Boosting the activity of hydrogen release from liquid organic hydrogen carrier systems by sulfur-additives to Pt on alumina catalysts

被引:109
作者
Auer, Franziska [1 ]
Blaumeiser, Dominik [2 ]
Bauer, Tanja [2 ]
Boesmann, Andreas [1 ]
Szesni, Normen [3 ]
Libuda, Joerg [2 ]
Wasserscheid, Peter [1 ,4 ]
机构
[1] Friedrich Alexander Univ Erlangen Nurnberg, Lehrstuhl Chem Reakt Tech, Egerlandstr 3, D-91058 Erlangen, Germany
[2] Friedrich Alexander Univ Erlangen Nurnberg, Lehrstuhl Katalyt Grenzflachenforsch, Egerlandstr 3, D-91058 Erlangen, Germany
[3] Clariant Prod Deutschland GmbH, D-83052 Bruckmuhl, Germany
[4] Forschungszentrum Julich, Helmholtz Inst Erlangen Nurnberg Renewable Energi, Egerlandstr 3, D-91058 Erlangen, Germany
关键词
CO ADSORPTION; PLATINUM; DEHYDROGENATION; METHYLCYCLOHEXANE; SULFURIZATION; STORAGE; SPECTROSCOPY; STABILITY; FTIR;
D O I
10.1039/c9cy00817a
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
Liquid organic hydrogen carrier (LOHC) systems are a promising alternative for energy storage and transport. The development of an active and selective LOHC-dehydrogenation catalyst is therefore of great importance. In this study we present a modification procedure of Pt/Al2O3 catalysts with a sulfur containing compound that results in improved activity as well as in reduced side product formation. Here, it appears that the right amount of applied sulfur species is crucial to reach the described effects. The optimum value depends on the support surface area and the molar ratio of sulfur to surface platinum. Mechanistic studies of the sulfur modification by infrared spectroscopy (DRIFTS) with adsorbed CO revealed that preferentially low coordinated defect sites (edges or corner/apex Pt atoms) are blocked by sulfur compounds and that these are the ones responsible for side reactions. The sulfur species were found to modify the electronic properties of Pt and this facilitates the desorption of the aromatic dehydrogenation products.
引用
收藏
页码:3537 / 3547
页数:11
相关论文
共 42 条
[1]   Influence of Sulfur Poisoning on CO Adsorption on Pd(100) [J].
Alfonso, Dominic R. .
TOPICS IN CATALYSIS, 2012, 55 (5-6) :267-279
[2]   Hydrogen Storage in Liquid Organic Hydride: Producing Hydrogen Catalytically from Methylcyclohexane [J].
Alhumaidan, Faisal ;
Cresswell, David ;
Garforth, Arthur .
ENERGY & FUELS, 2011, 25 (10) :4217-4234
[3]   SULFURIZATION OF PT/AL2O3-CL CATALYSTS .6. SULFUR PLATINUM INTERACTION STUDIED BY INFRARED-SPECTROSCOPY [J].
APESTEGUIA, CR ;
BREMA, CE ;
GARETTO, TF ;
BORGNA, A ;
PARERA, JM .
JOURNAL OF CATALYSIS, 1984, 89 (01) :52-59
[4]   THE ROLE OF CATALYST PRESULFURIZATION IN SOME REACTIONS OF CATALYTIC REFORMING AND HYDROGENOLYSIS [J].
APESTEGUIA, CR ;
BARBIER, J .
JOURNAL OF CATALYSIS, 1982, 78 (02) :352-359
[5]   SULFURIZATION OF PT-AL2O3-C1 CATALYSTS .2. ACCESSIBLE METAL FRACTION [J].
APESTEGUIA, CR ;
BARBIER, J ;
DELOSREYES, JFP ;
GARETTO, TF ;
PARERA, JM .
APPLIED CATALYSIS, 1981, 1 (3-4) :159-163
[6]   FTIR study of CO adsorption on coked Pt-Sn/Al2O3 catalysts [J].
Arteaga, GJ ;
Anderson, JA ;
Rochester, CH .
CATALYSIS LETTERS, 1999, 58 (04) :189-194
[7]  
Barbier J., 1980, SELECTIVE POISONING, P53
[8]  
Barbier J., 1985, Appl. Catal, V19, P375, DOI [10.1016/S0166-9834(00)81759-5, DOI 10.1016/S0166-9834(00)81759-5]
[9]   FT-IR study of CO adsorption on Pt/CeO2:: characterisation and structural rearrangement of small Pt particles [J].
Bazin, P ;
Saur, O ;
Lavalley, JC ;
Daturi, M ;
Blanchard, G .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2005, 7 (01) :187-194
[10]   DEHYDROGENATION AND HYDROGENOLYSIS OF CYCLOHEXANE AND CYCLOHEXENE ON STEPPED (HIGH MILLER INDEX) PLATINUM SURFACES [J].
BLAKELY, DW ;
SOMORJAI, GA .
JOURNAL OF CATALYSIS, 1976, 42 (02) :181-196