Single-Site AuI Catalyst for Silane Oxidation with Water

被引:194
作者
Chen, Zheng [1 ]
Zhang, Qi [2 ]
Chen, Wenxing [1 ]
Dong, Juncai [3 ]
Yao, Hurong [4 ]
Zhang, Xiangbo [1 ]
Tong, Xuanjue [1 ]
Wang, Dingsheng [1 ]
Peng, Qing [1 ]
Chen, Chen [1 ]
He, Wei [1 ,2 ]
Li, Yadong [1 ]
机构
[1] Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
[2] Tsinghua Univ, Sch Pharmaceut Sci, Beijing 100084, Peoples R China
[3] Chinese Acad Sci, Beijing Synchrotron Radiat Facil, Inst High Energy Phys, Beijing 100049, Peoples R China
[4] Chinese Acad Sci, CAS Key Lab Mol Nanostruct & Nanotechnol, Inst Chem, Beijing 100190, Peoples R China
基金
中国国家自然科学基金;
关键词
carbon nitrides; coordination environments; gold; mesoporous; single-site catalysis; SELECTIVE OXIDATION; HYDROGEN-PRODUCTION; ULTRASMALL NANOPARTICLES; HYDROLYTIC OXIDATION; GOLD NANOPARTICLES; CARBON NANOTUBE; ORGANOSILANES; ATOM; NANOCATALYSTS; NANOHYBRIDS;
D O I
10.1002/adma.201704720
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Single-site Au anchored on mpg-C3N4 (519 ppm Au loading) is developed as a highly active, selective, and stable catalyst for the oxidation of silanes with water with a turnover frequency as high as 50 200 h(-1), far exceeding most known catalysts based on total gold content. Other hydrosilanes bearing unsaturated functional groups also lead to corresponding silanols under mild reaction conditions without formation of any side products in good or excellent yields. The spherical aberration correction electron microscopy and extended X-ray absorption fine structure measurements both confirm the atomic dispersion of Au atoms stabilized by mpg-C3N4. The coordination of the catalytically active Au-I by three nitrogen or carbon atoms in the tri-s-triazine repeating units not only prevents the Au atoms from aggregation, but also renders the surface Au-I highly active, which is completely different than homogeneous Au-I species.
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页数:8
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