Browse
Submit Data
Databases
API
Help

Dataset Information

25 Views

0 Connections

0 Citations

0 Reanalyses

0 Downloads

Omics score: 0

Photosensitizer-Anchored 2D MOF Nanosheets as Highly Stable and Accessible Catalysts toward Artemisinin Production.

ABSTRACT: 2D metal-organic frameworks (2D-MOFs) have recently emerged as promising materials for gas separations, sensing, conduction, and catalysis. However, the stability of these 2D-MOF catalysts and the tunability over catalytic environments are limited. Herein, it is demonstrated that 2D-MOFs can act as stable and highly accessible catalyst supports by introducing more firmly anchored photosensitizers as bridging ligands. An ultrathin MOF nanosheet-based material, Zr-BTB (BTB = 1,3,5-tris(4-carboxyphenyl)benzene), is initially constructed by connecting Zr₆-clusters with the tritopic carboxylate linker. Surface modification of the Zr-BTB structure was realized through the attachment of porphyrin-based carboxylate ligands on the coordinatively unsaturated Zr metal sites in the MOF through strong Zr-carboxylate bond formation. The functionalized MOF nanosheet, namely PCN-134-2D, acts as an efficient photocatalyst for ¹O₂ generation and artemisinin production. Compared to the 3D analogue (PCN-134-3D), PCN-134-2D allows for fast reaction kinetics due to the enhanced accessibility of the catalytic sites within the structure and facile substrate diffusion. Additionally, PCN-134(Ni)-2D exhibits an exceptional yield of artemisinin, surpassing all reported homo- or heterogeneous photocatalysts for the artemisinin production.

SUBMITTER: Wang Y

PROVIDER: S-EPMC6548987 | biostudies-literature |

REPOSITORIES: biostudies-literature

ACCESS DATA

Json Xml

Similar Datasets

Benzotriazolium Salts: Emergent Readily Accessible Bench-Stable Lewis Acid Catalysts.

Project description:In this work, benzotriazolium salts have been introduced as efficient, readily accessible, bench-stable Lewis acid catalysts. Though these sorts of N-heterocyclic compounds have found wide applications as ionic liquids or electrolytes, their Lewis acid catalytic activity remained unexplored. Herein, their potential as Lewis acid catalysts was demonstrated in two prototypical allylic and Nazarov cyclization reactions, showing a matching reactivity and allowing low catalytic loadings (down to 0.5 mol %).

| S-EPMC9434991 | biostudies-literature

Surface oxygenation of multicomponent nanoparticles toward active and stable oxidation catalysts.

Project description:The need for active and stable oxidation catalysts is driven by the demands in production of valuable chemicals, remediation of hydrocarbon pollutants and energy sustainability. Traditional approaches focus on oxygen-activating oxides as support which provides the oxygen activation at the catalyst-support peripheral interface. Here we report a new approach to oxidation catalysts for total oxidation of hydrocarbons (e.g., propane) by surface oxygenation of platinum (Pt)-alloyed multicomponent nanoparticles (e.g., platinum-nickel cobalt (Pt-NiCo)). The in-situ/operando time-resolved studies, including high-energy synchrotron X-ray diffraction and diffuse reflectance infrared Fourier transform spectroscopy, demonstrate the formation of oxygenated Pt-NiOCoO surface layer and disordered ternary alloy core. The results reveal largely-irregular oscillatory kinetics associated with the dynamic lattice expansion/shrinking, ordering/disordering, and formation of surface-oxygenated sites and intermediates. The catalytic synergy is responsible for reduction of the oxidation temperature by ~100 °C and the high stability under 800 °C hydrothermal aging in comparison with Pt, and may represent a paradigm shift in the design of self-supported catalysts.

| S-EPMC7443134 | biostudies-literature

Molecular Design and Operational Stability: Toward Stable 3D/2D Perovskite Interlayers.

