Heterogeneous synergistic catalysis by Ru-RuO x nanoparticles for Se-Se bond activation

被引:16
作者
Lin, Mu [1 ]
Kang, Liqun [1 ]
Gu, Jun [1 ]
Dai, Linxiu [1 ]
Tang, Shengbo [1 ]
Zhang, Tao [1 ]
Wang, Yuhao [1 ]
Li, Lindong [1 ]
Zheng, Xiaoyu [1 ]
Zhu, Wei [1 ]
Si, Rui [2 ]
Fu, Xuefeng [1 ]
Sun, Lingdong [1 ]
Zhang, Yawen [1 ]
Yan, Chunhua [1 ]
机构
[1] Peking Univ, Beijing Natl Lab Mol Sci, Coll Chem & Mol Engn,PKU HKU Joint Lab Rare Earth, State Key Lab Rare Earth Mat Chem & Applicat, Beijing 100871, Peoples R China
[2] Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China
基金
中国博士后科学基金; 中国国家自然科学基金;
关键词
nanoparticle; ruthenium; selenium; heterogeneous catalysis; synergistic effect; ONE-POT SYNTHESIS; COUPLING REACTIONS; OXYGEN REDUCTION; RUTHENIUM CATALYSTS; SELECTIVE REDUCTION; AMBIENT CONDITIONS; DFT CALCULATIONS; IN-SITU; COMPLEXES; NANOCRYSTALS;
D O I
10.1007/s12274-016-1350-0
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The transition from homogeneous to heterogeneous synthetic chemistry enabled by nanocatalysts necessitates investigations of the reaction mechanism and structure-activity relationships for inorganic nanoparticles and organic substrates. Herein, we report that hydrothermally synthesized ruthenium nanoparticles performed differently in the Se-Se bond activation and selenylation of heterocycles, exhibiting a volcano-shaped relationship between catalytic activity and composition. A synergistic effect was observed for Ru-RuO (x) nanocatalysts, with numerous characterizations and density functional theory (DFT) calculations suggesting that a PhSeSePh molecule can initially be adsorbed on the metallic Ru sites and cleaved into two PhSe* species, which subsequently migrate to RuO (x) sites and react with the nucleophile to achieve the selenylation of heterocycles.
引用
收藏
页码:922 / 932
页数:11
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