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 language | English (US) |
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Article number | 2001493 |
Journal | Advanced Science |
Volume | 8 |
Issue number | 3 |
DOIs | |
State | Published - Feb 3 2021 |
Keywords
- N-doped carbon
- charge modulation
- covalent triazine frameworks
- sintering-resistance
ASJC Scopus subject areas
- Medicine (miscellaneous)
- Chemical Engineering(all)
- Materials Science(all)
- Biochemistry, Genetics and Molecular Biology (miscellaneous)
- Engineering(all)
- Physics and Astronomy(all)