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  Ultrathin 2D Fe-Nanosheets Stabilized by 2D Mesoporous Silica: Synthesis and Application in Ammonia Synthesis

Fan, H., Folke, J. M., Liu, Z., Girgsdies, F., Imlau, R., Ruland, H., et al. (2021). Ultrathin 2D Fe-Nanosheets Stabilized by 2D Mesoporous Silica: Synthesis and Application in Ammonia Synthesis. ACS Applied Materials and Interfaces, 13(25), 30187-30197. doi:10.1021/acsami.1c06771.

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 Creators:
Fan, Hua1, 2, 3, Author              
Folke, Jan Markus1, Author
Liu, Zigeng1, 4, Author
Girgsdies, Frank2, Author              
Imlau, Robert5, Author
Ruland, Holger1, Author
Heumann, Saskia1, Author
Granwehr, Josef4, 6, Author
Eichel, Rüdiger-A.4, 7, Author
Schlögl, Robert2, 4, Author              
Frei, Elias2, Author              
Huang, Xing1, 2, 3, Author              
Affiliations:
1Department of Heterogeneous Reactions, Max Planck Institute for Chemical Energy Conversion, 45470 Mülheim an der Ruhr, Germany; , ou_persistent22              
2Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              
3Fuzhou University, 350108 Fuzhou, P. R. China, ou_persistent22              
4Institute of Energy and Climate Research - Fundamental Electrochemistry (IEK-9), Forschungszentrum , Jülich, 52425 Jülich, Germany, ou_persistent22              
5Materials & Structural Analysis, Thermo Fisher Scientific, Achtseweg Noord 5, 5651 GG Eindhoven, Netherlands, ou_persistent22              
6Institute of Technical and Macromolecular Chemistry, RWTH Aachen University, 52074 Aachen, Germany, ou_persistent22              
7Institute of Physical Chemistry, RWTH Aachen University, 52074 Aachen, Germany, ou_persistent22              

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 Abstract: Developing high-performance Fe-based ammonia catalysts through simple and cost-efficient methods has received an increased level of attention. Herein, we report for the first time, the synthesis of two-dimensional (2D) FeOOH nanoflakes encapsulated by mesoporous SiO2 (mSiO2) via a simple solution-based method for ammonia synthesis. Due to the sticking of the mSiO2 coating layers and the limited spaces in between, the Fe after reduction retains the 2D morphology, showing high resistance against the sintering in the harsh Haber–Bosch process. Compared to supported Fe particles dispersed on mSiO2 spheres, the coated catalyst shows a significantly improved catalytic activity by 50% at 425 °C. Thermal desorption spectroscopy (TDS) reveals the existence of a higher density of reactive sites for N2 activation in the 2D Fe catalyst, which is possibly coupled to a larger density of surface defect sites (kinks, steps, point defects) that are generally considered as active centers in ammonia synthesis. Besides the structural impact of the coating on the 2D Fe, the electronic one is elucidated by partially substituting Si with Al in the coating, confirmed by 29Si and 27Al magic-angle spinning nuclear magnetic resonance (MAS NMR). An increased apparent activation energy (Ea) of the Al-containing catalyst evidences an influence on the nature of the active site. The herein-developed stable 2D Fe nanostructures can serve as an example of a 2D material applied in catalysis, offering the chance of a rational catalyst design based on a stepwise introduction of various promoters, in the coating and on the metal, maintaining the spatial control of the active centers.

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Language(s): eng - English
 Dates: 2021-04-132021-06-022021-06-152021-06-30
 Publication Status: Published in print
 Pages: 11
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/acsami.1c06771
 Degree: -

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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: 11 Volume / Issue: 13 (25) Sequence Number: - Start / End Page: 30187 - 30197 Identifier: ISSN: 1944-8244
CoNE: https://pure.mpg.de/cone/journals/resource/1944-8244