Project description:Despite organic/inorganic lead halide perovskite solar cells becoming one of the most promising next-generation photovoltaic materials, instability under heat and light soaking remains unsolved. In this work, a highly hydrophobic cation, perfluorobenzylammonium iodide (5FBzAI), is designed and a 2D perovskite with reinforced intermolecular interactions is engineered, providing improved passivation at the interface that reduces charge recombination and enhances cell stability compared with benchmark 2D systems. Motivated by the strong halogen bond interaction, (5FBzAI)2PbI4 used as a capping layer aligns in in-plane crystal orientation, inducing a reproducible increase of ≈60 mV in the V oc, a twofold improvement compared with its analogous monofluorinated phenylethylammonium iodide (PEAI) recently reported. This endows the system with high power conversion efficiency of 21.65% and extended operational stability after 1100 h of continuous illumination, outlining directions for future work.

| S-EPMC7539205 | biostudies-literature

Microwave- and ultrasonic-assisted synthesis of 2D La-based MOF nanosheets by coordinative unsaturation degree to boost phosphate adsorption.

Project description:The metal or metal clusters and organic ligands are relevant to the selectivity and performance of phosphate removal in MOFs, and the electron structure, chemical characteristics, and preparation method also affect efficiency and commercial promotion. However, few reports focus on the above, especially for 2D MOF nanomaterials. In this work, two 2D Ln-TDA (Ln = La, Ce) nanosheets assembled via microwave- and ultrasonic-assisted methods are employed as adsorbents for phosphate (H2PO4-, HPO42-) removal for the first time. Their microstructure and performance were characterized using XRD, TEM, SEM, AFM, FTIR, zeta potential, and DFT calculations. The prepared 2D Ln-TDA (Ln = La, Ce) nanosheets exposed more adsorption sites and effectively reduced the restrictions of mass transfer. Based on this, the Langmuir model was employed to estimate the maximum adsorption capacities of the two kinds of nanosheets, which reached 253.5 mg g-1 and 259.5 mg g-1, which are 553 times and 3054 times larger than those for bulk Ln-TDA (Ln = La, Ce), respectively. Additionally, the kinetic data showed that the adsorption equilibrium time is fast, approximately 15 min by the pseudo-second-order model. In addition, the prepared products not only have a wide application range (pH = 3-9) but also offer eco-safety in terms of residuals (no Ln leak out). Based on the XPS spectra, FTIR spectra and DFT calculations, the main adsorption mechanisms included ligand exchange and electrostatic interactions. This new insight provides a novel strategy to prepare 2D MOF adsorbents, achieving a more eco-friendly method (microwave- and ultrasonic-assisted synthesis) for preparing 2D Ln-based MOF nanosheets by coordinative unsaturation to boost phosphate adsorption.

| S-EPMC9743790 | biostudies-literature

A Brief Review of the Role of 2D Mxene Nanosheets toward Solar Cells Efficiency Improvement.

Project description:This article discusses the application of two-dimensional metal MXenes in solar cells (SCs), which has attracted a lot of interest due to their outstanding transparency, metallic electrical conductivity, and mechanical characteristics. In addition, some application examples of MXenes as an electrode, additive, and electron/hole transport layer in perovskite solar cells are described individually, with essential research issues highlighted. Firstly, it is imperative to comprehend the conversion efficiency of solar cells and the difficulties of effectively incorporating metal MXenes into the building blocks of solar cells to improve stability and operational performance. Based on the analysis of new articles, several ideas have been generated to advance the exploration of the potential of MXene in SCs. In addition, research into other relevant MXene suitable in perovskite solar cells (PSCs) is required to enhance the relevant work. Therefore, we identify new perspectives to achieve solar cell power conversion efficiency with an excellent quality-cost ratio.

| S-EPMC8541472 | biostudies-literature

Understanding CO<sub>2</sub>/CH<sub>4</sub> Separation in Pristine and Defective 2D MOF CuBDC Nanosheets via Nonequilibrium Molecular Dynamics.

Project description:The separation of CO2/CH4 gas mixtures is a key challenge for the energy sector and is essential for the efficient upgrading of natural gas and biogas. A new emerging field, that of metal-organic framework nanosheets (MONs), has shown the potential to outperform conventional separation methods and bulk metal-organic frameworks (MOFs). In this work, we model the CO2/CH4 separation in both defect-free and defective 2D CuBDC nanosheets and compare their performance with the bulk CuBDC MOF and experimental data. We report the results of external force nonequilibrium molecular dynamics (EF-NEMD) for pure components and binary mixtures. The EF-NEMD simulations reveal a pore blocking separation mechanism, in which the CO2 molecules occupy adsorption sites and significantly restrict the diffusion of CH4. The MON structure achieves a better selectivity of CO2 over CH4 compared to the bulk CuBDC MOF which is due to the mass transfer resistance of the methane molecules on the surface of the nanosheet. Our results show that it is essential to consider the real mixture in these systems rather than relying solely on pure component data and ideal selectivity. Furthermore, the separation is shown to be sensitive to the presence of missing linker defects in the nanosheets. Only 10% of missing linkers result in nonselective nanosheets. Hence, the importance of a defect-free synthetic method for CuBDC nanosheets is underlined.

