Nitrogen-Rich Barium–Organic Framework for Capture and Cocatalysts Free Chemical Fixation of CO₂ via Cyclic Carbonates and Oxazolidinones

ACS Applied Materials & Interfaces, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 17, 2025

The carbon dioxide (CO2) capture and utilization strategy has emerged as an innovative multifaceted approach to counteract emissions. In this study, a highly porous muffin polyhedral barium (Ba) ̵ organic framework (BaTATB; H3TATB = 4,4',4″-s-triazine-2,4,6-triyl-tribenzoic acid) was synthesized solvothermally. three-dimensional honeycomb pore architectures were densely populated with Lewis acidic Ba(II) metal sites basic nitrogen-rich triazines. BaTATB demonstrated selective CO2 adsorption high heat of adsorption. Its abundance (Ba clusters) (triazine) makes ideal catalyst for the cycloaddition epoxides in two- three-component reactions. Furthermore, is exceptional recyclable aromatic amines, enabling high-yield synthesis cyclic carbonates oxazolidinone at 1 bar under moderate, solvent-free, cocatalyst-free conditions. Additionally, recycled nine seven consecutive cycles carbonate no substantial decrease catalytic activity. Using density functional theory, we rational design metal-organic frameworks that exhibit excellent conversion.

Language: Английский

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Bifunctional two-dimensional copper-organic framework for high catalytic performance on cycloaddition of CO2 with epoxides and deacetalization-Knoevenagel condensation

Journal of Molecular Structure, Journal Year: 2024, Volume and Issue: 1306, P. 137849 - 137849

Published: Feb. 22, 2024

Language: Английский

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Metal Hydrogen-Bonded Organic Frameworks as Open Lewis Acid Catalysts for Two Types of CO₂ Transformations

Inorganic Chemistry, Journal Year: 2024, Volume and Issue: 63(25), P. 11554 - 11565

Published: May 30, 2024

Efficient and multiple CO2 utilization into high-value-added chemicals holds significant importance in carbon neutrality industry production. However, most catalysis systems generally exhibit only one type of transformation with the efficiency to be improved. The restricted abundance active catalytic sites or an inefficient rate these results constraint. Consequently, we designed constructed two metal hydrogen-bonded organic frameworks (M-HOFs) {[M3(L3–)2(H2O)10]·2H2O}n (M = Co (1), Ni (2); L 1-(4-carboxyphenyl)-1H-pyrazole-3,5-dicarboxylic acid) this research. 1 2 are well-characterized, both show excellent stability. networks connected by hydrogen bonds enhance structural flexibility create accessible Lewis acidic sites, promoting interactions between substrates centers. This enhancement facilitates efficient for types transformations, encompassing cycloaddition reactions epoxides aziridines afford cyclic carbonates oxazolidinones. activities (TON/TOF) superior compared those other catalysts. These heterogeneous catalysts still exhibited high performance after being reused several times. Mechanistic studies indicated intense substrates, demonstrating reason catalysis. marks first instance on M-HOFs efficiently catalyzing conversions, finding important significance catalyst design utilization.

Language: Английский

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Robust Nitro-Functionalized {Zn₃}-Organic Framework for Excellent Catalytic Performance on Cycloaddition Reaction of CO₂ with Epoxides and Knoevenagel Condensation

Crystal Growth & Design, Journal Year: 2024, Volume and Issue: 24(8), P. 3473 - 3482

Published: April 8, 2024

Adjusting the Lewis acid–base sites in MOF-based catalysts to meet demand for catalytic CO2 chemical fixation is a huge challenge. Herein, highly robust rectilinear {Zn3}-based metal–organic framework of {[Zn3(TNTNB)2(4,4′-bip)(H2O)2]·5DMF·9H2O}n (NUC-80) was generalized from solvothermal condition (H3TNTNB = 1,3,5-tri(3-nitro-4-carboxyphenyl)-2,4,6-trinitrobenzene, 4,4′-bip 4,4′-bipyridine). Activated NUC-80a not only owns large void volume (58%) and two kinds solvent-accessible channels: rhombic-like (ca. 14.24 × 14.57 Å) along axis rectangular-like 11.72 14.48 b axis, but also functionalized by rich metal plentiful nitro groups on its inner surface. Performed experiments confirmed that could efficiently catalyze cycloaddition reaction with epoxides Knoevenagel condensations aldehydes malononitrile under mild conditions high turnover frequency (TOF). Hence, this work provides nitro-functionalized cluster-based nanoporous wide range potential applications such as catalysis, gas adsorption, separation.

