Chem Catalysis, Journal Year: 2024, Volume and Issue: 4(9), P. 101076 - 101076
Published: Aug. 20, 2024
Language: Английский
Chemical Reviews, Journal Year: 2024, Volume and Issue: 124(16), P. 9457 - 9579
Published: Aug. 16, 2024
The large production volumes of commodity polyolefins (specifically, polyethylene, polypropylene, polystyrene, and poly(vinyl chloride)), in conjunction with their low unit values multitude short-term uses, have resulted a significant pressing waste management challenge. Only small fraction these is currently mechanically recycled, the rest being incinerated, accumulating landfills, or leaking into natural environment. Since are energy-rich materials, there considerable interest recouping some chemical value while simultaneously motivating more responsible end-of-life management. An emerging strategy catalytic depolymerization, which portion C-C bonds polyolefin backbone broken assistance catalyst and, cases, additional molecule reagents. When products molecules materials higher own right, as feedstocks, process called upcycling. This review summarizes recent progress for four major upcycling strategies: hydrogenolysis, (hydro)cracking, tandem processes involving metathesis, selective oxidation. Key considerations include macromolecular reaction mechanisms relative to mechanisms, design transformations, effect conditions on product selectivity. Metrics describing critically evaluated, an outlook future advances described.
Language: Английский
Citations
26
ACS Applied Materials & Interfaces, Journal Year: 2025, Volume and Issue: unknown
Published: Jan. 2, 2025
Combination therapy, which involves using multiple therapeutic modalities simultaneously or sequentially, has become a cornerstone of modern cancer treatment. Graphene-based nanomaterials (GBNs) have emerged as versatile platforms for drug delivery, gene and photothermal therapy. These materials enable synergistic approach, improving the efficacy treatments while reducing side effects. This review explores roles graphene, graphene oxide (GO), quantum dots (GQDs) in combination therapies highlights their potential to enhance immunotherapy targeted therapies. The large surface area high drug-loading capacity facilitate codelivery agents, promoting sustained release. GQDs, with unique optical properties, offer real-time imaging capabilities, adding another layer precision However, challenges such biocompatibility, long-term toxicity, scalability need be addressed ensure clinical safety. Preclinical studies show promising results GBNs, suggesting revolutionize treatment through innovative
Language: Английский
Citations
2
JACS Au, Journal Year: 2024, Volume and Issue: 4(6), P. 2081 - 2098
Published: June 4, 2024
Single-use polyolefins are widely used in our daily life and industrial production due to their light weight, low cost, superior stability, durability. However, the rapid accumulation of plastic waste low-profit recycling methods resulted a global crisis. Catalytic hydrogenolysis is regarded as promising technique, which can effectively selectively convert polyolefin value-added products. In this perspective, we focus on design synthesis structurally well-defined catalysts across mesoscopic, nanoscopic, atomic scales, accompanied by insights into future directions catalyst for further enhancing catalytic performance. These principles also be applied depolymerization other polymers ultimately realize chemical upcycling plastics.
Language: Английский
Citations
9
Giant, Journal Year: 2024, Volume and Issue: 19, P. 100307 - 100307
Published: June 14, 2024
Polyolefins are the most produced and widely used polymeric materials. However, chemically inert nature of polyolefins has led to severe environmental pollution, posing a threat human sustenance development. Managing recycling polyolefin plastic waste is crucial for transition from linear sustainable circular economy. Catalytic chemical includes traditional techniques like pyrolysis photolysis, innovative methods that introduce cleavable bonds into chain closed-loop recycling. post-functionalization post-consumer materials another strategy tackle waste, aiming upgrade materials' utility contribute sustainability. Overall, developing catalytic deconstructing upcycling plastics essential encourage better reclamation practices reduce impact waste.
Language: Английский
Citations
9
ACS Materials Letters, Journal Year: 2024, Volume and Issue: 6(7), P. 2609 - 2616
Published: May 28, 2024
The combination of photocatalysis and biocatalysis in a heterogeneous fashion for enantioselective catalysis is great importance but still underexplored. Herein, we rationally design construct photoenzymatic platform catalysis, by mechanochemical synthesis strategy to simultaneously encapsulate photocatalyst WGL into robust Zr-based MOF. Due the rapid minimizing use organic solvents strong acid, fabricated photobiocatalysts show high photobiological activity operational stability, hence affording good performance reusability asymmetric Mannich reactions. These wide substrate scope (up 12 substrates) are first used N-aryl-substituted tetrahydroisoquinoline substrates, which have not yet been achieved photobiocatalysis yet. Furthermore, various characterization techniques unveil superoxide anions singlet oxygen as main active substances catalysis. This research marks pivotal step toward crafting range enzyme-MOF tailored diverse applications across industrial processes.
