The high catalytic activity of metal-organic frameworks (MOFs) can be realized by increasing their effective active sites, which prompts us to perform the functionalization on selected linkers by introducing a strong Lewis basic group of fluorine. Herein, the exquisite combination of paddle-wheel [Cu(CO)(HO)] clusters and meticulously designed fluorine-funtionalized tetratopic 2',3'-difluoro-[-terphenyl]-3,3″,5,5″-tetracarboxylic acid (F-Hptta) engenders one peculiar nanocaged {Cu}-organic framework of {[Cu(F-ptta)(HO)]·5DMF·2HO} (), which features two types of nanocaged voids (9.8 Å × 17.2 Å and 10.1 Å × 12.4 Å) shaped by 12 paddle-wheel [Cu(COO)HO)] secondary building units, leaving a calculated solvent-accessible void volume of 60.6%. Because of the introduction of plentifully Lewis base sites of fluorine groups, activated exhibits excellent catalytic performance on the cycloaddition reaction of CO with various epoxides under mild conditions. Moreover, to expand the catalytic scope, the deacetalization-Knoevenagel condensation reactions of benzaldehyde dimethyl acetal and malononitrile were performed using the heterogenous catalyst of . Also, features high recyclability and catalytic stability with excellent catalytic performance in subsequent catalytic tests. Therefore, this work not only puts forward a new solution for developing high-efficiency heterogeneous catalysts, but also enriches the functionalization strategies for nanoporous MOFs.
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http://dx.doi.org/10.1021/acs.inorgchem.2c01686 | DOI Listing |
ACS Appl Mater Interfaces
January 2025
Department of Aviation Oil and Material, Air Force Logistics Academy, 72 Xi Ge Road, Xuzhou, Jiangsu 221000, China.
Metal-air batteries desire highly active, durable, and low-cost oxygen reduction catalysts to replace expensive platinum (Pt). The Fe-N-C catalyst is recognized as the most promising candidate for Pt; however, its durability is hindered by carbon corrosion, while activity is restricted due to limited oxygen for the reaction. Herein, TiN is creatively designed to be hybridized with Fe-N-C (TiN/Fe-N-C) to relieve carbon corrosion and absorb more oxygen when catalyzing oxygen reduction.
View Article and Find Full Text PDFJ Am Chem Soc
January 2025
State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China.
Monolayer MoS is an effective electrocatalyst for the hydrogen evolution reaction (HER). Despite significant efforts to optimize the active sites, its catalytic performance still falls short of theoretical predictions. One key factor that has often been overlooked is the electron injection from the conductive substrate into the MoS.
View Article and Find Full Text PDFACS Appl Mater Interfaces
January 2025
Faculty of Chemistry, Jagiellonian University in Krakow, Gronostajowa 2, 30-387 Krakow, Poland.
Hydrogen, a sustainable and environmentally friendly fuel, can be obtained through the ethanol steam reforming (ESR) process. The most promising catalysts for this process are those based on non-noble metals such as cobalt. The activity, selectivity, and stability of these catalysts strongly depend on the presence of alkali dopants.
View Article and Find Full Text PDFACS Appl Bio Mater
January 2025
Department of Chemistry, University of North Dakota, Grand Forks, North Dakota 58202, United States.
Synergistic photodynamic/photothermal therapy (PDT/PTT) can be used to target cancer cells by locally generating singlet oxygen species or increasing temperature under laser irradiation. This approach offers higher tumor ablation efficiency, lower therapeutic dose requirements, and reduced side effects compared to single treatment approaches. However, the therapeutic efficiency of PDT/PTT is still limited by the low oxygen levels within the solid tumors caused by abnormal vasculature and altered cancer cell metabolism.
View Article and Find Full Text PDFPhys Chem Chem Phys
January 2025
State Key Laboratory of Fine Chemicals, Liaoning Key Laboratory for Catalytic Conversion of Carbon Resources, School of Chemistry, Dalian University of Technology, Dalian 116024, China.
Metal-free boron-based materials exhibit remarkable performance in oxidative dehydrogenation of propane (ODHP). Rational design of boron-based catalysts requires a systematic understanding of the underlying mechanisms to constitute a knowledge base. This work provides a comprehensive view of the reaction mechanism of the boron-based ODH reaction and discusses the key features of the reaction systems, including the inhibition of deep oxidation, high olefin selectivity, and the role of water in the ODHP reaction.
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