Re/AC catalysts for selective hydrogenation of dimethyl 1, 4-cyclohexanedicarboxylate to 1, 4-cyclohexanedimethanol: Essential roles of metal dispersion and chemical environment

被引:15
|
作者
Luo, Jingjie [1 ,2 ]
Qu, Enhui [1 ,2 ]
Zhou, Yixue [1 ,2 ]
Dong, Yanan [1 ,2 ]
Liang, Changhai [1 ,2 ]
机构
[1] Dalian Univ Technol, Sch Chem Engn, State Key Lab Fine Chem, Panjin Campus, Panjin 124221, Peoples R China
[2] Dalian Univ Technol, Sch Chem Engn, Lab Adv Mat & Catalyt Engn AMCE, Panjin Campus, Panjin 124221, Peoples R China
基金
中国国家自然科学基金;
关键词
Rhenium catalyst; Selective hydrogenation; DMCD; CHDM; Activated carbon; Surface functionalization; AQUEOUS-PHASE HYDROGENATION; BIMETALLIC CATALYSTS; RAMAN-SPECTROSCOPY; SINGLE-STEP; CARBON; PERFORMANCE; RE; 1,4-CYCLOHEXANEDIMETHANOL; TEREPHTHALATE; ACID;
D O I
10.1016/j.apcata.2020.117669
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
Rhenium, although viewed as one of the noble metals with lower-price, has been commonly used as doping element in the bimetallic catalysts due to its middlebrow to activate hydrogen. Its major role as catalyst is less frequently mentioned. In this work, rhenium has been decorated on the surface of activated carbon and used for the selective hydrogenation of dimethyl 1, 4-cyclohexanedicarboxylate (DMCD) to 1, 4-cyclohexanedimethanol (CHDM). Characterizations suggested that ReOx particles were anchored occupying the surface oxygenated groups on pre-functionalized carbon. Rhenium decoration modified both the textural and chemical properties of the samples. Electrons were easily transferred from Re to the neighboring C atoms as a result of the formation of fine ReOx particles. Medium strong acid sites were generated and rhenium species in the reduced states could be still maintained under appropriate rhenium dispersion. The moderate hydrogenation ability of rhenium catalyst partially restrained the excessive hydrogenation of CHDM to other by-products. Rational decoration of 5 wt% Re performed the better catalytic performance with complete conversion of diester and 66 % yield of diol. The specific rate reached 9.5 x 10 mmol(DMCD).g(Re)(-1).h(-1) at 220 degrees C under 10 MPa H-2.
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页数:10
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