Furan Hydrogenation over Pt(111) and Pt(100) Single-Crystal Surfaces and Pt Nanoparticles from 1 to 7 nm: A Kinetic and Sum Frequency Generation Vibrational Spectroscopy Study

被引:105
作者
Kliewer, Christopher J. [1 ,3 ]
Aliaga, Cesar [1 ,3 ]
Bieri, Marco [1 ,3 ]
Huang, Wenyu [1 ,3 ]
Tsung, Chia-Kuang [1 ,3 ]
Wood, Jennifer B. [1 ,3 ]
Komvopoulos, Kyriakos [2 ]
Somorjai, Gabor A. [1 ,3 ]
机构
[1] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA
[2] Univ Calif Berkeley, Dept Mech Engn, Berkeley, CA 94720 USA
[3] Univ Calif Berkeley, Lawrence Berkeley Lab, Div Mat Sci, Berkeley, CA 94720 USA
基金
瑞士国家科学基金会;
关键词
HIGH-PRESSURE; ULTRAHIGH-VACUUM; PYRROLE HYDROGENATION; STRUCTURE SENSITIVITY; IN-SITU; BENZENE; ADSORPTION; DEHYDROGENATION; ORIENTATION; MOLECULE;
D O I
10.1021/ja105800z
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Sum frequency generation surface vibrational spectroscopy and kinetic measurements using gas chromatography have been used to systematically study the adsorption and hydrogenation of furan over Pt(111) and Pt(100) single-crystal surfaces and size-controlled 1.0-nm, 3.5-nm and 7.0-nm Pt nanoparticles at Torr pressures (10 Torr of furan, 100 Torr of H-2) to form dihydrofuran, tetrahydrofuran, and the ring-cracking products butanol and propylene. As determined by SFG, the furan ring lies parallel to all Pt surfaces studied under hydrogenation conditions. Upright THF and the oxametallacycle intermediate are observed over the nanoparticle catalysts under reaction conditions. Butoxy increases in surface concentration over Pt(111) with increasing temperature in agreement with selectivity trends.
引用
收藏
页码:13088 / 13095
页数:8
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