Inorganic Chemistry Frontiers, Journal Year: 2023, Volume and Issue: 11(2), P. 462 - 469
Published: Nov. 15, 2023
Presented herein is a study focusing on the effect of organic shell ligands configuration ring structure with same nuclearity, and their photo-related applications, such as fluorescence third-order nonlinear response.
Language: Английский
Chemical Reviews, Journal Year: 2023, Volume and Issue: 123(9), P. 5225 - 5261
Published: Jan. 20, 2023
Because sunlight is the most abundant energy source on earth, it has huge potential for practical applications ranging from sustainable supply to light driven chemistry. From a chemical perspective, excited states generated by make thermodynamically uphill reactions possible, which forms basis storage into fuels. In addition, with light, open-shell species can be open up new reaction pathways in organic synthesis. Crucial are photosensitizers, absorb and transfer substrates various mechanisms, processes that highly depend distance between molecules involved. Supramolecular coordination cages well studied synthetically accessible vessels single cavities guest binding, ensuring close proximity of different components. Due high modularity their size, shape, nature metal centers ligands, ideal platforms exploit preorganization photocatalysis. Herein we focus application supramolecular photocatalysis artificial photosynthesis photo(redox) catalysis. Finally, brief overview immobilization strategies provides tools implementing devices. This review inspiration future design photocatalytic host-guest systems producing solar fuels complex molecules.
Language: Английский
Citations
169
Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(14), P. 7692 - 7711
Published: March 28, 2023
Self-assembled discrete molecular architectures that show selective recognition within their internal cavities are highly desirable. Such hosts often guest through several noncovalent interactions. This emulates the activity of naturally occurring enzymes and proteins. Research in formation 3D cages different shapes sizes has progressed rapidly since development coordination-driven self-assembly dynamic covalent chemistry. find applications catalysis, stabilization metastable molecules, purification isomeric mixtures via encapsulation, even biomedical applications. Most these stem from ability host to bind guests strongly a fashion, providing suitable environment for perform functions. Molecular having closed with small windows either poor encapsulation or inhibit easy release while those wide open structures fail form stable host-guest complexes. In this context, barrels obtained by metal-ligand/covalent bond techniques possess optimized architectures. With hollow-walled cavity two large openings, satisfy structural requirements many perspective, we will discuss detail synthetic strategies obtaining barrel-like employing coordination interactions, structure-based classification, storing transient separation chemicals, photoinduced antibacterial activity. We aim highlight advantages over other efficiently carrying out functions new
Language: Английский
Citations
64
Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)
Published: Sept. 28, 2023
Developing efficient adsorbents to capture radioactive iodine produced from nuclear wastes is highly desired. Here we report the facial synthesis of a hexacationic imidazolium organic cage and its adsorption properties. Crucial role counteranions has been disclosed for with this cage, where distinct behaviors were observed when different used. Mechanistic investigations, especially X-ray crystallographic analysis iodine-loaded sample, allowed direct visualization binding modes at molecular level. A network multiple non-covalent interactions including hydrogen bonds, halogen anion···π interactions, electrostatic interaction between polyiodides skeleton are found responsible high performance. Our results may provide an alternative strategy design adsorbents.
Language: Английский
Citations
44
Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(42), P. 23361 - 23371
Published: Oct. 16, 2023
Molecular recognition lies at the heart of biological functions, which inspires lasting research in artificial host syntheses to mimic biomolecules that can recognize, process, and transport molecules with highest level complexity; nonetheless, design principle quantifying methodology hosts for multiple guests (≥4) remain a formidable task. Herein, we report two rhombic dodecahedral cages [(Zn/Fe)8Pd6-MOC-16], embrace 12 adaptive pockets multiguest binding distinct conformational dynamics inherent metal-center lability are able capture 4-24 manifest surprising complexity scenarios. The exceptional high-order hierarchical encapsulation phenomena suggest wide host-guest dynamic-fit, enabling adjustment adaptation beyond duality induced-fit selection protein interactions. A critical inspection events solution has been performed by NMR ESI-MS spectra, highlighting importance acquiring reliable repertoire from different techniques uncertainty affinities multiplying an oversimplified method.
