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  Tuning the adsorption energy of methanol molecules along Ni-N-doped carbon phase boundaries via the Mott-Schottky effect for highly efficient dehydrogenation of gas-phase methanol

Xue, Z.-H., Han, J.-T., Feng, W.-J., Yu, Q.-Y., Li, X.-H., Antonietti, M., et al. (2018). Tuning the adsorption energy of methanol molecules along Ni-N-doped carbon phase boundaries via the Mott-Schottky effect for highly efficient dehydrogenation of gas-phase methanol. Angewandte Chemie International Edition, 57(10), 2697-2701. doi:10.1002/anie.201713429.

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Item Permalink: http://hdl.handle.net/21.11116/0000-0000-3AE9-9 Version Permalink: http://hdl.handle.net/21.11116/0000-0000-CC8E-B
Genre: Journal Article

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 Creators:
Xue, Zhong-Hua, Author
Han, Jing-Tan, Author
Feng, Wei-Jie, Author
Yu, Qiu-Ying, Author
Li, Xin-Hao, Author
Antonietti, Markus1, Author              
Chen, Jie-Sheng, Author
Affiliations:
1Markus Antonietti, Kolloidchemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_1863321              

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Free keywords: heterogeneous catalysis, Mott-Schottky effect, Nanostructures, adsorption energy, gas-solid reactions
 Abstract: Engineering the adsorption of molecules on active sites is an integral and challenging part for the design of highly efficient transition-metal-based catalysts for methanol dehydrogenation. Here we report a Mott-Schottky catalyst composed of Ni nanoparticles and tailorable nitrogen-doped carbon-foam (Ni/NCF) and thus tunable adsorption energy for highly efficient and selective dehydrogenation of gas-phase methanol to hydrogen and CO even under relatively high weight hourly space velocities (WHSV). Both theoretical and experimental results reveal the key role of the rectifying contact at the Ni/NCF boundaries in tailoring the electron density of Ni species and enhancing the absorption energies of methanol molecules, which leads to a remarkably high turnover frequency (TOF) value (356 mol methanol mol−1 Ni h−1 at 350 °C), 10-fold outpacing the bench-marked transition-metal catalysts in the literature.

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 Dates: 2018-01-172018-03-01
 Publication Status: Published in print
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 Identifiers: DOI: 10.1002/anie.201713429
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Title: Angewandte Chemie International Edition
  Other : Angew. Chem., Int. Ed.
  Other : Angew. Chem. Int. Ed.
  Other : Angewandte Chemie, International Edition
Source Genre: Journal
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Publ. Info: Weinheim : Wiley-VCH
Pages: - Volume / Issue: 57 (10) Sequence Number: - Start / End Page: 2697 - 2701 Identifier: ISSN: 1433-7851