Pd nanoparticles immobilized on MIL-53(Al) as highly effective bifunctional catalysts for oxidation of liquid methanol to methyl formate

被引:18
作者
Liu, Jian-Fang [1 ]
Mu, Jin-Cheng [1 ]
Qin, Rong-Xian [1 ]
Ji, Sheng-Fu [1 ]
机构
[1] Beijing Univ Chem Technol, State Key Lab Chem Resource Engn, Beijing 100029, Peoples R China
基金
中国国家自然科学基金;
关键词
MIL-53(Al); Pd; Bifunctional catalyst; Methanol; Methyl formate; SUPPORTED PALLADIUM NANOPARTICLES; METAL-ORGANIC FRAMEWORKS; SELECTIVE OXIDATION; PHASE OXIDATION; AEROBIC OXIDATION; BENZYL ALCOHOL; MOLECULAR-OXYGEN; AU; PHOSPHORESCENCE; NANOCLUSTERS;
D O I
10.1007/s12182-019-0334-6
中图分类号
TE [石油、天然气工业]; TK [能源与动力工程];
学科分类号
0807 ; 0820 ;
摘要
A series of Pd/MIL-53(Al) heterogeneous bifunctional catalysts with different Pd contents were prepared by an impregnation method. The prepared metal-organic frameworks MIL-53(Al) and catalysts were characterized by XRD, SEM, HRTEM, FT-IR and N-2 adsorption/desorption techniques. The results showed that MIL-53(Al) was synthesized successfully, and the structure was unchanged during and after the preparation of the catalysts. The Pd nanoparticles (NPs) with an average particle size of 4.6 nm were uniformly dispersed on the MIL-53(Al). The catalyst exhibited good catalytic activity in the selective oxidation of liquid methanol to methyl formate. Under the conditions of 150 degrees C, 2 MPa O-2 and solvent-free for 5 h, the conversion of methanol could reach 60.3%, and the selectivity of methyl formate was up to 62.2%. In addition, the Pd/MIL-53(Al) bifunctional catalyst exhibited excellent stability and maintained high catalytic activity after five cycles.
引用
收藏
页码:901 / 911
页数:11
相关论文
共 63 条
[1]   Catalyst parameters determining activity and selectivity of supported gold nanoparticles for the aerobic oxidation of alcohols:: The molecular reaction mechanism [J].
Abad, Alberto ;
Corma, Avelino ;
Garcia, Hermenegildo .
CHEMISTRY-A EUROPEAN JOURNAL, 2008, 14 (01) :212-222
[3]  
[Anonymous], 2017, Angew. Chem
[4]   Selective oxidation of alcohols and aldehydes on metal catalysts [J].
Besson, M ;
Gallezot, P .
CATALYSIS TODAY, 2000, 57 (1-2) :127-141
[5]   Size-dependent catalytic activity of supported palladium nanoparticles for aerobic oxidation of alcohols [J].
Chen, Jing ;
Zhang, Qinghong ;
Wang, Ye ;
Wan, Huilin .
ADVANCED SYNTHESIS & CATALYSIS, 2008, 350 (03) :453-464
[6]   CH3O decomposition on PdZn(111), Pd(111), and Cu(111).: A theoretical study [J].
Chen, ZX ;
Neyman, KM ;
Lim, KH ;
Rösch, N .
LANGMUIR, 2004, 20 (19) :8068-8077
[7]   Engineering Metal Organic Frameworks for Heterogeneous Catalysis [J].
Corma, A. ;
Garcia, H. ;
Llabres i Xamena, F. X. L. I. .
CHEMICAL REVIEWS, 2010, 110 (08) :4606-4655
[8]   Au, Pd (mono and bimetallic) catalysts supported on graphite using the immobilisation method - Synthesis and catalytic testing for liquid phase oxidation of glycerol [J].
Dimitratos, N ;
Porta, F ;
Prati, L .
APPLIED CATALYSIS A-GENERAL, 2005, 291 (1-2) :210-214
[9]   Slective liquid phase oxidation with supported metal nanoparticles [J].
Dimitratos, Nikolaos ;
Lopez-Sanchez, Jose A. ;
Hutchings, Graham J. .
CHEMICAL SCIENCE, 2012, 3 (01) :20-44
[10]   Discrimination of active palladium sites in catalytic liquid-phase oxidation of benzyl alcohol [J].
Ferri, Davide ;
Mondelli, Cecilia ;
Krumeich, Frank ;
Baiker, Alfons .
JOURNAL OF PHYSICAL CHEMISTRY B, 2006, 110 (46) :22982-22986