In Situ Industrial Bimetallic Catalyst Characterization using Scanning Transmission Electron Microscopy and X-ray Absorption Spectroscopy at One Atmosphere and Elevated Temperature

被引:15
作者
Prestat, Eric [1 ]
Kulzick, Matthew A. [2 ]
Dietrich, Paul J. [2 ]
Smith, Matthew [1 ]
Tien, Eu-Pin [1 ]
Burke, M. Grace [1 ]
Haigh, Sarah J. [1 ]
Zaluzec, Nestor J. [1 ,3 ]
机构
[1] Univ Manchester, Sch Mat, Manchester M13 9PL, Lancs, England
[2] BP Res Ctr, Naperville, IL 60563 USA
[3] Argonne Natl Lab, Photon Sci Div, Argonne, IL 60439 USA
基金
英国工程与自然科学研究理事会;
关键词
electron microscopy; energy dispersive X-ray spectroscopy; nanoparticles; supported catalysts; X-ray absorption spectroscopy; PHASE REFORMING CATALYSTS; ENERGY-LOSS SPECTROSCOPY; SUPPORTED CATALYSTS; SELECTIVITY; CO; NANOPARTICLES; CLUSTERS; CELL; MO; PD;
D O I
10.1002/cphc.201700425
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
We have developed a new experimental platform for in situ scanning transmission electron microscope (STEM) energy dispersive X-ray spectroscopy (EDS) which allows real time, nanoscale, elemental and structural changes to be studied at elevated temperature (up to 1000 degrees C) and pressure (up to 1 atm). Here we demonstrate the first application of this approach to understand complex structural changes occurring during reduction of a bimetallic catalyst, PdCu supported on TiO2, synthesized by wet impregnation. We reveal a heterogeneous evolution of nanoparticle size, distribution, and composition with large differences in reduction behavior for the two metals. We show that the data obtained is complementary to in situ STEM electron energy loss spectroscopy (EELS) and when combined with in situ X-ray absorption spectroscopy (XAS) allows correlation of bulk chemical state with nanoscale changes in elemental distribution during reduction, facilitating new understanding of the catalytic behavior for this important class of materials.
引用
收藏
页码:2151 / 2156
页数:6
相关论文
共 30 条
[1]   Heterogeneous Catalyst Deactivation and Regeneration: A Review [J].
Argyle, Morris D. ;
Bartholomew, Calvin H. .
CATALYSTS, 2015, 5 (01) :145-269
[2]   Limits and advantages of x-ray absorption near edge structure for nanometer scale metallic clusters [J].
Bazin, D ;
Rehr, JJ .
JOURNAL OF PHYSICAL CHEMISTRY B, 2003, 107 (45) :12398-12402
[3]   Environmental Transmission Electron Microscopy Study of the Origins of Anomalous Particle Size Distributions in Supported Metal Catalysts [J].
Benavidez, Angelica D. ;
Kovarik, Libor ;
Genc, Arda ;
Agrawal, Nitin ;
Larsson, Elin M. ;
Hansen, Thomas W. ;
Karim, Ayman M. ;
Datye, Abhaya K. .
ACS CATALYSIS, 2012, 2 (11) :2349-2356
[4]   PLATINUM-TIN REFORMING CATALYSTS .2. ACTIVITY AND SELECTIVITY IN HYDROCARBON REACTIONS [J].
BURCH, R ;
GARLA, LC .
JOURNAL OF CATALYSIS, 1981, 71 (02) :360-372
[5]   BIMETALLIC CATALYSTS - APPLICATION IN CATALYTIC REFORMING [J].
CARTER, JL ;
MCVICKER, GB ;
WEISSMAN, W ;
KMAK, WS ;
SINFELT, JH .
APPLIED CATALYSIS, 1982, 3 (04) :327-346
[6]  
Chenna S., 2011, MICROSC MICROANAL S2, V17, P476, DOI [10.1017/S1431927611003254, DOI 10.1017/S14319276]
[7]   Atomic-scale electron microscopy at ambient pressure [J].
Creemer, J. F. ;
Helveg, S. ;
Hoveling, G. H. ;
Ullmann, S. ;
Molenbroek, A. M. ;
Sarro, P. M. ;
Zandbergen, H. W. .
ULTRAMICROSCOPY, 2008, 108 (09) :993-998
[8]   In situ analysis of gas composition by electron energy-loss spectroscopy for environmental transmission electron microscopy [J].
Crozier, Peter A. ;
Chenna, Santhosh .
ULTRAMICROSCOPY, 2011, 111 (03) :177-185
[9]   Nanoscale chemical imaging of a working catalyst by scanning transmission X-ray microscopy [J].
de Smit, Emiel ;
Swart, Ingmar ;
Creemer, J. Fredrik ;
Hoveling, Gerard H. ;
Gilles, Mary K. ;
Tyliszczak, Tolek ;
Kooyman, Patricia J. ;
Zandbergen, Henny W. ;
Morin, Cynthia ;
Weckhuysen, Bert M. ;
de Groot, Frank M. F. .
NATURE, 2008, 456 (7219) :222-U39
[10]   Structural and catalytic differences in the effect of Co and Mo as promoters for Pt-based aqueous phase reforming catalysts [J].
Dietrich, Paul J. ;
Sollberger, Fred G. ;
Akatay, M. Cem ;
Stach, Eric A. ;
Delgass, W. Nicholas ;
Miller, Jeffrey T. ;
Ribeiro, Fabio H. .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2014, 156 :236-248