Identification of active sites in CO oxidation and water-gas shift over supported Pt catalysts

被引:1079
作者
Ding, Kunlun [1 ]
Gulec, Ahmet [2 ]
Johnson, Alexis M. [1 ]
Schweitzer, Neil M. [3 ]
Stucky, Galen D. [4 ]
Marks, Laurence D. [2 ]
Stair, Peter C. [1 ,5 ]
机构
[1] Northwestern Univ, Dept Chem, Evanston, IL 60208 USA
[2] Northwestern Univ, Dept Mat Sci & Engn, Evanston, IL 60208 USA
[3] Northwestern Univ, Dept Chem & Biol Engn, Evanston, IL 60208 USA
[4] Univ Calif Santa Barbara, Dept Chem & Biochem, Santa Barbara, CA 93106 USA
[5] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA
基金
美国国家科学基金会;
关键词
CARBON-MONOXIDE OXIDATION; INFRARED-SPECTRA; TEMPERATURE; PLATINUM; SINGLE; GOLD; FTIR; ATOM; ADSORPTION; PT/AL2O3;
D O I
10.1126/science.aac6368
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
Identification and characterization of catalytic active sites are the prerequisites for an atomic-level understanding of the catalytic mechanism and rational design of high-performance heterogeneous catalysts. Indirect evidence in recent reports suggests that platinum (Pt) single atoms are exceptionally active catalytic sites. We demonstrate that infrared spectroscopy can be a fast and convenient characterization method with which to directly distinguish and quantify Pt single atoms from nanoparticles. In addition, we directly observe that only Pt nanoparticles show activity for carbon monoxide (CO) oxidation and water-gas shift at low temperatures, whereas Pt single atoms behave as spectators. The lack of catalytic activity of Pt single atoms can be partly attributed to the strong binding of CO molecules.
引用
收藏
页码:189 / 192
页数:4
相关论文
共 36 条
[21]   Metallic Pt as active sites for the water-gas shift reaction on alkali-promoted supported catalysts [J].
Pazmino, Jorge H. ;
Shekhar, Mayank ;
Williams, W. Damion ;
Akatay, M. Cem ;
Miller, Jeffrey T. ;
Delgass, W. Nicholas ;
Ribeiro, Fabio H. .
JOURNAL OF CATALYSIS, 2012, 286 :279-286
[22]   Oxidation of CO in H2-CO mixtures catalyzed by platinum:: alkali effects on rates and selectivity [J].
Pedrero, C ;
Waku, T ;
Iglesia, E .
JOURNAL OF CATALYSIS, 2005, 233 (01) :242-255
[23]   Low-temperature carbon monoxide oxidation catalysed by regenerable atomically dispersed palladium on alumina [J].
Peterson, Eric J. ;
Delariva, Andrew T. ;
Lin, Sen ;
Johnson, Ryan S. ;
Guo, Hua ;
Miller, Jeffrey T. ;
Kwak, Ja Hun ;
Peden, Charles H. F. ;
Kiefer, Boris ;
Allard, Lawrence F. ;
Ribeiro, Fabio H. ;
Datye, Abhaya K. .
NATURE COMMUNICATIONS, 2014, 5
[24]   Low temperature water-gas shift:: Characterization of Pt-based ZrO2 catalyst promoted with Na discovered by combinatorial methods [J].
Pigos, John M. ;
Brooks, Christopher J. ;
Jacobs, Gary ;
Davis, Burtron H. .
APPLIED CATALYSIS A-GENERAL, 2007, 319 :47-57
[25]  
Qiao BT, 2011, NAT CHEM, V3, P634, DOI [10.1038/NCHEM.1095, 10.1038/nchem.1095]
[26]   Water Gas Shift Catalysis [J].
Ratnasamy, Chandra ;
Wagner, Jon P. .
CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 2009, 51 (03) :325-440
[27]   DFT and in situ EXAFS investigation of gold/ceria-zirconia low-temperature water gas shift catalysts: Identification of the nature of the active form of gold [J].
Tibiletti, D ;
Amieiro-Fonseca, A ;
Burch, R ;
Chen, Y ;
Fisher, JM ;
Goguet, A ;
Hardacre, C ;
Hu, P ;
Thompsett, A .
JOURNAL OF PHYSICAL CHEMISTRY B, 2005, 109 (47) :22553-22559
[28]   Promotion effects in the oxidation of CO over zeolite-supported Pt nanoparticles [J].
Visser, T ;
Nijhuis, TA ;
van der Eerden, AMJ ;
Jenken, K ;
Ji, YY ;
Bras, W ;
Nikitenko, S ;
Ikeda, Y ;
Lepage, M ;
Weckhuysen, BM .
JOURNAL OF PHYSICAL CHEMISTRY B, 2005, 109 (09) :3822-3831
[29]   Metal carbonyl cations: generation, characterization and catalytic application [J].
Xu, Q .
COORDINATION CHEMISTRY REVIEWS, 2002, 231 (1-2) :83-108
[30]  
Yang C., 1957, J PHYS CHEM-US, V61, P1504