Selective hydrogenolysis of glycerol to propylene glycol on hydroxycarbonate-derived Cu-ZnO-Al2O3 catalysts
文献类型:期刊论文
作者 | Wang, Shuai; Liu, Haichao |
刊名 | CHINESE JOURNAL OF CATALYSIS
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出版日期 | 2014-05-01 |
卷号 | 35期号:5页码:631-643 |
关键词 | Glycerol Selective Hydrogenolysis Propylene Glycol Copper Zinc Oxide Alumina Hydroxycarbonate Precursor Structure-activity Relationship Stability |
ISSN号 | 0253-9837 |
DOI | 10.1016/S1872-2067(14)60094-2 |
英文摘要 | Three Cu-ZnO-Al2O3 catalysts with similar compositions were prepared by homogeneous coprecipitation (CZA-HP), deposition-precipitation (CZA-DP), and conventional coprecipitation (CZA-CP). A Cu-ZnO catalyst was also prepared by homogeneous coprecipitation (CZ-HP) for reference. X-ray diffraction results showed that the degree of mixing of Cu2+, Zn2+, and Al3+ ions in the Cu-Zn-Al hydroxycarbonate precursor followed the order of CZA-DP < CZA-HP < CZA-CP. A more homogeneous aluminum distribution and intimate contact between Al2O3 and ZnO led to smaller CuO and ZnO crystallites in the CuO-ZnO-Al2O3 composite oxides, and consequently smaller Cu and ZnO crystallites in the final Cu-ZnO-Al2O3 catalysts. However, the intimate ZnO-Al2O3 contact hindered the interaction between Cu and ZnO in the Cu-ZnO-Al2O3 catalysts. As a result of these effects of Al2O3, for the samples other than CZA-CP, the Cu particles on CZA-HP showed the highest redox activity, which was characterized by N2O chemisorption-H-2 temperature-programmed reduction. These catalysts catalyzed glycerol hydrogenolysis to propylene glycol with high selectivities above 90% at 30% glycerol conversion (473 K and 6.0 MPa H-2). Their activities normalized per exposed surface Cu atom to give turnover frequencies increased in the order CZA-DP < CZA-CP < CZ-HP < CZA-HP, which was the order of the redox ability of the Cu particles. The addition of alumina increased the stability of Cu-ZnO catalysts. After six cycles (6 h per run), the activity of CZ-HP decreased by 45% accompanied by an increase of Cu crystallite size from 13.2 to 45.2 nm, while that of CZA-HP decreased only by 10% with an increase of the Cu crystallite size from 8.3 to 19.0 nm. These results demonstrated the promoting effects of Al2O3 on the activity and stability of Cu-ZnO catalysts derived from the hydroxycarbonates. (C) 2014, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved. |
语种 | 英语 |
WOS记录号 | WOS:000335622300005 |
出版者 | SCIENCE PRESS |
源URL | [http://ir.iccas.ac.cn/handle/121111/52625] ![]() |
专题 | 中国科学院化学研究所 |
通讯作者 | Liu, Haichao |
作者单位 | Peking Univ, Coll Chem & Mol Engn, Beijing Natl Lab Mol Sci, State Key Lab Struct Chem Unstable & Stable Speci, Beijing 100871, Peoples R China |
推荐引用方式 GB/T 7714 | Wang, Shuai,Liu, Haichao. Selective hydrogenolysis of glycerol to propylene glycol on hydroxycarbonate-derived Cu-ZnO-Al2O3 catalysts[J]. CHINESE JOURNAL OF CATALYSIS,2014,35(5):631-643. |
APA | Wang, Shuai,&Liu, Haichao.(2014).Selective hydrogenolysis of glycerol to propylene glycol on hydroxycarbonate-derived Cu-ZnO-Al2O3 catalysts.CHINESE JOURNAL OF CATALYSIS,35(5),631-643. |
MLA | Wang, Shuai,et al."Selective hydrogenolysis of glycerol to propylene glycol on hydroxycarbonate-derived Cu-ZnO-Al2O3 catalysts".CHINESE JOURNAL OF CATALYSIS 35.5(2014):631-643. |
入库方式: OAI收割
来源:化学研究所
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