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Journal of the American Chemical Society Jul 2024Oscillations in the chemical or physical properties of materials, composed of an odd or even number of connected repeating methylene units, are a well-known phenomenon...
Oscillations in the chemical or physical properties of materials, composed of an odd or even number of connected repeating methylene units, are a well-known phenomenon in organic chemistry and materials science. So far, such behavior has not been reported for the important class of materials, perovskite semiconductors. This work reports a distinct odd-even oscillation of the molecular structure and charge carrier transport properties of phenylalkylammonium two-dimensional (2D) Sn-based perovskites in which the alkyl chains in the phenylalkylammonium cations contain varying odd and even carbon numbers. Density functional theory calculations and grazing-incidence wide-angle X-ray scattering characterization reveal that perovskites with organic ligands containing an alkyl chain with an odd number of carbon atoms display a disordered crystal lattice and tilted inorganic octahedra accompanied by reduced mobilities. In contrast, perovskites with cations of an even number of carbon atoms in the alkyl chain form more ordered crystal structures, resulting in improved charge carrier mobilities. Our findings disclose the importance of minor changes in the molecular conformation of organic cations have an effect on morphology, photophysical properties, and charge carrier transport of 2D layered perovskites, showcasing alkyl chain engineering of organic cations to control key properties, of layered perovskite semiconductors.
PubMed: 38953716
DOI: 10.1021/jacs.4c03936 -
Chemical Communications (Cambridge,... Jul 2024The emergence of materials that can effectively convert photon energy (light) into motion (mechanical work) and change their shapes on command is of great interest for... (Review)
Review
The emergence of materials that can effectively convert photon energy (light) into motion (mechanical work) and change their shapes on command is of great interest for their potential in the fabrication of devices (powered by light) that will revolutionize the technologies of optical actuators, smart medical devices, soft robotics, artificial muscles and flexible electronics. Recently, metal-organic crystals have emerged as desirable smart hybrid materials that can hop, split and jump. Thus, their incorporation into polymer host objects can control movement from molecules to millimetres, opening up a new world of light-switching smart materials. This feature article briefly summarizes the recent part of the fast-growing literature on photomechanical properties in metal-organic crystals, such as coordination compounds, coordination polymers (CPs), and metal-organic frameworks (MOFs). The article highlights the contributions of our group along with others in this area and aims to provide a consolidated idea of the engineering strategies and structure-property relationships of these hybrid materials for such rare phenomena with diverse potential applications.
PubMed: 38953709
DOI: 10.1039/d4cc02655a -
ACS Nano Jul 2024Chronic wound rescue is critical for diabetic patients but is challenging to achieve with a specific and long-term strategy. The prolonged bacterial inflammation is...
Chronic wound rescue is critical for diabetic patients but is challenging to achieve with a specific and long-term strategy. The prolonged bacterial inflammation is particularly prevalent in hyperglycemia-induced wounds, usually leading to severe tissue damage. Such a trend could further suffer from an environmental suitability provided by macrophages for persisting () and even deteriorate by their mutual reinforcement. However, the strategy of both suppressing bacteria growth and immunoreprogramming the inflammatory type of macrophages to break their vicious harm to wound healing is still lacking. Here, a self-adapting biomass carboxymethyl chitosan (CMC) hydrogel comprising immunomodulatory nanoparticles is reported to achieve Gram-negative/Gram-positive bacteria elimination and anti-inflammatory cytokines induction to ameliorate the cutaneous microenvironment. Mechanistically, antibacterial peptides and CMCs synergistically result in a long-term inhibition against methicillin-resistant (MRSA) over a period of 7 days, and miR-301a reprograms the M2 macrophage via the PTEN/PI3Kγ/mTOR signaling pathway, consequently mitigating inflammation and promoting angiogenesis for diabetic wound healing in rats. In this vein, immunoregulatory hydrogel is a promising all-biomass dressing ensuring biocompatibility, providing a perspective to regenerate cutaneous damaged tissue, and repairing chronic wounds on skin.
PubMed: 38953692
DOI: 10.1021/acsnano.4c02736 -
Journal of the American Chemical Society Jul 2024The development of intrinsically recyclable cross-linked materials remains challenged by the inherently unfavorable chemical equilibrium that dictates the efficiency of...
The development of intrinsically recyclable cross-linked materials remains challenged by the inherently unfavorable chemical equilibrium that dictates the efficiency of the reversible covalent bonding/debonding chemistry. Rather than having to (externally) manipulate the bonding equilibrium, we here introduce a new reversible chemistry platform based on monosubstituted thiomaleimides that can undergo complete and independent light-activated covalent bonding and on-demand thermal debonding above 120 °C. Specifically, repeated bonding/debonding of a small-molecule thiomaleimide [2 + 2] photodimer is demonstrated over five heat/light cycles with full conversion in both directions, thereby regenerating its initial monothiomaleimide constituents. This motivated the synthesis of multifunctional thiomaleimide reagents as precursors for the design of covalently cross-linked networks that display intrinsic switching between a monomeric and polymeric state. The resulting materials are shown to covalently dissociate and depolymerize upon heating both in solution and in bulk, thus transforming the densely photo-cross-linked material back into a viscous liquid. Temperature-regulated photorheology evidenced the intrinsic recyclability of the thiomaleimide-based thermosets during multiple cycles of UV cross-linking and thermal de-cross-linking. The thermally reversible photodimerization of thiomaleimides presents a new addition to the designer playground of dynamic polymer networks, providing interesting opportunities for the reprocessing and closed-loop recycling of covalently cross-linked materials.
