Understanding the Active Sites of CO Hydrogenation on Pt-Co Catalysts Prepared Using Atomic Layer Deposition

被引:38
作者
Singh, Joseph A. [1 ]
Yang, Nuoya [2 ]
Liu, Xinyan [3 ]
Tsai, Charlie [3 ]
Stone, Kevin H. [4 ]
Johnson, Bart [4 ]
Koh, Ai Leen [5 ]
Bent, Stacey F. [3 ]
机构
[1] Stanford Univ, Dept Chem, 333 Campus Dr, Stanford, CA 94305 USA
[2] Stanford Univ, Dept Mat Sci & Engn, 496 Lomita Mall, Stanford, CA 94305 USA
[3] Stanford Univ, Dept Chem Engn, 443 Via Ortega, Stanford, CA 94305 USA
[4] SLAC Natl Accelerator Lab, SSRL, Menlo Pk, CA 94025 USA
[5] Stanford Univ, Stanford Nano Shared Facil, 476 Lomita Mall, Stanford, CA 94305 USA
基金
美国国家科学基金会;
关键词
FISCHER-TROPSCH SYNTHESIS; TEMPERATURE-PROGRAMMED DESORPTION; CARBON-MONOXIDE; COBALT CATALYSTS; SUPPORTED COBALT; ALCOHOLS SYNTHESIS; HETEROGENEOUS CATALYSTS; STRUCTURE SENSITIVITY; BIMETALLIC CATALYSTS; ADSORPTION BEHAVIOR;
D O I
10.1021/acs.jpcc.7b10541
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 production of liquid fuels and industrial feedstocks from renewable carbon sources is an ongoing scientific challenge. Using atomic layer deposition together with conventional techniques, we synthesize Pt-Co bimetallic catalysts that show improvement for syngas conversion to alcohols. By combining reaction testing, X-ray diffraction, electron microscopy, and in situ infrared spectroscopy experiments, supported by density functional theory calculations, we uncover insights into how Pt modulates the selectivity of Co catalysts. The prepared Pt Co catalysts demonstrate increased selectivity toward methanol and low molecular weight hydrocarbons as well as a modest increase in selectivity toward higher alcohols. The in situ infrared spectroscopic measurements suggest that these changes in selectivity result from an interplay between linear and bridging carbon monoxide configurations on the catalyst surface.
引用
收藏
页码:2184 / 2194
页数:11
相关论文
共 69 条
[1]   An object-oriented scripting interface to a legacy electronic structure code [J].
Bahn, SR ;
Jacobsen, KW .
COMPUTING IN SCIENCE & ENGINEERING, 2002, 4 (03) :56-66
[2]   Carbon monoxide poisoning of proton exchange membrane fuel cells [J].
Baschuk, JJ ;
Li, XG .
INTERNATIONAL JOURNAL OF ENERGY RESEARCH, 2001, 25 (08) :695-713
[3]   MOLECULAR ORBITAL VIEW OF CHEMISORBED CARBON MONOXIDE [J].
BLYHOLDER, G .
JOURNAL OF PHYSICAL CHEMISTRY, 1964, 68 (10) :2772-&
[4]  
Bravo-Suárez JJ, 2013, ACS SYM SER, V1132, P3
[5]   Catalyst synthesis and evaluation using an integrated atomic layer deposition synthesis-catalysis testing tool [J].
Camacho-Bunquin, Jeffrey ;
Shou, Heng ;
Aich, Payoli ;
Beaulieu, David R. ;
Klotzsch, Helmut ;
Bachman, Stephen ;
Marshall, Christopher L. ;
Hock, Adam ;
Stair, Peter .
REVIEW OF SCIENTIFIC INSTRUMENTS, 2015, 86 (08)
[6]   DIRECT SYNTHESIS OF HIGHER ALCOHOLS USING BIMETALLIC COPPER COBALT CATALYSTS [J].
CAO, R ;
PAN, WX ;
GRIFFIN, GL .
LANGMUIR, 1988, 4 (05) :1108-1112
[7]   DRIFTS studies of carbon monoxide coverage on highly dispersed bimetallic Pt-Cu and Pt-An catalysts [J].
Chandler, BD ;
Pignolet, LH .
CATALYSIS TODAY, 2001, 65 (01) :39-50
[8]   Mechanism of Ethanol Synthesis from Syngas on Rh(111) [J].
Choi, YongMan ;
Liu, Ping .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2009, 131 (36) :13054-13061
[9]   High Pressure CO Hydrogenation Over Bimetallic Pt-Co Catalysts [J].
Christensen, Jakob M. ;
Medford, Andrew J. ;
Studt, Felix ;
Jensen, Anker D. .
CATALYSIS LETTERS, 2014, 144 (05) :777-782
[10]   Heats of adsorption of linearly adsorbed CO species on Co2+ and Co sites of reduced Co/Al2O3 catalysts in relationship with the CO/H2 reaction [J].
Couble, Julien ;
Bianchi, Daniel .
APPLIED CATALYSIS A-GENERAL, 2012, 445 :1-13