Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 57, Issue 40, Pages 13163-13166Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201807717
Keywords
electrocatalysis; energy efficiency; hydrogen evolution reaction; nanostructures; primary amine oxidation
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Funding
- National Natural Science Foundation of China [21871206]
- Natural Science Foundation of Tianjin City [17JCJQJC44700]
- China Postdoctoral Science Foundation [2018M630269]
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For electrocatalytic water splitting, the sluggish anodic oxygen evolution reaction (OER) restricts the cathodic hydrogen evolution reaction (HER). Therefore, developing an alternative anodic reaction with accelerating kinetics to produce value-added chemicals, especially coupled with HER, is of great importance. Now, a thermodynamically more favorable primary amine (-CH2-NH2) electrooxidation catalyzed by NiSe nanorod arrays in water is reported to replace OER for enhancing HER. The increased H-2 production can be obtained at cathode; meanwhile, a variety of aromatic and aliphatic primary amines are selectively electrooxidized to nitriles with good yields at the anode. Mechanistic investigations suggest that Ni-II/Ni-III may serve as the redox active species for the primary amines transformation. Hydrophobic nitrile products can readily escape from aqueous electrolyte/electrode interface, avoiding the deactivation of the catalyst and thus contributing to continuous gram-scale synthesis.
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