Journal
ACS OMEGA
Volume 2, Issue 10, Pages 6852-6862Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsomega.7b01088
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Funding
- RFBR [14-29-04063, 15-03-07509, 15-29-01112, 16-33-00233, 16-03-00688, 16-33-60196]
- Council of the President of the Russian Federation [MK-6320.2016.3]
- Russian Science Foundation [17-13-01456]
- Volkswagen Foundation
- Ministry of Education and Science of the Russian Federation [RFMEFI61917X0007]
- Russian Science Foundation [17-13-01456] Funding Source: Russian Science Foundation
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The study tackles one of the challenges in developing platinum-free molecular electrocatalysts for hydrogen evolution, which is to seek for new possibilities to ensure large turnover numbers by stabilizing electrocatalytic intermediates. These species are often much more reactive than the initial electrocatalysts, and if not properly stabilized by a suitable choice of functionalizing substituents, they have a limited long-time activity. Here, we describe new iron and cobalt(II) cage complexes (clathrochelates) that in contrast to many previously reported complexes of this type do not act as electrocatalysts for hydrogen evolution. We argue that the most probable reason for this behavior is an excessive stabilization of the metal(I) species by perfluoroaryl ribbed groups, resulting in an unprecedented long-term stability of the metal(I) complexes even in acidic solutions.
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