期刊
INORGANIC CHEMISTRY
卷 59, 期 12, 页码 8161-8172出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.inorgchem.0c00481
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资金
- Universita dell'Insubria
- Italian MIUR through the PRIN 2017 Project Multi-e: Multielectron Transfer for the Conversion of Small Molecules: an Enabling Technology for the Chemical Use of Renewable Energy [20179337R7]
- TRAINER project (Catalysts for Transition to Renewable Energy Future) [ANR-17-MPGA-0017]
- Italian MIUR throughout the PRIN 2015 Project Towards a Sustainable Chemistry [20154 x 9ATP_002]
- European Union's Horizon 2020 research and innovation program under the Marie Sklodowska-Curie grant [641887]
- Spanish Government [MAT2017-82288-C2-1-P, SEV-2016-0683]
Three metal-organic frameworks with the general formula Co(BPZX) (BPZX(2-) = 3-X-4,4'-bipyrazolate, X = H, NH2, NO2) constructed with ligands having different functional groups on the same skeleton have been employed as heterogeneous catalysts for aerobic liquid-phase oxidation of cumene with O-2 as oxidant. O-2 adsorption isotherms collected at p(O2) = 1 atm and T = 195 and 273 K have cast light on the relative affinity of these catalysts for dioxygen. The highest gas uptake at 195 K is found for Co(BPZ) (3.2 mmol/g (10.1 wt % O-2)), in line with its highest BET specific surface area (926 m(2)/g) in comparison with those of Co(BPZNH(2)) (317 m(2)/g) and Co(BPZNO(2)) (645 m(2)/g). The O-2 isosteric heat of adsorption (Q(2)) trend follows the order Co(BPZ) > Co(BPZNH(2)) > Co(BPZNO(2)). Interestingly, the selectivity in the cumene oxidation products was found to be dependent on the tag present in the catalyst linker: while cumene hydroperoxide (CHP) is the main product obtained with Co(BPZ) (84% selectivity to CHP after 7 h, p(O2) = 4 bar, and T = 363 K), further oxidation to 2-phenyl-2-propanol (PP) is observed in the presence of Co(BPZNH(2)) as the catalyst (69% selectivity to PP under the same experimental conditions).
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