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

被引：55

作者：

Zhang, Zihao ^{[1
,3
,4
]}

Yao, Siyu ^{[1
]}

Hu, Xiaobing ^{[5
,6
]}

Okejiri, Francis ^{[3
,4
]}

He, Kun ^{[5
,6
]}

Liu, Pingying ^{[7
]}

Tian, Ziqi ^{[7
]}

Dravid, Vinayak P. ^{[5
,6
]}

Fu, Jie ^{[1
,8
]}

Zhu, Xiang ^{[2
]}

Dai, Sheng ^{[3
,4
]}

机构：

[1] Zhejiang Univ, Key Lab Biomass Chem Engn, Minist Educ, Coll Chem & Biol Engn, Hangzhou 310027, Peoples R China

[2] Chinese Acad Sci, State Key Lab Oxo Synth & Select Oxidat, Suzhou Res Inst, Lanzhou Inst Chem Phys, Lanzhou 730000, Peoples R China

[3] Univ Tennessee, Dept Chem, Knoxville, TN 37996 USA

[4] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA

[5] Northwestern Univ, Dept Mat Sci & Engn, Evanston, IL 60208 USA

[6] Northwestern Univ, NUANCE Ctr, Evanston, IL 60208 USA

[7] Chinese Acad Sci, Ningbo Inst Mat Technol & Engn, Ningbo 315201, Zhejiang, Peoples R China

[8] Inst Zhejiang Univ Quzhou, 78 Jiuhua Blvd North, Quzhou 324000, Peoples R China

来源：

ADVANCED SCIENCE | 2021年 / 8卷 / 03期

基金：

中国国家自然科学基金;

关键词：

charge modulation; covalent triazine frameworks; N‐ doped carbon; sintering‐ resistance; METAL-ORGANIC FRAMEWORK; POROUS CARBON; TRANSFER HYDROGENATION; NANOPOROUS CARBON; CATALYSTS; NANOPARTICLES; OXIDATION; REDUCTION;

D O I：

10.1002/advs.202001493

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

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 degrees C under N-2 atmosphere. Predictably, the dispersed Ru on pristine CTF carrier suffered severe sintering of the Ru nanoparticles (NPs) during heat treatment at 900 degrees 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.

引用

页数：8

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