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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, Ali and Moradabadi, Ashkan and Martinaiou, Ioanna and Lauterbach, Stefan and Klemenz, Sebastian and Dolique, Stephanie and Kleebe, Hans-Joachim and Kaghazchi, Payam and Kramm, Ulrike I. (2017):
Elucidating the Origin of Hydrogen Evolution Reaction Activity in Mono- and Bimetallic Metal- and Nitrogen-Doped Carbon Catalysts (Me–N–C).
In: ACS Applied Materials & Interfaces, ACS Publications, pp. 25184-25193, 9, (30), ISSN 1944-8244, DOI: 10.1021/acsami.7b01647, [Online-Edition: https://doi.org/10.1021/acsami.7b01647],
[Article]

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. Based on structural analysis by X-ray diffraction, X-ray induced photoelectron spectroscopy and Transition 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 is formed and the energy of formation related to these sites integrated at the edge of a graphene layer, as obtained from 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 result 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 (HBE) on one MeN4 site due to 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.

Item Type: Article
Erschienen: 2017
Creators: Shahraei, Ali and Moradabadi, Ashkan and Martinaiou, Ioanna and Lauterbach, Stefan and Klemenz, Sebastian and Dolique, Stephanie and Kleebe, Hans-Joachim and Kaghazchi, Payam and Kramm, Ulrike I.
Title: Elucidating the Origin of Hydrogen Evolution Reaction Activity in Mono- and Bimetallic Metal- and Nitrogen-Doped Carbon Catalysts (Me–N–C)
Language: English
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. Based on structural analysis by X-ray diffraction, X-ray induced photoelectron spectroscopy and Transition 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 is formed and the energy of formation related to these sites integrated at the edge of a graphene layer, as obtained from 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 result 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 (HBE) on one MeN4 site due to 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.

Journal or Publication Title: ACS Applied Materials & Interfaces
Volume: 9
Number: 30
Publisher: ACS Publications
Divisions: 11 Department of Materials and Earth Sciences
11 Department of Materials and Earth Sciences > Earth Science
11 Department of Materials and Earth Sciences > Earth Science > Geo-Material-Science
11 Department of Materials and Earth Sciences > Material Science
11 Department of Materials and Earth Sciences > Material Science > Catalysts and Electrocatalysts
Date Deposited: 11 Dec 2018 11:43
DOI: 10.1021/acsami.7b01647
Official URL: https://doi.org/10.1021/acsami.7b01647
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