Language: Английский

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Structure regulation and catalytic performance of amine-functionalized zeolitic imidazolate frameworks for CO2 cycloaddition

Separation and Purification Technology, Journal Year: 2024, Volume and Issue: 348, P. 127465 - 127465

Published: April 16, 2024

Language: Английский

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A multifunctional fluorescent Eu‐MOF probe: Its synthesis, structure, and sensing properties

Applied Organometallic Chemistry, Journal Year: 2024, Volume and Issue: 38(7)

Published: May 11, 2024

Based on 3‐(2,4‐dicarboxylphenyl)‐6‐carboxylpyridine ligand (H 3 dpcp), a lanthanide metal–organic framework with the porous three‐dimensional structure was successfully synthesized, namely, [Eu (dpcp)(H 2 O)] n ( 1 ). The experimental results indicated that complex exhibited stable luminescence in range of pH = 2–11 aqueous solution. It is noteworthy could recognize tryptophan (Trp) and trans, trans‐ muconic acid tt ‐MA) molecules through fluorescence quenching effect, showed high sensitivity, selectivity, recoverability, anti‐interference, low detection limits for identification Trp ‐MA In addition, mechanisms sensing were elucidated detail.

Language: Английский

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Revealing the roles of the dual active-sites on a polyoxometalate-based metal–organic framework in catalyzing Knoevenagel condensations

Applied Surface Science, Journal Year: 2024, Volume and Issue: 654, P. 159459 - 159459

Published: Jan. 20, 2024

Language: Английский

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Ultrahigh Stable Heterometallic InCo-Organic Framework for Efficiently Catalyzing Cycloaddition of CO2 with Epoxides and Knoevenagel condensation

Journal of Molecular Structure, Journal Year: 2024, Volume and Issue: 1318, P. 139223 - 139223

Published: July 6, 2024

Language: Английский

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Mechanochemical Encapsulation of Caffeine in UiO-66 and UiO-66-NH2 to Obtain Polymeric Composites by Extrusion with Recycled Polyamide 6 or Polylactic Acid Biopolymer

Polymers, Journal Year: 2024, Volume and Issue: 16(5), P. 637 - 637

Published: Feb. 27, 2024

The development of capsules with additives that can be added to polymers during extrusion processing lead advances in the manufacturing textile fabrics improved and durable properties. In this work, caffeine (CAF), which has anti-cellulite properties, been encapsulated by liquid-assisted milling zirconium-based metal–organic frameworks (MOFs) different textural properties chemical functionalization: commercial UiO-66, UiO-66 synthesized without solvents, UiO-66-NH2 ethanol. CAF@MOF obtained through grinding procedure have process recycled polyamide 6 (PA6) a biopolymer based on polylactic acid (PLA) obtain load approximately 2.5 wt% caffeine. materials characterized various techniques (XRD, NMR, TGA, FTIR, nitrogen sorption, UV–vis, SEM, TEM) confirm encapsulation, preservation process, good contact between polymer MOF. Studies PA6 polymer+capsules composites shown release is slower when than it free, influence more prominently NH2 group. However, an interaction established PLA delays additive.

Language: Английский

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Robust {Pb₁₀}-Cluster-Based Metal–Organic Framework for Capturing and Converting CO₂ into Cyclic Carbonates under Mild Conditions

Inorganic Chemistry, Journal Year: 2024, Volume and Issue: 63(30), P. 14183 - 14192

Published: July 15, 2024

Developing a highly active catalyst that can efficiently capture and convert carbon dioxide (CO2) into high-value-added energy materials remains severe challenge, which inspires us to explore effective metal–organic frameworks (MOFs) with high chemical stability high-density sites. Herein, we report robust 3D lead(II)-organic framework of {(Me2NH2)2[Pb5(PTTPA)2(H2O)3]·2DMF·3H2O}n (NUC-111) unreported [Pb10(COO)22(H2O)6] clusters (abbreviated as {Pb10}) nodes (H6PTTPA = 4,4′,4″-(pyridine-2,4,6-triyl)triisophthalic acid). After thermal activation, NUC-111a is functionalized by the multifarious symbiotic acid–base sites open Pb2+ uncoordinated pyridine groups on inner surface void volume. Gas adsorption tests confirm displays higher separation performance for mixed gases f CO2 CH4 selectivity CO2/CH4 at 273 K 101 kPa being 31 (1:99, v/v), 23 (15:85, 8 (50:50, respectively. When temperature rises 298 K, 26 22 11 v/v). Moreover, activated exhibited excellent catalytic performance, stability, recyclability cycloaddition epoxides under mild conditions. Hence, this work provides valuable insight designing MOFs multifunctionality capture, separation, conversion.

Language: Английский

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