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Hydrogenolysis of methyl heptanoate over Co based catalysts: Mediation of support property on activity and product distribution
Liu, Qiying1; Bie, Yuwei2; Qiu, Songbai1; Zhang, Qi1; Sainio, Jani3; Wang, Tiejun1; Ma, Longlong1; Lehtonen, Juha2
2014-04-05
发表期刊APPLIED CATALYSIS B-ENVIRONMENTAL
卷号147页码:236-245
摘要Co/MgO, Co/SiO2 and Co/H beta catalysts were prepared by incipient wetness impregnation. The formation of MgO-CoO solid solution and MgCo2O4 spinel in Co/MgO resulted in high dispersions of Co on MgO even at the low calcined temperatures and the high Co loadings. The second impregnation of Co on Co/MgO enhanced Co cations in surface/subsurface of catalysts, which led to the enlarged metallic Co particle sizes by H-2 reduction. Comparatively, the highly dispersion of Co was only observed on SiO2 and H beta at the low Co loadings owing to the Co delta+ species of strong interactions with these supports. The solid solution/spinel and the strongly interacted Co delta+ species induced the Co cations reduced at higher temperatures with obtaining the small Co particle sizes. These cases also significantly decreased the basicities of Co/MgO depending on calcined temperature and Co loadings, and increased the acidic sites of Co/SiO2 and Co/H beta with obtaining enhanced acidities, respectively. During hydrogenolysis processing, the basic sites of Co/MgO triggers the splitting of acyl C-O bond of methyl heptanoate to form heptanal and methanol, followed by further hydrogenation of heptanal to 1-heptanol. While the acidic Co/SiO2 and Co/H beta induce the cracking of ether C-O bond to heptanoic acid and CH4. Heptanoic acid intermediate is then converted into C-6 and C-7 alkanes by the parallel decarbonylation and HDO pathways, respectively. The activity and product distribution could be facilely mediated by the synergistic catalysis of metal and acid/base. Under optimal conditions, the maximal 1-heptanol and summed C-6/C-7 alkanes yields of 55% and 89% were observed over Co/MgO and Co/SiO2 with desire Co loadings, respectively, indicating the promising applications of these catalysts in hydrogenolysis of vegetable oils. (C) 2013 Elsevier B.V. All rights reserved.
文章类型Article
关键词Methyl Heptanoate Hydrogenolysis Co Catalyst Support Property Product Distribution
WOS标题词Science & Technology ; Physical Sciences ; Technology
DOI10.1016/j.apcatb.2013.08.045
研究领域[WOS]Chemistry ; Engineering
关键词[WOS]FISCHER-TROPSCH SYNTHESIS ; VEGETABLE-OILS ; ETHYL-ACETATE ; FATTY-ACIDS ; ESTER HYDROGENOLYSIS ; COBALT CATALYSTS ; MODEL-COMPOUND ; TIN CATALYSTS ; ACETIC-ACID ; HYDROGENATION
收录类别SCI
语种英语
WOS类目Chemistry, Physical ; Engineering, Environmental ; Engineering, Chemical
WOS记录号WOS:000330489400027
引用统计
被引频次:21[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://ir.giec.ac.cn/handle/344007/10710
专题中国科学院广州能源研究所
作者单位1.Chinese Acad Sci, Guangzhou Inst Energy Convers, CAS Key Lab Renewable Energy, Guangzhou 510640, Guangdong, Peoples R China
2.Aalto Univ, Dept Biotechnol & Chem Technol, Aalto 00076, Finland
3.Aalto Univ, Dept Appl Phys, Aalto 00076, Finland
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Liu, Qiying,Bie, Yuwei,Qiu, Songbai,et al. Hydrogenolysis of methyl heptanoate over Co based catalysts: Mediation of support property on activity and product distribution[J]. APPLIED CATALYSIS B-ENVIRONMENTAL,2014,147:236-245.
APA Liu, Qiying.,Bie, Yuwei.,Qiu, Songbai.,Zhang, Qi.,Sainio, Jani.,...&Lehtonen, Juha.(2014).Hydrogenolysis of methyl heptanoate over Co based catalysts: Mediation of support property on activity and product distribution.APPLIED CATALYSIS B-ENVIRONMENTAL,147,236-245.
MLA Liu, Qiying,et al."Hydrogenolysis of methyl heptanoate over Co based catalysts: Mediation of support property on activity and product distribution".APPLIED CATALYSIS B-ENVIRONMENTAL 147(2014):236-245.
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