Strong Metal-Support Interactions for Palladium Supported on TiO2 Catalysts in the Heterogeneous Hydrogenation with Parahydrogen

被引:60
作者
Kovtunov, Kirill V. [1 ,2 ]
Barskiy, Danila A. [1 ,2 ]
Salnikov, Oleg G. [1 ,2 ]
Burueva, Dudari B. [1 ,2 ]
Khudorozhkov, Alexander K. [2 ,3 ]
Bukhtiyarov, Andrey V. [2 ,3 ]
Prosvirin, Igor P. [2 ,3 ]
Gerasimov, Evgeny Y. [2 ]
Bukhtiyarov, Valerii I. [2 ]
Koptyug, Igor V. [1 ,2 ]
机构
[1] SB RAS, Int Tomog Ctr, Lab Magnet Resonance Microimaging, Novosibirsk 630090, Russia
[2] Novosibirsk State Univ, Novosibirsk 630090, Russia
[3] SB RAS, Boreskov Inst Catalysis, Novosibirsk 630090, Russia
基金
俄罗斯基础研究基金会; 俄罗斯科学基金会;
关键词
heterogeneous catalysis; hydrogenation; metal-support interactions; polarization; supported catalysts; INDUCED POLARIZATION; PD CATALYSTS; NANOPARTICLES; SPECTROSCOPY; ALIGNMENT; BEHAVIOR; OXIDES; XPS;
D O I
10.1002/cctc.201500618
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
Parahydrogen-induced polarization (PHIP) was successfully utilized to demonstrate the strong metal-support interaction (SMSI) effect for palladium supported on titania catalysts. Heterogeneous hydrogenation of 1,3-butadiene over Pd/TiO2 catalysts led to the formation of 1- and 2-butenes and butane, and hyperpolarized products were obtained if parahydrogen was used in the reaction. However, if the catalysts were reduced in H-2 flow at 500 degrees C before the hydrogenation reaction, the observed polarization levels were significantly lower or even zero, which was indicative of the suppression of the pairwise addition of hydrogen route. This observation indicated the possibility to detect the SMSI effect by the PHIP technique. Moreover, by using X-ray photoelectron spectroscopy it was shown that Pd is partially present as Pd delta+ after reduction under a hydrogen atmosphere at 500 degrees C. These results were confirmed by transmission electron microscopy, which revealed the formation of Pd delta+ and the dissolution of Pd in the titania lattice.
引用
收藏
页码:2581 / 2584
页数:4
相关论文
共 28 条
  • [1] Furfuraldehyde Hydrogenation on Titanium Oxide-Supported Platinum Nanoparticles Studied by Sum Frequency Generation Vibrational Spectroscopy: Acid-Base Catalysis Explains the Molecular Origin of Strong Metal-Support Interactions
    Baker, L. Robert
    Kennedy, Griffin
    Van Spronsen, Matthijs
    Hervier, Antoine
    Cai, Xiaojun
    Chen, Shiyou
    Wang, Lin-Wang
    Somorjai, Gabor A.
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2012, 134 (34) : 14208 - 14216
  • [2] Para-hydrogen induced polarisation effects in liquid phase hydrogenations catalysed by supported metal nanoparticles
    Balu, Alina M.
    Duckett, Simon B.
    Luque, Rafael
    [J]. DALTON TRANSACTIONS, 2009, (26) : 5074 - 5076
  • [3] PARA-HYDROGEN AND SYNTHESIS ALLOW DRAMATICALLY ENHANCED NUCLEAR ALIGNMENT
    BOWERS, CR
    WEITEKAMP, DP
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1987, 109 (18) : 5541 - 5542
  • [4] XPS, AES and Auger parameter of Pd and PdO
    Brun, M
    Berthet, A
    Bertolini, JC
    [J]. JOURNAL OF ELECTRON SPECTROSCOPY AND RELATED PHENOMENA, 1999, 104 (1-3) : 55 - 60
  • [5] Application of Parahydrogen Induced Polarization Techniques in NMR Spectroscopy and Imaging
    Duckett, Simon B.
    Mewis, Ryan E.
    [J]. ACCOUNTS OF CHEMICAL RESEARCH, 2012, 45 (08) : 1247 - 1257
  • [6] Exchange reactions of hydrogen on metallic catalysts.
    Horiuti, I
    Polanyi, M
    [J]. TRANSACTIONS OF THE FARADAY SOCIETY, 1934, 30 : 1164 - 1172
  • [7] BEHAVIOR OF TI-3+ CENTERS IN THE LOW-TEMPERATURE AND HIGH-TEMPERATURE REDUCTION OF PT-TIO2, STUDIED BY ELECTRON-SPIN-RESONANCE
    HUIZINGA, T
    PRINS, R
    [J]. JOURNAL OF PHYSICAL CHEMISTRY, 1981, 85 (15) : 2156 - 2158
  • [8] Observation of parahydrogen-induced polarization in heterogeneous hydrogenation on supported metal catalysts
    Kovtunov, Kirill V.
    Beck, Irene E.
    Bukhtiyarov, Valery I.
    Koptyug, Igor V.
    [J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2008, 47 (08) : 1492 - 1495
  • [9] Propane-d6 Heterogeneously Hyperpolarized by Parahydrogen
    Kovtunov, Kirill V.
    Truong, Milton L.
    Barskiy, Danila A.
    Salnikov, Oleg G.
    Bukhtiyarov, Valery I.
    Coffey, Aaron M.
    Waddell, Kevin W.
    Koptyug, Igor V.
    Chekmenev, Eduard Y.
    [J]. JOURNAL OF PHYSICAL CHEMISTRY C, 2014, 118 (48) : 28234 - 28243
  • [10] High-Resolution 3D Proton MRI of Hyperpolarized Gas Enabled by Parahydrogen and Rh/TiO2 Heterogeneous Catalyst
    Kovtunov, Kirill V.
    Barskiy, Danila A.
    Coffey, Aaron M.
    Truong, Milton L.
    Salnikov, Oleg G.
    Khudorozhkov, Alexander K.
    Inozemtseva, Elizaveta A.
    Prosvirin, Igor P.
    Bukhtiyarov, Valery I.
    Waddell, Kevin W.
    Chekmenev, Eduard Y.
    Koptyug, Igor V.
    [J]. CHEMISTRY-A EUROPEAN JOURNAL, 2014, 20 (37) : 11636 - 11639