Pd-LaFeO3 Catalysts in Aqueous Ethanol: Pd Reduction, Leaching, and Structural Transformations in the Presence of a Base

被引:6
作者
Checchia, Stefano [4 ,5 ]
Mulligan, Christopher J. [1 ]
Emerich, Hermann [6 ]
Alxneit, Ivo [2 ]
Krumeich, Frank [3 ]
Di Michiel, Marco [4 ]
Thompson, Paul B. J. [7 ]
Hii, King Kuok Mimi [1 ]
Ferri, Davide [2 ]
Newton, Mark A. [3 ]
机构
[1] Imperial Coll London, Dept Chem, London W12 0BZ, England
[2] Paul Scherrer Inst, CH-5232 Villigen, Switzerland
[3] Swiss Fed Inst Technol, Dept Chem & Appl Biosci, CH-8093 Zurich, Switzerland
[4] ESRF European Synchrotron, ID15A, F-38000 Grenoble, France
[5] Lund Univ, Max IV Lab, SE-22100 Lund, Sweden
[6] ESRF European Synchrotron, Swiss Norwegian Beamlines SNBL, F-38000 Grenoble, France
[7] ESRF European Synchrotron, XMaS UK CRG Beamline, F-38000 Grenoble, France
基金
英国工程与自然科学研究理事会;
关键词
palladium catalysis; leaching; Suzuki coupling; basic condition; X-ray absorption spectroscopy; X-ray diffraction; pair distribution function; X-RAY-DIFFRACTION; OXYGEN REDUCTION; SUPPORTED PD; PALLADIUM CATALYSTS; FOURIER-ANALYSIS; PEROVSKITE; FLOW; TRANSITION; CHEMISTRY; SIZE;
D O I
10.1021/acscatal.9b04869
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 reactive behavior of three catalysts based on Pd-loaded LaFeO3 was investigated in terms of the reducibility of Pd and its propensity to leaching into the liquid phase in flowing solutions prototypical of C-C coupling catalysis in a continuous flow reactor cell. In situ quick extended X-ray absorption fine structure spectroscopy showed that Pd remains stable and nonreducible in the flowing ethanol/water solvent mixture under heating to 353 K. However, ex situ transmission electron microscopy, high-energy X-ray diffraction, and fluorescence yield Fe K-edge X-ray absorption near-edge structure show that the addition of a significant amount of base (K2CO3, 0.1 M) results in the structural degradation of the perovskite support as well as the mobilization of Pd along the sample bed that is dependent on the structure and crystallite size of the perovskite. The results are discussed in terms of the use of perovskite-type oxides in various areas of research where they are placed in contact with liquid phases of variable temperature and elevated pH.
引用
收藏
页码:3933 / 3944
页数:12
相关论文
共 68 条
[1]   A Novel and Efficient Continuous-Flow Route To Prepare Trifluoromethylated N-Fused Heterocycles for Drug Discovery and Pharmaceutical Manufacturing [J].
Amini-Rentsch, Lara ;
Vanoli, Ennio ;
Richard-Bildstein, Sylvia ;
Marti, Roger ;
Vile, Gianvito .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2019, 58 (24) :10164-10171
[2]   Heterogeneous or homogeneous? A case study involving palladium-containing perovskites in the Suzuki reaction [J].
Andrews, SP ;
Stepan, AF ;
Tanaka, H ;
Ley, SV ;
Smith, MD .
ADVANCED SYNTHESIS & CATALYSIS, 2005, 347 (05) :647-654
[3]   The fast azimuthal integration Python']Python library: pyFAI [J].
Ashiotis, Giannis ;
Deschildre, Aurore ;
Nawaz, Zubair ;
Wright, Jonathan P. ;
Karkoulis, Dimitrios ;
Picca, Frederic Emmanuel ;
Kieffer, Jerome .
JOURNAL OF APPLIED CRYSTALLOGRAPHY, 2015, 48 :510-519
[4]   VOIGT-FUNCTION MODELING IN FOURIER-ANALYSIS OF SIZE-BROADENED AND STRAIN-BROADENED X-RAY-DIFFRACTION PEAKS [J].
BALZAR, D ;
LEDBETTER, H .
JOURNAL OF APPLIED CRYSTALLOGRAPHY, 1993, 26 (pt 1) :97-103
[5]   Size-strain line-broadening analysis of the ceria round-robin sample [J].
Balzar, D ;
Audebrand, N ;
Daymond, MR ;
Fitch, A ;
Hewat, A ;
Langford, JI ;
Le Bail, A ;
Louër, D ;
Masson, O ;
McCowan, CN ;
Popa, NC ;
Stephens, PW ;
Toby, BH .
JOURNAL OF APPLIED CRYSTALLOGRAPHY, 2004, 37 :911-924
[6]   PROFILE FITTING OF X-RAY-DIFFRACTION LINES AND FOURIER-ANALYSIS OF BROADENING [J].
BALZAR, D .
JOURNAL OF APPLIED CRYSTALLOGRAPHY, 1992, 25 :559-570
[7]   MEAN COORDINATION NUMBERS AND THE NONMETAL METAL TRANSITION IN CLUSTERS [J].
BENFIELD, RE .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1992, 88 (08) :1107-1110
[8]  
Binsted N, 1988, PAXAS PROGRAMME ANAL
[9]  
Binsted N., 1998, EXCURV98, CCLRC Daresbury Laboratory computer program
[10]   Supported palladium catalysts for fine chemicals synthesis [J].
Blaser, HU ;
Indolese, A ;
Schnyder, A ;
Steiner, H ;
Studer, M .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2001, 173 (1-2) :3-18