Nanocage-Based In^III{Tb^III}₂-Organic Framework Featuring Lotus-Shaped Channels for Highly Efficient CO₂ Fixation and I₂ Capture

ACS Applied Materials & Interfaces, Год журнала: 2020, Номер 12(24), С. 27803 - 27811

Опубликована: Май 28, 2020

The exquisite combination of independent 3p [In(CO2)4] units and 4f [Tb2(CO2)8] clusters in the presence designed hexatopic 2,4,6-tri(2,4-dicarboxyphenyl)pyridine ligand engenders one peculiar nanocaged In(III){Tb(III)}2-organic framework: ({(Me2NH2)[InTb2(HTDP)2]·3DMF·3H2O}n, designated as NUC-5), which features dual types lotus-shaped channels along [100] [110] axes with related node windows 5.3 × 6.8 12.1 9.2 Å2, respectively. To best our knowledge, except several coexisted 3p-4f In/Ln {In3Ln}- {In3Ln2}-based metal–organic frameworks (MOFs), NUC-5 is novel type heterometallic framework. In addition, its topology was an unprecedented 3D TAYZIC net a Schläfli symbol {4.462}{4.565}2{4.66.88}. Moreover, activated proved to be efficient adsorbent for CO2 recycled cycloaddition catalyst transformation epoxides into carbonates high yields under mild conditions. Furthermore, excellent reversible sorption performance I2 volatilization phase or cyclohexane solution maximum adsorption capacity 609.1 mg/g (3.75 iodine molecules per unit cell) makes promising radioactive products 129I 131I field nuclear industry. This study provides synthetic strategy that original nature MOFs could enhanced by introducing some specific function-prompted inorganic subunits aid predesigned supporting ligands.

Язык: Английский

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Alterations to secondary building units of metal–organic frameworks for the development of new functions

Inorganic Chemistry Frontiers, Год журнала: 2019, Номер 7(1), С. 12 - 27

Опубликована: Окт. 28, 2019

Post-synthetic modification methods for the secondary building units in MOFs facilitate unique structures and properties that are impossible to accessviadirect syntheses, which can be classified as four categories.

Язык: Английский

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Metal–Organic Layers for Synergistic Lewis Acid and Photoredox Catalysis

Journal of the American Chemical Society, Год журнала: 2020, Номер 142(4), С. 1746 - 1751

Опубликована: Янв. 13, 2020

We report the design of a new multifunctional metal-organic layer (MOL), Hf12-Ir-OTf, comprising triflate (OTf)-capped Hf12 secondary building units (SBUs) and photosensitizing Ir(DBB)[dF(CF3)ppy]2+ [DBB-Ir-F, DBB = 4,4'-di(4-benzoato)-2,2'-bipyridine; dF(CF3)ppy 2-(2,4-difluorophenyl)-5-(trifluoromethyl)pyridine] bridging ligands. Hf12-Ir-OTf effectively catalyzed dehydrogenative cross-couplings heteroarenes with ethers, amines, unactivated alkanes turnover numbers 930, 790, 950, respectively. also competently late-stage functionalization bioactive drug molecules such as caffeine, Fasudil, Metyrapone. The superior catalytic performance over mixture photoredox catalyst stoichiometric amounts Brønsted acids or substoichiometric (20 mol %) Lewis is attributed to close proximity (1.2 nm) between acid catalysts in which not only facilitates reaction carbon radical activated heteroarene but accelerates electron transfer from nitrogen intermediate Ir(IV) species cycle.

