PdHx Entrapped in a Covalent Triazine Framework Modulates Selectivity in Glycerol Oxidation

被引:34
作者
Chan-Thaw, Carine E. [1 ]
Villa, Alberto [1 ]
Wang, Di [2 ]
Dal Santo, Vladimiro [3 ]
Biroli, Alessio Orbelli [3 ]
Veith, Gabriel M. [4 ]
Thomas, Arne [5 ]
Prati, Laura [1 ]
机构
[1] Univ Milan, Dept Chem, I-20133 Milan, Italy
[2] Karlsruhe Inst Technol, Inst Nanotechnol & Karlsruhe Nano Micro Facil, Eggenstein Leopoldshafen, Germany
[3] CNR Ist Sci & Tecnol Mol, I-20133 Milan, Italy
[4] Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN 37831 USA
[5] Tech Univ Berlin, Dept Chem, Funct Mat, D-10623 Berlin, Germany
关键词
cleavage reactions; heterogeneous catalysis; nitrogen heterocycles; oxidation; palladium; AEROBIC OXIDATION; PHASE OXIDATION; SUPPORTED GOLD; CATALYSTS; NANOPARTICLES; POLYMERS; ALCOHOLS; HYDROGEN; LIGANDS; SIZE;
D O I
10.1002/cctc.201500055
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
Pd nanoparticles within a nitrogen-containing covalent triazine framework (CTF) material are investigated to understand if the highly tunable CTF chemistry mediates the catalytic properties of the Pd nanoparticles. Surprisingly, our results demonstrate that the CTF stabilizes the formation of 2.6nm PdHx particles within the pores. These confined PdHx particles are very active for the liquid-phase oxidation of glycerol and promote CC cleavage, probably connected with the enhanced insitu formation of H2O2. During recycling tests, the confined particles are transformed progressively to very stable Pd-0 particles. This stability has been attributed mainly to a confinement effect as nanoparticles trapped outside the pores lose activity rapidly. These results indicate that there is a potential to tune CTF chemistry to modify the chemistry of the catalytic metals significantly.
引用
收藏
页码:2149 / 2154
页数:6
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