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Nat Commun. 2015 Aug 7;6:7992. doi: 10.1038/ncomms8992.

Molecular metal-Nx centres in porous carbon for electrocatalytic hydrogen evolution.

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Max-Planck-Institute for Polymer Research, Ackermannweg 10, 55128 Mainz, Germany.
Department of Chemistry and Food Chemistry &Center for Advancing Electronics Dresden (cfaed), Technische Universität Dresden, Mommsenstrasse 4, 01062 Dresden, Germany.


Replacement of precious platinum with efficient and low-cost catalysts for electrocatalytic hydrogen evolution at low overpotentials holds tremendous promise for clean energy devices. Here we report a novel type of robust cobalt-nitrogen/carbon catalyst for the hydrogen evolution reaction (HER) that is prepared by the pyrolysis of cobalt-N4 macrocycles or cobalt/o-phenylenediamine composites and using silica colloids as a hard template. We identify the well-dispersed molecular CoNx sites on the carbon support as the active sites responsible for the HER. The CoNx/C catalyst exhibits extremely high turnover frequencies per cobalt site in acids, for example, 0.39 and 6.5 s(-1) at an overpotential of 100 and 200 mV, respectively, which are higher than those reported for other scalable non-precious metal HER catalysts. Our results suggest the great promise of developing new families of non-precious metal HER catalysts based on the controlled conversion of homogeneous metal complexes into solid-state carbon catalysts via economically scalable protocols.

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