Catalysis on singly dispersed bimetallic sites

被引:276
作者
Zhang, Shiran [1 ,2 ]
Nguyen, Luan [1 ,2 ]
Liang, Jin-Xia [3 ,4 ,5 ]
Shan, Junjun [1 ,2 ]
Liu, Jingyue [6 ]
Frenkel, Anatoly I. [7 ]
Patlolla, Anitha [7 ]
Huang, Weixin [1 ,2 ]
Li, Jun [3 ,4 ]
Tao, Franklin [1 ,2 ]
机构
[1] Univ Kansas, Dept Chem & Petr Engn, Lawrence, KS 66047 USA
[2] Univ Kansas, Dept Chem, Lawrence, KS 66047 USA
[3] Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
[4] Tsinghua Univ, Key Lab Organ Optoelect & Mol Engn, Minist Educ, Beijing 100084, Peoples R China
[5] Guizhou Normal Coll, Guizhou Prov Key Lab Computat Nano Mat Sci, Guiyang 550018, Peoples R China
[6] Arizona State Univ, Dept Phys, Tempe, AZ 85287 USA
[7] Yeshiva Univ, Dept Phys, New York, NY 10016 USA
基金
美国国家科学基金会;
关键词
SURFACE-CHEMISTRY; IN-SITU; NO; CO; REDUCTION; OXIDATION; METHANE; OXIDE; NANOPARTICLES; PERFORMANCE;
D O I
10.1038/ncomms8938
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
A catalytic site typically consists of one or more atoms of a catalyst surface that arrange into a configuration offering a specific electronic structure for adsorbing or dissociating reactant molecules. The catalytic activity of adjacent bimetallic sites of metallic nanoparticles has been studied previously. An isolated bimetallic site supported on a non-metallic surface could exhibit a distinctly different catalytic performance owing to the cationic state of the singly dispersed bimetallic site and the minimized choices of binding configurations of a reactant molecule compared with continuously packed bimetallic sites. Here we report that isolated Rh1Co3 bimetallic sites exhibit a distinctly different catalytic performance in reduction of nitric oxide with carbon monoxide at low temperature, resulting from strong adsorption of two nitric oxide molecules and a nitrous oxide intermediate on Rh1Co3 sites and following a low-barrier pathway dissociation to dinitrogen and an oxygen atom. This observation suggests a method to develop catalysts with high selectivity.
引用
收藏
页数:10
相关论文
共 40 条
[1]   Electronic structure and bonding properties of cobalt oxide in the spinel structure [J].
Chen, Jia ;
Wu, Xifan ;
Selloni, Annabella .
PHYSICAL REVIEW B, 2011, 83 (24)
[2]   The promotional effect of gold in catalysis by palladium-gold [J].
Chen, MS ;
Kumar, D ;
Yi, CW ;
Goodman, DW .
SCIENCE, 2005, 310 (5746) :291-293
[3]   INTERPRETATION OF X-RAY PHOTOEMISSION SPECTRA OF COBALT OXIDES AND COBALT OXIDE SURFACES [J].
CHUANG, TJ ;
BRUNDLE, CR ;
RICE, DW .
SURFACE SCIENCE, 1976, 59 (02) :413-429
[4]  
Ertl G., 2008, Handbook of Heterogeneous Catalysis, V1, DOI DOI 10.1002/9783527619474.FMATTER
[5]   A view from the inside: Complexity in the atomic scale ordering of supported metal nanoparticles [J].
Frenkel, AI ;
Hills, CW ;
Nuzzo, RG .
JOURNAL OF PHYSICAL CHEMISTRY B, 2001, 105 (51) :12689-12703
[6]   Solving the 3D structure of metal nanoparticles [J].
Frenkel, Anatoly .
ZEITSCHRIFT FUR KRISTALLOGRAPHIE, 2007, 222 (11) :605-611
[7]   Applications of extended X-ray absorption fine-structure spectroscopy to studies of bimetallic nanoparticle catalysts [J].
Frenkel, Anatoly I. .
CHEMICAL SOCIETY REVIEWS, 2012, 41 (24) :8163-8178
[8]   Modeling the Structure and Composition of Nanoparticles by Extended X-Ray Absorption Fine-Structure Spectroscopy [J].
Frenkel, Anatoly I. ;
Yevick, Aaron ;
Cooper, Chana ;
Vasic, Relja .
ANNUAL REVIEW OF ANALYTICAL CHEMISTRY, VOL 4, 2011, 4 :23-39
[9]   CO/NO and CO/NO/O2 reactions over a Au-Pd single crystal catalyst [J].
Gao, Feng ;
Wang, Yilin ;
Goodman, D. Wayne .
JOURNAL OF CATALYSIS, 2009, 268 (01) :115-121
[10]   Direct, Nonoxidative Conversion of Methane to Ethylene, Aromatics, and Hydrogen [J].
Guo, Xiaoguang ;
Fang, Guangzong ;
Li, Gang ;
Ma, Hao ;
Fan, Hongjun ;
Yu, Liang ;
Ma, Chao ;
Wu, Xing ;
Deng, Dehui ;
Wei, Mingming ;
Tan, Dali ;
Si, Rui ;
Zhang, Shuo ;
Li, Jianqi ;
Sun, Litao ;
Tang, Zichao ;
Pan, Xiulian ;
Bao, Xinhe .
SCIENCE, 2014, 344 (6184) :616-619