalytic Hydrogen Evolution from a Cobaloxime-Based Metal–Organic Framework Thin Film

Roy, Souvik, Huang, Zhehao, Bhunia, Asamanjoy , Castner, Ashleigh, Gupta, Arvind K., Zou, Xiaodong and Ott, Sascha (2019) Electrocatalytic Hydrogen Evolution from a Cobaloxime-Based Metal–Organic Framework Thin Film. Journal of the American Chemical Society, 141 (40). pp. 15942-15950. ISSN 0002-7863

Full content URL: https://doi.org/10.1021/jacs.9b07084

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Item Type:Article
Item Status:Live Archive


Molecular hydrogen evolution catalysts (HECs) are synthetically tunable and often exhibit high activity, but they are also hampered by stability concerns and practical limitations associated with their use in the homogeneous phase. Their incorporation as integral linker units in metal–organic frameworks (MOFs) can remedy these shortcomings. Moreover, the extended three-dimensional structure of MOFs gives rise to high catalyst loadings per geometric surface area. Herein, we report a new MOF that exclusively consists of cobaloximes, a widely studied HEC, that act as metallo-linkers between hexanuclear zirconium clusters. When grown on conducting substrates and under applied reductive potential, the cobaloxime linkers promote electron transport through the film as well as function as molecular HECs. The obtained turnover numbers are orders of magnitude higher than those of any other comparable cobaloxime system, and the molecular integrity of the cobaloxime catalysts is maintained for at least 18 h of electrocatalysis. Being one of the very few hydrogen evolving electrocatalytic MOFs based on a redox-active metallo-linker, this work explores uncharted terrain for greater catalyst diversity and charge transport pathways.

Keywords:Thin films, Electrodes, Metal organic frameworks, Catalysts, Physical and chemical processes
Subjects:F Physical Sciences > F100 Chemistry
F Physical Sciences > F161 Organometallic Chemistry
Divisions:College of Science > School of Chemistry
ID Code:40662
Deposited On:17 Apr 2020 12:30

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