Sacrificial Synthesis of Supported Ru Single Atoms and Clusters on N-doped Carbon Derived from Covalent Triazine Frameworks: A Charge Modulation Approach

Zihao Zhang, Siyu Yao, Xiaobing Hu, Francis Okejiri, Kun He, Pingying Liu, Ziqi Tian, Vinayak P. Dravid, Jie Fu*, Xiang Zhu, Sheng Dai

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

1 Scopus citations

Abstract

High-temperature pyrolysis of nitrogen (N)-rich, crystalline porous organic architectures in the presence of a metal precursor is an important chemical process in heterogeneous catalysis for the fabrication of highly porous N-carbon-supported metal catalysts. Herein, covalent triazine framework (CTF) and CTF-I (that is, CTF after charge modulation with iodomethane) are presented as sacrificial templates, for the synthesis of carbon-supported Ru catalysts—Ru-CTF-900 and Ru-CTF-I-900 respectively, following high-temperature pyrolysis at 900 °C under N2 atmosphere. Predictably, the dispersed Ru on pristine CTF carrier suffered severe sintering of the Ru nanoparticles (NPs) during heat treatment at 900 °C. However, the Ru-CTF-I-900 catalyst is composed of ultra-small Ru NPs and abundant Ru single atoms which may have resulted from much stronger Ru-N interactions. Through modification of the micro-environment within the CTF architecture, Ru precursor interacted on charged-modulated CTF framework shows electrostatic repulsion and steric hindrance, thus contributing toward the high density of single Ru atoms and even smaller Ru NPs after pyrolysis. A Ru-Ru coordination number of only 1.3 is observed in the novel Ru-CTF-I-900 catalyst, which exhibits significantly higher catalytic activity than Ru-CTF-900 for transfer hydrogenation of acetophenone.

Original languageEnglish (US)
Article number2001493
JournalAdvanced Science
Volume8
Issue number3
DOIs
StatePublished - Feb 3 2021

Keywords

  • N-doped carbon
  • charge modulation
  • covalent triazine frameworks
  • sintering-resistance

ASJC Scopus subject areas

  • Medicine (miscellaneous)
  • Chemical Engineering(all)
  • Biochemistry, Genetics and Molecular Biology (miscellaneous)
  • Materials Science(all)
  • Engineering(all)
  • Physics and Astronomy(all)

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