Alumina Supported Au-Ni: Surface Synergism in the Gas Phase Hydrogenation of Nitro-Compounds

被引:31
作者
Cardenas-Lizana, Fernando [1 ,3 ]
Gomez-Quero, Santiago [1 ]
Jacobs, Gary [2 ]
Ji, Yaying [2 ]
Davis, Burtron H. [2 ]
Kiwi-Minsker, Lioubov [3 ]
Keane, Mark A. [1 ]
机构
[1] Heriot Watt Univ, Sch Engn & Phys Sci, Edinburgh EH14 4AS, Midlothian, Scotland
[2] Ctr Appl Energy Res, Lexington, KY 40511 USA
[3] Ecole Polytech Fed Lausanne, Grp Catalyt React Engn, CH-1015 Lausanne, Switzerland
基金
英国工程与自然科学研究理事会; 瑞士国家科学基金会;
关键词
M-DINITROBENZENE; SELECTIVE HYDROGENATION; NITROBENZENE HYDROGENATION; CO OXIDATION; CATALYTIC-HYDROGENATION; BIMETALLIC CATALYSTS; NI/AL2O3; CATALYSTS; NITRO-COMPOUNDS; METAL-CLUSTERS; GOLD CATALYSTS;
D O I
10.1021/jp3025528
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 catalytic gas phase hydrogenation of 1,3-dinitrobenzene over Au/Al2O3 delivered exclusive reduction of a single -NO2 substituent to generate 1,3-nitroaniline (E-a = 131 kJ mol(-1)), reaction over Ni/Al2O3 resulted in full hydrogenation to 1,3-phenylenediamine (E-a = 38 kJ mo1(-1)), whereas both products were isolated over Au-Ni/Al2O3. In the hydrogenation of 1,3,5-trinitrobenzene, Au/Al2O3 promoted preferential partial hydrogenation (3,5-dinitroaniline), Ni/Al2O3 generated 1,3,5-triaminobenzene as the predominant product, while Au-Ni/Al2O3 exhibited an intermediate catalytic response. The catalysts have been characterized in terms of temperature programmed reduction (TPR), H-2 chemisorption, powder XRD, high-resolution TEM, XPS, and XANES/EXAFS measurements. Post-TPR, there was evidence of a metal particle redispersion resulting from the introduction of Au to Ni/Al2O3 where HRTEM-EDX mapping has established close proximity of Au and Ni on Au-Ni/Al2O3 with electron transfer from Ni to Au (from XPS analysis). Hydrogen chemisorption on Au-Ni/Al2O3 was 3 times lower than that recorded for Ni/Al2O3, suggesting Au-Ni interaction that inhibits H-2 uptake. Simulation of the XANES/EXAFS response provided a better fit when incorporating Au-Ni interaction. The results demonstrate control of selectivity in poly nitroarene hydrogenation through the use of mono- (Au and Ni) and bi- (Au-Ni) metallic catalysts, where catalytic response is governed by surface composition.
引用
收藏
页码:11166 / 11180
页数:15
相关论文
共 94 条
[1]   Local, global and electronic structure of supported gold nanoclusters determined by EXAFS, XRD and XPS methods [J].
Aldea, Nicolae ;
Rednic, Vasile ;
Pintea, Stelian ;
Marginean, Petru ;
Barz, Bogdan ;
Gluhoi, Andreea ;
Nieuwenhuys, Bernard E. ;
Neumann, Manfred ;
Xie Yaning ;
Matei, Florica .
SUPERLATTICES AND MICROSTRUCTURES, 2009, 46 (1-2) :141-148
[2]  
[Anonymous], ULLMANNS ENCY IND CH
[3]   Characterization of Catalysts in Reactive Atmospheres by X-ray Absorption Spectroscopy [J].
Bare, Simon R. ;
Ressler, Thorsten .
ADVANCES IN CATALYSIS, VOL 52, 2009, 52 :339-465
[4]   Characterization of Pd-Au/SiO2 catalysts by X-ray diffraction, temperature-programmed hydride decomposition, and catalytic probes [J].
Bonarowska, M ;
Pielaszek, J ;
Juszczyk, W ;
Karpinski, Z .
JOURNAL OF CATALYSIS, 2000, 195 (02) :304-315
[5]  
Bond G.C., 2006, CATALYSIS GOLD, DOI 10.1007/bf03215560
[6]   Hydrogen chemisorption on Al2O3-supported gold catalysts [J].
Bus, E ;
Miller, JT ;
van Bokhoven, JA .
JOURNAL OF PHYSICAL CHEMISTRY B, 2005, 109 (30) :14581-14587
[7]   Investigation of alumina-supported an catalyst for CO oxidation by isotopic transient analysis and X-ray absorption spectroscopy [J].
Calla, JT ;
Davis, RJ .
JOURNAL OF PHYSICAL CHEMISTRY B, 2005, 109 (06) :2307-2314
[8]   Liquid phase hydrogenation of crotonaldehyde over Au/CeO2 catalysts [J].
Campo, Betiana ;
Santori, Gerardo ;
Petit, Corinne ;
Volpe, Maria .
APPLIED CATALYSIS A-GENERAL, 2009, 359 (1-2) :79-83
[9]   XPS calibration study of thin-film nickel silicides [J].
Cao, Yu ;
Nyborg, Lars ;
Jelvestam, Urban .
SURFACE AND INTERFACE ANALYSIS, 2009, 41 (06) :471-483
[10]   Exclusive production of chloroaniline from chloronitrobenzene over Au/TiO2 and Au/Al2O3 [J].
Cardenas-Lizana, Fernando ;
Gomez-Quero, Santiago ;
Keane, Mark A. .
CHEMSUSCHEM, 2008, 1 (03) :215-221