| S-EPMC7685532 | biostudies-literature

Toward High-Performance Hydrogenation at Room Temperature Through Tailoring Nickel Catalysts Stable in Aqueous Solution.

Project description:The development of highly active, reusable catalysts for aqueous-phase reactions is challenging. Herein, metallic nickel is encapsulated in a nitrogen-doped carbon-silica composite (SiO2@Ni@NC) as a catalyst for the selective hydrogenation of vanillin in aqueous media. The constructed catalyst achieved 99.8% vanillin conversion and 100% 4-hydroxymethyl-2-methoxyphenol selectivity at room temperature. Based on combined scanning transmission electron microscopy, X-ray photoelectron spectroscopy, and Raman analyses, the satisfactory catalytic performance is attributed to the composite structure consisting of an active metal, carbon, and silica. The hydrophilic silica core promoted dispersion of the catalyst in aqueous media. Moreover, the external hydrophobic NC layer has multiple functions, including preventing oxidation or leaching of the internal metal, acting as a reducing agent to reduce the internal metal, regulating the active-site microenvironment by enriching the concentrations of H2 and organic reactants, and modifying the electronic structure of the active metal via metal-support interactions. Density functional theory calculations indicated that NC facilitates vanillin adsorption and hydrogen dissociation to promote aqueous-phase hydrogenation. This study provides an efficient strategy for constructing encapsulated Ni-based amphiphilic catalysts to upgrade biomass-derived compounds.

| S-EPMC11199984 | biostudies-literature

Ultrapermeable Composite Membranes Enhanced Via Doping with Amorphous MOF Nanosheets.

Project description:Thin-film composite (TFC) polymeric membranes have attracted increasing interest to meet the demands of industrial gas separation. However, the development of high-performance TFC membranes within their current configuration faces two key challenges: (i) the thickness-dependent gas permeability of polymeric materials (mainly poly(dimethylsiloxane) (PDMS)) and (ii) the geometric restriction effect due to the limited pore accessibility of the underlying porous substrate. Here we demonstrate that the incorporation of trace amounts (∼1.8 wt %) of amorphous metal-organic framework (MOF) nanosheets into the gutter layer of TFC assemblies can simultaneously address these two limitations by the creation of rapid, transmembrane gas diffusion pathways. The resultant PDMS&MOF membrane displayed excellent CO2 permeance of 10450 GPU and CO2/N2 selectivity of 9.1. Leveraging this strategy, we successfully fabricate a novel TFC membrane, consisting of a PDMS&MOF gutter and an ultrathin (∼54 nm) poly(ethylene glycol) top selective layer via surface-initiated atom transfer radical polymerization. The complete TFC membrane exhibits excellent processability and remarkable CO2/N2 separation performance (1990 GPU with a CO2/N2 ideal selectivity of 39). This study reveals a strategy for the design and fabrication of a new TFC membrane system with unprecedented gas-separation performance.

| S-EPMC8155479 | biostudies-literature

Synthesis of a 2D phosphorus material in a MOF-based 2D nano-reactor.

Project description:Synthesis of two dimensional (2D) materials mainly relies on interface-templates, exfoliation of layered crystals and surfactant-assistance. Here we have realized another strategy of polymerization in a 2D nano-reactor. As an application of this strategy, a 2D nano-reactor was constructed within a new pillar-layer metal organic framework (MOF) and in this nano-reactor a moderately stable 2D phosphorus material was synthesized from white phosphorus (P4). Our research may provide a new approach for the synthesis of various 2D materials.

| S-EPMC6050534 | biostudies-literature

2D/2D coupled MOF/Fe composite metamaterials enable robust ultra–broadband microwave absorption

Project description: Not available

| S-EPMC11226717 | biostudies-literature