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Nanodisperse gold catalysts in oxidation of benzyl alcohol: comparison of various supports under different conditions
Nagy, Gergely1; Beck, Andrea1; Safran, Gyorgy2; Schay, Zoltan1; Liu, Shaofeng3,4; Li, Tianbo3; Qiao, Botao3; Wang, Junhu3,4; Lazar, Karoly5
Corresponding AuthorLazar, Karoly(lazar.karoly@energia.mta.hu)
KeywordBenzyl alcohol oxidation Supported gold catalysts Distinction of active sites Acid base support effects Binary concentration pulse chromatograohy
Source PublicationREACTION KINETICS MECHANISMS AND CATALYSIS
2019-10-01
ISSN1878-5190
DOI10.1007/s11144-019-01615-8
Volume128Issue:1Pages:71-95
Funding ProjectMTA Wigner Research Centre for Physics (MTA Wigner FK, MTA EK) ; Hungarian-Chinese bilateral cooperation[TET_15-1-2016-0120]
Funding OrganizationMTA Wigner Research Centre for Physics (MTA Wigner FK, MTA EK) ; MTA Wigner Research Centre for Physics (MTA Wigner FK, MTA EK) ; Hungarian-Chinese bilateral cooperation ; Hungarian-Chinese bilateral cooperation ; MTA Wigner Research Centre for Physics (MTA Wigner FK, MTA EK) ; MTA Wigner Research Centre for Physics (MTA Wigner FK, MTA EK) ; Hungarian-Chinese bilateral cooperation ; Hungarian-Chinese bilateral cooperation ; MTA Wigner Research Centre for Physics (MTA Wigner FK, MTA EK) ; MTA Wigner Research Centre for Physics (MTA Wigner FK, MTA EK) ; Hungarian-Chinese bilateral cooperation ; Hungarian-Chinese bilateral cooperation ; MTA Wigner Research Centre for Physics (MTA Wigner FK, MTA EK) ; MTA Wigner Research Centre for Physics (MTA Wigner FK, MTA EK) ; Hungarian-Chinese bilateral cooperation ; Hungarian-Chinese bilateral cooperation
WOS SubjectChemistry, Physical
WOS Research AreaChemistry
WOS KeywordSOLVENT-FREE OXIDATION ; AEROBIC OXIDATION ; SELECTIVE OXIDATION ; MOLECULAR-OXYGEN ; ADSORPTION-ISOTHERMS ; AU ; AU/AL2O3 ; SIZE ; CO ; NANOCOMPOSITE
AbstractMonodisperse gold particles (ca. 2 nm) were prepared and deposited on various supports (SiO2, Al2O3, HAP, MgAl2O4 and MgO). The acid/base properties of supports were characterized by NH3 and CO2 sorption. The size of the gold nanoparticles spans in the 1.7-6.5 nm mean diameter range after calcination as determined from TEM measurements. The amounts of accessible surface sites were estimated by binary concentration pulse chromatography of CO with Kr adsorption. The data are in agreement with the results of CO adsorption obtained by DRIFT spectroscopy. The activities of the catalysts were compared in the oxidation of benzyl alcohol in stirred batch reactors under two different conditions: in xylene solvent with atmospheric oxygen at 60 degrees C (in presence and in absence of K2CO3), and in a solvent-free mixture at elevated pressure and temperature (5 bar O-2, 150 degrees C, 5 h). The activities of catalysts in benzyl alcohol conversion are described in two variants, namely related to (i) active catalytic sites (ASNA), and (ii) number of Au atoms on the geometric surface of particles (GSNA). The activities of catalysts in xylene solvent at 60 degrees C were excellent, with 0.28-1.11 s(-1) characteristic GSNA(ini) values (initial reaction rates related to surface Au atoms, Au-surf) in presence of K2CO3. The observed order of activities under these conditions is Au/SiO2 < Au/Al2O3 < Au/HAP < Au/MgAl2O4 < Au/MgO. In the experiments performed at 150 degrees C under solvent-free conditions, the reaction partners are depleted in greater extents (with the exception of Au/Al2O3), thus the obtained average GSNA(ave) (average reaction rate during 5 h reaction related to Au-surf) values are less reliable, however selectivity data provide useful information as well. These estimated average GSNA(ave) values (0.14-0.83 s(-1)) attest still good activities. For the interpretation of the obtained data, the roles of active sites on gold nanoparticles of various dispersion and the accessibility of their surfaces as well as the acid-base properties and surface hydroxyl concentration of supports, water ad- and desorption phenomena are considered simultaneously.
Language英语
Funding OrganizationMTA Wigner Research Centre for Physics (MTA Wigner FK, MTA EK) ; MTA Wigner Research Centre for Physics (MTA Wigner FK, MTA EK) ; Hungarian-Chinese bilateral cooperation ; Hungarian-Chinese bilateral cooperation ; MTA Wigner Research Centre for Physics (MTA Wigner FK, MTA EK) ; MTA Wigner Research Centre for Physics (MTA Wigner FK, MTA EK) ; Hungarian-Chinese bilateral cooperation ; Hungarian-Chinese bilateral cooperation ; MTA Wigner Research Centre for Physics (MTA Wigner FK, MTA EK) ; MTA Wigner Research Centre for Physics (MTA Wigner FK, MTA EK) ; Hungarian-Chinese bilateral cooperation ; Hungarian-Chinese bilateral cooperation ; MTA Wigner Research Centre for Physics (MTA Wigner FK, MTA EK) ; MTA Wigner Research Centre for Physics (MTA Wigner FK, MTA EK) ; Hungarian-Chinese bilateral cooperation ; Hungarian-Chinese bilateral cooperation
WOS IDWOS:000486027900005
PublisherSPRINGER
Citation statistics
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/172824
Collection中国科学院大连化学物理研究所
Corresponding AuthorLazar, Karoly
Affiliation1.HAS, Energy Res Ctr, Dept Surface Chem & Catalysis, Konkoly Thege M Ut 29-33, H-1121 Budapest, Hungary
2.HAS, Energy Res Ctr, Inst Mat Sci, Lab Thin Layer Phys, Konkoly Thege M Ut 29-33, H-1121 Budapest, Hungary
3.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, 457 Zhongshan Rd, Dalian 116023, Peoples R China
4.Chinese Acad Sci, Dalian Inst Chem Phys, Mossbauer Effect Data Ctr, 457 Zhongshan Rd, Dalian 116023, Peoples R China
5.HAS, Energy Res Ctr, Dept Nucl Anal & Radiog, Konkoly Thege M Ut 29-33, H-1121 Budapest, Hungary
Recommended Citation
GB/T 7714
Nagy, Gergely,Beck, Andrea,Safran, Gyorgy,et al. Nanodisperse gold catalysts in oxidation of benzyl alcohol: comparison of various supports under different conditions[J]. REACTION KINETICS MECHANISMS AND CATALYSIS,2019,128(1):71-95.
APA Nagy, Gergely.,Beck, Andrea.,Safran, Gyorgy.,Schay, Zoltan.,Liu, Shaofeng.,...&Lazar, Karoly.(2019).Nanodisperse gold catalysts in oxidation of benzyl alcohol: comparison of various supports under different conditions.REACTION KINETICS MECHANISMS AND CATALYSIS,128(1),71-95.
MLA Nagy, Gergely,et al."Nanodisperse gold catalysts in oxidation of benzyl alcohol: comparison of various supports under different conditions".REACTION KINETICS MECHANISMS AND CATALYSIS 128.1(2019):71-95.
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