Selective hydrogenation of aromatic carboxylic acids over basic N-doped mesoporous carbon supported palladium catalysts

被引:67
作者
Jiang, Hezhan [1 ]
Yu, Xiaolong [1 ]
Nie, Renfeng [1 ]
Lu, Xinhuan [1 ]
Zhou, Dan [1 ]
Xia, Qinghua [1 ]
机构
[1] Hubei Univ, Hubei Collaborat Innovat Ctr Adv Organ Chem Mat, Key Lab Synth & Applicat Organ Funct Mol, Minist Educ,Sch Chem & Chem Engn, Wuhan 430062, Peoples R China
基金
中国国家自然科学基金;
关键词
Mesoporous carbon nitride; Polymerization; Basicity; Palladium; Selective hydrogenation; REDUCED GRAPHENE OXIDE; FREE AEROBIC OXIDATION; BENZOIC-ACID; CHEMOSELECTIVE HYDROGENATION; AMORPHOUS ALLOY; ACTIVE-CARBON; NITROGEN; EFFICIENT; NANOTUBE; PHENOL;
D O I
10.1016/j.apcata.2016.04.009
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
Mesoporous carbon nitride (MCN) has been prepared through a simple polymerization reaction between ethylenediamine (EDA) and carbon tetrachloride (CTC) by a nano hard-templating approach. The obtained MCN possesses high surface area (166.3 m(2)/g), average pore size of 9.2 nm and high N content (up to 18.5 wt%). The negative charge and the basicity on MCN surface are originated from its rich carbon nitride heterocycles, which notably improves the surface hydrophilicity and the adsorption of acidic molecules. Furthermore, MCN can be adopted as the proper support for highly dispersed Pd NPs with well-controlled size distribution. Compared with microporous N-doped active carbon with low N-content, the MCN-supported Pd catalyst shows an enhanced activity in water phase for the selective ring hydrogenation of benzoic acid, benzamide and phenol, in which 11.3 times higher activity in comparison to undoped catalyst is achieved. Wide characterizations reveal that big pore size, selective adsorption for acid substrate and strong interaction between N and Pd may lead to the high activity of Pd/MCN. (C) 2016 Elsevier B.V. All rights reserved.
引用
收藏
页码:73 / 81
页数:9
相关论文
共 63 条
[1]   Nanostructured materials for advanced energy conversion and storage devices [J].
Aricò, AS ;
Bruce, P ;
Scrosati, B ;
Tarascon, JM ;
Van Schalkwijk, W .
NATURE MATERIALS, 2005, 4 (05) :366-377
[2]   Nature of the N-Pd Interaction in Nitrogen-Doped Carbon Nanotube Catalysts [J].
Arrigo, Rosa ;
Schuster, Manfred E. ;
Xie, Zailai ;
Yi, Youngmi ;
Wowsnick, Gregor ;
Sun, Li L. ;
Hermann, Klaus E. ;
Friedrich, Matthias ;
Kast, Patrick ;
Haevecker, Michael ;
Knop-Gericke, Axel ;
Schloegl, Robert .
ACS CATALYSIS, 2015, 5 (05) :2740-2753
[3]   Dynamics of Palladium on Nanocarbon in the Direct Synthesis of H2O2 [J].
Arrigo, Rosa ;
Schuster, Manfred E. ;
Abate, Salvatore ;
Wrabetz, Sabine ;
Amakawa, Kazuhiko ;
Teschner, Detre ;
Freni, Maria ;
Centi, Gabriele ;
Perathoner, Siglinda ;
Haevecker, Michael ;
Schloegl, Robert .
CHEMSUSCHEM, 2014, 7 (01) :179-194
[4]   New Insights from Microcalorimetry on the FeOx/CNT-Based Electrocatalysts Active in the Conversion of CO2 to Fuels [J].
Arrigo, Rosa ;
Schuster, Manfred E. ;
Wrabetz, Sabine ;
Girgsdies, Frank ;
Tessonnier, Jean-Philippe ;
Centi, Gabriele ;
Perathoner, Siglinda ;
Su, Dang Sheng ;
Schloegl, Robert .
CHEMSUSCHEM, 2012, 5 (03) :577-586
[5]   ORGANIC FUNCTIONAL-GROUP HYDROGENATION [J].
AUGUSTINE, RL .
CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 1976, 13 (02) :285-316
[6]   Chemoselective Hydrogenation of Benzoic Acid over Ni-Zr-B-PEG(800) Nanoscale Amorphous Alloy in Water [J].
Bai, Guoyi ;
Wen, Xin ;
Zhao, Zhen ;
Li, Fei ;
Dong, Huixian ;
Qiu, Mande .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2013, 52 (06) :2266-2272
[7]   Unexpected Inversions in Asymmetric Reactions: Reactions with Chiral Metal Complexes, Chiral Organocatalysts, and Heterogeneous Chiral Catalysts [J].
Bartok, Mihaly .
CHEMICAL REVIEWS, 2010, 110 (03) :1663-1705
[8]  
Bianchi D, 2000, ANGEW CHEM INT EDIT, V39, P4321, DOI 10.1002/1521-3773(20001201)39:23<4321::AID-ANIE4321>3.0.CO
[9]  
2-5
[10]   Electrochemical properties of nitrogen-doped carbon nanotube anode in Li-ion batteries [J].
Bulusheva, L. G. ;
Okotrub, A. V. ;
Kurenya, A. G. ;
Zhang, Hongkun ;
Zhang, Huijuan ;
Chen, Xiaohong ;
Song, Huaihe .
CARBON, 2011, 49 (12) :4013-4023