期刊
ADVANCED MATERIALS
卷 32, 期 25, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.201902177
关键词
conducting polymers; electrocatalysis; hydrogen bonds; hydrogen evolution reaction; polydopamine
类别
资金
- Austrian Science Fund (FWF) [FWF I3822-N37]
- Government of Upper Austria within the Sabbatical program Internationalization of the University of Linz
- Linz Institute of Technology (LIT)
- Upper Austrian Government [LIT-2017-4-YOU-005]
- Austrian Federal Ministry of Science, Research and Economy
- National Foundation for Research, Technology and Development
- Natural Sciences and Engineering Research Council (NSERC) of Canada
The most active and efficient catalysts for the electrochemical hydrogen evolution reaction (HER) rely on platinum, a fact that increases the cost of producing hydrogen and thereby limits the widespread adoption of this fuel. Here, a metal-free organic electrocatalyst that mimics the platinum surface by implementing a high work function and incorporating hydrogen-affine hydrogen bonds is introduced. These motifs, inspired from enzymology, are deployed here as selective reaction centres. It is shown that the keto-amine hydrogen-bond motif enhances the rate-determining step in proton reduction to molecular hydrogen. The keto-amine-functionalized polymers reported herein evolve hydrogen at an overpotential of 190 mV. They share certain key properties with platinum: a similar work function and excellent electrochemical stability and chemical robustness. These properties allow the demonstration of one week of continuous HER operation without notable degradation nor delamination from the carrier electrode. Scaled continuous-flow electrolysis is reported and 1 L net molecular hydrogen is produced within less than 9 h using 2.3 mg of polymer electrocatalyst.
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