期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 120, 期 28, 页码 15310-15321出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.6b05428
关键词
-
资金
- Universita dell'Insubria
The three Ni-based metal-organic frameworks (MOFs) Ni(BDP), Ni(BPEB), and Ni-3(BTP)(2) [H2BDP = 1,4(4-bispyrazolyl)benzene; H2BPEB = 1,4-bis(1H-pyrazol-4-ylethynyl)benzene; H3BTP = 1,3,5-tris(1H-pyrazol-4-yl)benzene] possessing square planar, potentially accessible metal sites, were preliminarily tested as catalysts in the base free selective oxidation of hydroxymethylfurfural to 2,5-diformylfuran (DFF). While Ni(BDP) undergoes degradation, Ni-3(BTP)(2) is the most active of the three MOFs, yielding 27% DFF after 24 h with a selectivity close to 100% under relatively mild reaction conditions (120 degrees C, 30 bar O-2, water as solvent). Upon flowing a model probe, in situ DRIFT and FT-IR spectroscopy were employed to rationalize the different performances of Ni(BPEB) and Ni-3(BTP)(2) in terms of adsorbate adsorbent interactions: Not only hydrogen bonds are at work between the hydroxyl functionality of the probe and the pore walls of the MOF, but also and more importantly, bands ascribed to Ni-OR stretching are detected, denouncing the insurgence of Ni-probe interactions. The different intensity of these bands in the two cases confirms the different accessibility of the metal centers, as suggested by crystal structure analysis and catalytic tests.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据