Elucidating the promotional effect of a covalent triazine framework in aerobic oxidation

被引:18
作者
Abednatanzi, Sara [1 ]
Derakhshandeh, Parviz Gohari [1 ]
Tack, Pieter [2 ]
Muniz-Miranda, Francesco [3 ]
Liu, Ying-Ya [4 ]
Everaert, Jonas [5 ]
Meledina, Maria [6 ,7 ]
Vanden Bussche, Flore [1 ,5 ]
Vincze, Laszlo [2 ]
Stevens, Christian, V [5 ]
Van Speybroeck, Veronique [3 ]
Vrielinck, Henk [8 ]
Callens, Freddy [8 ]
Leus, Karen [1 ]
Van Der Voort, Pascal [1 ]
机构
[1] Univ Ghent, Ctr Ordered Mat Organometall & Catalysis COMOC, Dept Chem, Krijgslaan 281-S3, B-9000 Ghent, Belgium
[2] Univ Ghent, Dept Chem, Xray Microspect & Imaging XMI, Krijgslaan 281,S12, B-9000 Ghent, Belgium
[3] Univ Ghent, Ctr Mol Modeling CMM, Technol Pk 903, B-9052 Zwijnaarde, Belgium
[4] Dalian Univ Technol, State Key Lab Fine Chem, Dalian 116024, Peoples R China
[5] Univ Ghent, Fac Biosci Engn, Dept Green Chem & Technol, Coupure Links 653, B-9000 Ghent, Belgium
[6] Rhein Westfal TH Aachen, Cent Facil Electron Microscopy, D-52074 Aachen, Germany
[7] Forschungszentrum Julich, Ernst Ruska Ctr ER C 2, D-52425 Julich, Germany
[8] Univ Ghent, Dept Solid State Sci, Krijgslaan 281-S1, B-9000 Ghent, Belgium
基金
中国国家自然科学基金;
关键词
Covalent triazine frameworks; Heterogeneous catalysis; Synergistic effect; Oxygen activation; Mechanistic studies; ALCOHOL OXIDATION; LIQUID-PHASE; CATALYSTS; TEMPERATURE; DEHYDROGENATION; IRIDIUM(III); COMPLEXES; OXYGEN; GREEN;
D O I
10.1016/j.apcatb.2020.118769
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
Synergistic catalysis holds great promise to enhance the catalytic performance of heterogeneous catalysts suffering from sluggish reaction kinetics. Much effort has been dedicated to the development of bimetallic systems in which the two promoter elements display synergistic benefits compared to monometallic counterparts. However, the use of bimetallic catalysts inescapably raises the cost of preparation and environmental issues. This study discovers a synergistic effect when using a bipyridine covalent triazine framework (bipy-CTF) as support for an Ir-III complex in the aerobic oxidation reaction. The detailed mechanistic study provides insights into the function of the bipy-CTF in this synergistic catalysis. The EPR and in-situ XANES analyses confirm the applicability of bipy-CTF to activate oxygen and alcohol, resulting in an enhancement of the performance of the Ir-III complex to exceed the activity of the homogeneous counterpart. This is an unprecedented report on promoting the activity of a heterogeneous catalyst through its solid support.
引用
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页数:9
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