Language: Английский
Citations
30
Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(14)
Published: Feb. 8, 2023
Post-synthetic modification (PSM) is an effective approach for the tailored functionalization of metal-organic architectures, but its generalizability remains challenging. Herein we report a general covalent PSM strategy to functionalize Pdn L2n cages (MOCs, n=2, 12) through efficient Diels-Alder cycloaddition between peripheral anthracene substituents and various functional motifs bearing maleimide group. As expected, solubility functionalized Pd12 L24 in common solvents can be greatly improved. Interestingly, concentration-dependent circular dichroism aggregation-induced emission are achieved with chiral binaphthol (BINOL)- tetraphenylethylene-modified , respectively. Furthermore, introduced two different groups (e.g., BINOL achiral pyrene) step-by-step route obtain chirality-induced circularly polarized luminescence. Moreover, similar results readily observed smaller Pd2 L4 system.
Language: Английский
Citations
27
Nano-Micro Letters, Journal Year: 2024, Volume and Issue: 16(1)
Published: June 25, 2024
The development of supramolecular hosts which can efficiently encapsulate photosensitizers to improve the photodynamic efficacy holds great promise for cancer therapy. Here, we report two perylene diimide-based metallacages that form stable host-guest complexes with planar conjugated molecules including polycyclic aromatic hydrocarbons and (hypocrellin A). Such complexation not only prevents aggregation in aqueous environments, but also offers fluorescence resonance energy transfer (FRET) from metallacage further singlet oxygen generation (Φ
Language: Английский
Citations
11
Analytical Chemistry, Journal Year: 2024, Volume and Issue: 96(36), P. 14508 - 14515
Published: Aug. 23, 2024
An ultrasensitive self-powered biosensor is constructed for miRNA-21 detection based on Au nanoparticles @ Pd nanorings (Au NPs@Pd NRs) and catalytic hairpin assembly (CHA). The NRs possess excellent electrical conductivity to improve the electron transfer rate show good elimination of byproduct H2O2 assist glucose oxidase (GOD) catalyze glucose; CHA used as an amplification strategy effectively enhance sensitivity biosensor. To further amplify output signal, a capacitor integrated into With multiple signal strategies, possesses linear range 0.1–10–4 fM lower limit (LOD) 0.032 (S/N = 3). In addition, as-prepared displays potential applicability in assay toward human serum samples.
Language: Английский
Citations
9
Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)
Published: March 4, 2025
Supramolecular nanoreactor as artificial mimetic enzyme is attracting a growing interest due to fine-tuned cavity and host-guest molecular recognition. Here, we design three 3d-4f metallo-supramolecular nanocages with different sizes active sites (Zn2Er4L14, Zn4Er6L26, Zn2Er8L38) based on "bimetallic cluster cutting" strategy. Three exhibit differential catalysis for the three-component aza-Darzens reaction without another additive, only Zn2Er8L38 largest most lanthanides centers has excellent catalytic conversion monosubstituted disubstituted N-aryl aziridine products. The relationship investigations confirm that significantly outperforms Zn2Er4L14 smaller Zn4Er6L26 fewer Lewis acidic in multi-component mainly attributed synergy of inherent confinement effect multiple nanocage. strategy construction large windows may represent potential approach develop supramolecular high efficiency.
Language: Английский
Citations
1
Science China Chemistry, Journal Year: 2023, Volume and Issue: 66(7), P. 1940 - 1962
Published: May 22, 2023
Language: Английский
Citations
18
Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(11)
Published: Jan. 13, 2024
Abstract Modifying redox potential of substrates and intermediates to balance pairs steps are important stages for multistep photosynthesis but faced marked challenges. Through co‐clathration iridium photosensitizer imine substrate within one packet a metal‐organic capsule shift the potentials substrate, herein, we reported multiphoton enzymatic strategy generation heterocycles by intramolecular C−X hydrogen evolution cross‐couplings. The cage facilitated pre‐equilibrium substrate‐involving clathrate that cathodic shifts oxidation substrate‐dye‐host ternary complex configuration inversion via spatial constraints in confined space. new two photon excitation enabled precise control electron transfer between each pair (photosensitizer, capsule), endowing catalytic system proceeding smoothly with an fashion. Three kinds 2‐subsituted (−OH, −NH 2 , −SH) imines N‐aryl enamines all give corresponding cyclization products efficiently under visible light irradiation, demonstrating promising microenvironment driven thermodynamic activation host‐dye‐substrate synergistic combination photocatalytic transformations.
Language: Английский
Citations
8