Language: Английский
Citations
8
Chemistry - A European Journal, Journal Year: 2024, Volume and Issue: unknown
Published: April 16, 2024
Although it is well-known that the Lewis acidity of Metal-Organic Frameworks (MOFs) can effectively enhance their catalytic activity in organic transformations, access to these Lewis-acidic sites remains a key hurdle widespread applications catalysis by MOFs. Easy accessibility strong acidic onto 2D MOFs using proper activation methods be cornerstone attaining desired performance. Herein, we report new chemically stable MOF, IITKGP-60, which displayed excellent framework robustness over wide pH range (2-12). Benefiting from abundant open metal (OMSs) and robustness, developed material was explored one-pot three-component Strecker reaction Knoevenagel condensation reaction. Moreover, catalyst superior catalyzing reactions involving sterically hindered substrate (1-naphthaldehyde) with high turnover number. A comparative study conducted different (chloroform methanol exchanged activated samples), highlighting significant effect on its performances. The sustainable synthetic pathway under solvent-free conditions for broad scope substrates low loading recyclability made pH-stable promising heterogeneous catalyst.
Language: Английский
Citations
5
New Journal of Chemistry, Journal Year: 2025, Volume and Issue: 49(6), P. 2071 - 2078
Published: Jan. 1, 2025
A porous and recyclable metal–organic framework-confined bipyridyl-Co( ii ) chloride catalyst enables direct N -alkylation of anilines to the corresponding amines in high yield produces H 2 O as by-product.
Language: Английский
Citations
0
JACS Au, Journal Year: 2025, Volume and Issue: 5(4), P. 1760 - 1770
Published: April 16, 2025
Ru/C-catalyzed polyethylene (PE) and hydrocarbon hydrogenolysis under quasi-supercritical fluid of isopentane was kinetically mechanistically investigated. PE with C-C C-H cleavage showed zeroth order, suggesting strong adsorption hydrocarbons. yielded broad product distribution heavy (C21-40) diesel-range (C11-20) hydrocarbons in the primary step due to stochastic over Ru surface. Catalytic n-hexadecane, squalane, light such as n-pentane, iso-pentane, n-hexane further described reactivity between secondary carbons, i.e., 1C-2C 2C-2C, which has an order magnitude higher rate than that involving a tertiary carbon. The saturated surface lower carbon therefore, imited sovlent conversion during hydrogenolysis, whereas leading selective conversion. Using hexadecane, we observed comparable rates H2 D2 (k H /k D ∼ 1), indicating relevant facilitating rehydrogenation. However, normal kinetic isotope effect hexadecane deuterated C16H34 C16D34 5) revealed dehydrogenation, cleavage, can be involved kinetic. By considering 8-fold H-D exchange compared for attributed C-D bond dissociation energy being 3 kJ/mol bond. Increasing pressure favors internal terminal one. This minimizes formation hydrocarbons, particularly methane. increase increases coverage adsorbed hydrogen on particles competitive polyethylene, which, turn, reduces rates.
Language: Английский
Citations
0
Inorganic Chemistry, Journal Year: 2024, Volume and Issue: 63(25), P. 11907 - 11916
Published: June 8, 2024
Direct hydroxylation of benzene to phenol is more appealing in the industry for economic and environmentally friendly synthesis than conventional cumene process. We have developed a UiO-metal-organic framework (MOF)-supported mono bipyridyl-Iron(II) hydroxyl catalyst [bpy-UiO-Fe(OH)
Language: Английский
Citations
3
Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(44)
Published: Aug. 1, 2024
Abstract Polyolefins such as polyethylenes and polypropylenes are the most‐produced plastic waste globally, yet difficult to convert into useful products due their unreactivity. Pyrolysis is a practical method for large‐scale treatment of mixed, contaminated plastic, allowing conversion industrially‐relevant petrochemicals. Metal–organic frameworks (MOFs), despite tremendous utility in heterogeneous catalysis, have been overlooked polyolefin depolymerization perceived thermal instabilities inability penetrate pores. Herein, we demonstrate viability UiO‐66 MOFs containing coordinatively‐unsaturated zirconium nodes, effective catalysts pyrolysis that significantly enhances yields valuable liquid gas hydrocarbons, whilst halving amounts residual solids produced. Reactions occur on Lewis‐acidic without need noble metals, yield aliphatic product distributions distinctly different from aromatic‐rich hydrocarbons can be obtained zeolite catalysis. We also first unambiguous characterization penetration pores at pyrolytic temperatures, access abundant Zr‐oxo nodes within MOF interior efficient C−C cleavage. Our work highlights potential highly‐designable depolymerisation plastics, which complement conventional reactivity.
Language: Английский
Citations
3