Nanodisperse gold catalysts in oxidation of benzyl alcohol: comparison of various supports under different conditions
文献类型：期刊论文
| 作者 | Nagy, Gergely2; Beck, Andrea2; Safran, Gyorgy3; Schay, Zoltan2; Liu, Shaofeng4,5; Li, Tianbo4; Qiao, Botao4; Wang, Junhu4,5; Lazar, Karoly1 |
| 刊名 | REACTION KINETICS MECHANISMS AND CATALYSIS
 |
| 出版日期 | 2019-10-01 |
| 卷号 | 128期号:1页码:71-95 |
| ISSN号 | 1878-5190 |
| 关键词 | Benzyl alcohol oxidation Supported gold catalysts Distinction of active sites Acid base support effects Binary concentration pulse chromatograohy |
| DOI | 10.1007/s11144-019-01615-8 |
| 通讯作者 | Lazar, Karoly(lazar.karoly@energia.mta.hu) |
| 英文摘要 | Monodisperse 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. |
| WOS关键词 | SOLVENT-FREE OXIDATION ; AEROBIC OXIDATION ; SELECTIVE OXIDATION ; MOLECULAR-OXYGEN ; ADSORPTION-ISOTHERMS ; AU ; AU/AL2O3 ; SIZE ; CO ; NANOCOMPOSITE |
| 资助项目 | MTA Wigner Research Centre for Physics (MTA Wigner FK, MTA EK) ; Hungarian-Chinese bilateral cooperation[TET_15-1-2016-0120] |
| WOS研究方向 | Chemistry |
| 语种 | 英语 |
| 出版者 | SPRINGER |
| WOS记录号 | WOS:000486027900005 |
| 资助机构 | 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 ; 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 |
| 源URL | [http://cas-ir.dicp.ac.cn/handle/321008/172823]  |
| 专题 | 大连化学物理研究所_中国科学院大连化学物理研究所 |
| 通讯作者 | Lazar, Karoly |
| 作者单位 | 1.HAS, Energy Res Ctr, Dept Nucl Anal & Radiog, Konkoly Thege M Ut 29-33, H-1121 Budapest, Hungary 2.HAS, Energy Res Ctr, Dept Surface Chem & Catalysis, Konkoly Thege M Ut 29-33, H-1121 Budapest, Hungary 3.HAS, Energy Res Ctr, Inst Mat Sci, Lab Thin Layer Phys, Konkoly Thege M Ut 29-33, H-1121 Budapest, Hungary 4.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, 457 Zhongshan Rd, Dalian 116023, Peoples R China 5.Chinese Acad Sci, Dalian Inst Chem Phys, Mossbauer Effect Data Ctr, 457 Zhongshan Rd, Dalian 116023, Peoples R China |
| 推荐引用方式 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. |
入库方式： OAI收割
来源：大连化学物理研究所
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