Tuning the Adsorption Energy of Methanol Molecules Along Ni-N-Doped Carbon Phase Boundaries by the Mott–Schottky Effect for Gas-Phase Methanol Dehydrogenation

Zhong Hua Xue, Jing Tan Han, Wei Jie Feng, Qiu Ying Yu, Xin Hao Li*, Markus Antonietti, Jie Sheng Chen

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

83 Scopus citations

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. A Mott–Schottky catalyst composed of Ni nanoparticles and tailorable nitrogen-doped carbon-foam (Ni/NCF) and thus tunable adsorption energy is presented 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), outpacing previously reported bench-marked transition-metal catalysts 10-fold.

Original languageEnglish (US)
Pages (from-to)2697-2701
Number of pages5
JournalAngewandte Chemie - International Edition
Volume57
Issue number10
DOIs
StatePublished - Mar 1 2018

Bibliographical note

Funding Information:
This work was supported by the National Natural Science Foundation of China (21720102002, 21722103, and 21673140), Shanghai Basic Research Program (16JC1401600), SJTU-MPI partner group, SJTU-Chuntsung Program (2017603), and the Shanghai Eastern Scholar Program and Shanghai Rising-Star Program (16QA1402100). The authors thank the Shanghai Synchrotron Radiation Facility for providing beam time (BL14W1).

Publisher Copyright:
© 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

Keywords

  • adsorption energy
  • gas–solid reactions
  • heterogeneous catalysis
  • Mott–Schottky effect
  • nanostructures

ASJC Scopus subject areas

  • Catalysis
  • General Chemistry

Fingerprint

Dive into the research topics of 'Tuning the Adsorption Energy of Methanol Molecules Along Ni-N-Doped Carbon Phase Boundaries by the Mott–Schottky Effect for Gas-Phase Methanol Dehydrogenation'. Together they form a unique fingerprint.

Cite this