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  Elucidating the Origin of Hydrogen Evolution Reaction Activity in Mono- and Bimetallic Metal- and Nitrogen-Doped Carbon Catalysts (Me-N-C)

Shahraei, A., Moradabadi, A., Martinaiou, I., Lauterbach, S., Klemenz, S., Dolique, S., et al. (2017). Elucidating the Origin of Hydrogen Evolution Reaction Activity in Mono- and Bimetallic Metal- and Nitrogen-Doped Carbon Catalysts (Me-N-C). ACS Applied Materials and Interfaces, 9(30), 25184-25193. doi:10.1021/acsami.7b01647.

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Shahraei, Ali1, Author
Moradabadi, Ashkan1, Author
Martinaiou, Ioanna1, Author
Lauterbach, Stefan1, Author
Klemenz, Sebastian2, Author              
Dolique, Stephanie1, Author
Kleebe, Hans-Joachim1, Author
Kaghazchi, Payam1, Author
Kramm, Ulrike L.1, Author
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1External Organizations, ou_persistent22              
2Inorganic Chemistry, Max Planck Institute for Chemical Physics of Solids, Max Planck Society, ou_1863425              

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 Abstract: In this work, we present a comprehensive study on the role of metal species in MOF-based Me-N-C (mono- and bimetallic) catalysts for the hydrogen evolution reaction (HER). The catalysts are investigated with respect to HER activity and stability in alkaline electrolyte. On the basis of the structural analysis by X-ray diffraction, X-ray-induced photoelectron spectroscopy, and transmission electron microscopy, it is concluded that MeN4 sites seem to dominate the HER activity of these catalysts. There is a strong relation between the amount of MeN4 sites that are formed and the energy of formation related to these sites integrated at the edge of a graphene layer, as obtained from density functional theory (DFT) calculations. Our results show, for the first time, that the combination of two metals (Co and Mo) in a bimetallic (Co,Mo)-N-C catalyst allows hydrogen production with a significantly improved overpotential in comparison to its monometallic counterparts and other Me-N-C catalysts. By the combination of experimental results with DFT calculations, we show that the origin of the enhanced performance of our (Co,Mo)-N-C catalyst seems to be provided by an improved hydrogen binding energy on one MeN4 site because of the presence of a second MeN4 site in its close vicinity, as investigated in detail for our most active (Co,Mo)-N-C catalyst. The outstanding stability and good activity make especially the bimetallic Me-N-C catalysts interesting candidates for solar fuel applications.

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Language(s): eng - English
 Dates: 2017-06-272017-06-27
 Publication Status: Published in print
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 Rev. Type: -
 Identifiers: ISI: 000407089300014
DOI: 10.1021/acsami.7b01647
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Title: ACS Applied Materials and Interfaces
  Abbreviation : ACS Appl. Mater. Interfaces
Source Genre: Journal
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Publ. Info: Washington, DC : American Chemical Society
Pages: - Volume / Issue: 9 (30) Sequence Number: - Start / End Page: 25184 - 25193 Identifier: ISSN: 1944-8244
CoNE: https://pure.mpg.de/cone/journals/resource/1944-8244