Язык: Английский

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Improved photocatalytic CO2 and epoxides cycloaddition via the synergistic effect of Lewis acidity and charge separation over Zn modified UiO-bpydc

Applied Catalysis B Environment and Energy, Год журнала: 2021, Номер 301, С. 120793 - 120793

Опубликована: Окт. 7, 2021

Язык: Английский

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Boosting Photocatalytic Hydrogen Peroxide Production from Oxygen and Water Using a Hafnium-Based Metal–Organic Framework with Missing-Linker Defects and Nickel Single Atoms

ACS Catalysis, Год журнала: 2022, Номер 12(24), С. 14825 - 14835

Опубликована: Ноя. 22, 2022

Metal–organic frameworks (MOFs) are one of the most promising candidates for photocatalytic hydrogen peroxide (H2O2) production from dioxygen (O2) and water. However, MOF-driven H2O2 O2 water remains a challenge because MOF photocatalysts need to exhibit high structural stability in aqueous reaction systems while suppressing decomposition. In present study, we demonstrate that Hf-based UiO-66-NH2 with missing-linker defects Ni single atoms dramatically promotes under visible-light (λ > 420 nm) irradiation. The acetate-capped lead suppression nonradiative relaxation organic linkers prevention decomposition, whereas single-atom cocatalysts promote separation photogenerated charges selective two-electron oxidation generate H2O2. synergetic effect improves production, resulting 6.3-fold increase activity compared pristine Hf-UiO-66-NH2. This study provides not only new insights into defect engineering but also an important strategy achieving highly via reduction oxidation.

Язык: Английский

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Metal-organic framework as a heterogeneous catalyst for biodiesel production: A review

Chemical Engineering Journal Advances, Год журнала: 2022, Номер 12, С. 100415 - 100415

Опубликована: Окт. 17, 2022

Nowadays, as there is a rapid depletion of fossil fuels, the need for alternative resources has become inevitable. Biodiesel such an that environmentally friendly and sustainable. Over years been significant amount research done biofuel production by converting various feedstocks edible non-edible vegetable oil, animal fats, waste cooking microalgae feedstock which requires highly workable efficient catalyst transesterification process. Several heterogeneous catalysts have used biodiesel to biodiesel, among metal-organic framework (MOF) gained popularity owing its high surface area, pore volume, facile tunability active sites. This review focuses on different types MOFs, characterization techniques identify vital structurally invoked changes, deactivation MOFs due leaching species, blocking sites, unzipping covering literature from year 2000 till date. Finally, brief conclusion author's perspective depicting several challenges scope future needs in MOF study provided.

Язык: Английский

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The Local Vibrational Mode Theory and Its Place in the Vibrational Spectroscopy Arena

The Journal of Physical Chemistry A, Год журнала: 2022, Номер 126(47), С. 8781 - 8798

Опубликована: Ноя. 8, 2022

This Feature Article starts highlighting some recent experimental and theoretical advances in the field of IR Raman spectroscopy, giving a taste breadth dynamics this striving field. The local mode theory is then reviewed, showing how vibrational modes are derived from fundamental normal modes. New features introduced that add to current efforts: (i) unique measure bond strength based on force constants ranging bonding single molecules different environments periodic systems crystals (ii) new way interpret spectra by pinpointing probing interactions between particular stretching contributions All represents means work around very nature modes, namely motions polyatomic delocalized. Three focus points analysis reported, demonstrating extracts important information hidden spectroscopy data supporting experiments: metal–ligand heme proteins, such as myoglobin neuroglobin; disentanglement DNA modes; (iii) hydrogen water clusters ice. Finally, use other research groups summarized. Our vision future will be routinely applied community serves an incubator for collaborations experiment theory.

Язык: Английский

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Recent advances in metal-organic-framework-based catalysts for thermocatalytic selective oxidation of organic substances

Chem Catalysis, Год журнала: 2022, Номер 2(5), С. 1009 - 1045

Опубликована: Март 14, 2022

Язык: Английский

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Defective iron based metal-organic frameworks derived from zero-valent iron for highly efficient fenton-like catalysis

Journal of Hazardous Materials, Год журнала: 2022, Номер 445, С. 130426 - 130426

Опубликована: Ноя. 21, 2022

Язык: Английский

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Engineering of catalytically active sites in photoactive metal–organic frameworks

Coordination Chemistry Reviews, Год журнала: 2022, Номер 465, С. 214561 - 214561

Опубликована: Апрель 25, 2022

Язык: Английский

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