PubMed: 38953610
DOI: 10.1021/jacs.4c04193 -
Clinical Cardiology Jul 2024The DESyne novolimus-eluting coronary stent (NES) is a new-generation drug-eluting stent (DES) that is widely used, but clinical data are rarely reported for this stent.... (Observational Study)
Observational Study Comparative Study
INTRODUCTION
The DESyne novolimus-eluting coronary stent (NES) is a new-generation drug-eluting stent (DES) that is widely used, but clinical data are rarely reported for this stent. We compared the safety and effectiveness of the DESyne NES and the Orsiro bioresorbable polymer sirolimus-eluting stent (SES) in patients undergoing percutaneous coronary intervention (PCI).
METHODS
This was a retrospective, single-center, observational study. Between July 2017 and December 2022, patients who presented with chronic or acute coronary syndrome undergoing PCI with DESyne NES or Orsiro SES were consecutively enrolled in the present study. The primary endpoint, major adverse cardiovascular event (MACE), was a composite of cardiovascular death, target-vessel myocardial infarction, or clinically driven target-lesion revascularization.
RESULTS
A total of 776 patients (age 68.8 ± 12.2; 75.9% male) undergoing PCI were included. Overall, 231 patients with 313 lesions received NES and 545 patients with 846 lesions received SES. During a follow-up duration of 784 ± 522 days, the primary endpoint occurred in 10 patients (4.3%) in the NES group and in 36 patients (6.6%) in the SES group. After multivariate adjustment, the risk of MACE did not significantly differ between groups (NES vs. SES, hazard ratio 0.74, 95% CI, 0.35-1.55, p = 0.425). The event rate of individual components of the primary endpoint was comparable between the two groups.
CONCLUSIONS
Favorable and similar clinical outcomes were observed in patients undergoing PCI with either NES or SES in a medium-term follow-up duration. Future studies with adequately powered clinical endpoints are required for further evaluation.
Topics: Humans; Drug-Eluting Stents; Male; Female; Sirolimus; Retrospective Studies; Aged; Percutaneous Coronary Intervention; Treatment Outcome; Prosthesis Design; Coronary Artery Disease; Time Factors; Follow-Up Studies; Acute Coronary Syndrome; Risk Factors; Middle Aged; Coronary Angiography; Macrolides
PubMed: 38953595
DOI: 10.1002/clc.24317 -
Dalton Transactions (Cambridge, England... Jul 2024Synthesis and reactivity with carbon dioxide (CO) of divalent samarium in the bis-tris(pyrazolyl)borate ligand environment has been reported. In addition, CO activation...
Synthesis and reactivity with carbon dioxide (CO) of divalent samarium in the bis-tris(pyrazolyl)borate ligand environment has been reported. In addition, CO activation and functionalisation by lanthanide silylamides in the bis-tris(pyrazolyl)borate ligand environment was demonstrated. Reduction of the Sm(III) precursor [Sm(Tp)(OTf)] (Tp = hydrotris(1-pyrazolyl)borate; OTf = triflate) with KC yielded the insoluble Sm(II) multi-metallic coordination polymer [{Sm(Tp)}] 1-Sm. Addition of 1,2-dimethoxyethane (DME) to 1-Sm enabled isolation of the monomeric complex [Sm(Tp)(DME)] 1-Sm(DME). Complex 1-Sm(DME) reduced CO to yield the oxalate-bridged dimeric Sm(III) complex [{Sm(Tp)}(μ-η:η-OCCO)] 2-Sm. The reactions of heteroleptic Ln(III) silylamide complexes [Ln(Tp)(N'')] (Ln = Y, Sm; N'' = N(SiMe)) with CO yielded monomeric Ln(III) silyloxides [Ln(Tp)(OSiMe)] 3-Ln and trimethylsilyl isocyanate (OCNSiMe). Complexes 3-Ln are the first crystallographically characterised examples of Ln(III)-OSiMe bonds accessed CO activation and functionalisation. Full characterisation data are presented for all complexes, including solid-state molecular structure determination by single-crystal X-ray diffraction.
PubMed: 38953525
DOI: 10.1039/d4dt01382d -
ACS Applied Materials & Interfaces Jul 2024Since the discovery of aggregation-induced emission from tetraphenylethylene derivatives, various methods have been explored to prepare highly efficient multicolored...
Since the discovery of aggregation-induced emission from tetraphenylethylene derivatives, various methods have been explored to prepare highly efficient multicolored luminescent materials. Herein, we report a simple and efficient strategy for constructing luminescent organic salts of the tetracationic luminogen, tetrapyridinium-tetraphenylethylene (T4Py-TPE), combined with seven di- and tetra-anionic aromatic sulfonate ligands. When aqueous solutions of the cationic luminogen and the anionic ligands were mixed, they rapidly aggregated into organic salts within seconds to minutes, giving yields of up to >90%. This was accompanied by an increase in the emission efficiency from ∼58% to almost 100%, and the ability to tune the emission color between 511 and 586 nm. These improvements were mainly attributed to the strong electrostatic attractions between the cation and anions, which resulted in the formation of a rigid hydrophobic network of the T4Py-TPE luminogen with various π-conjugation lengths. Because these compounds are commercially available, this method opens the possibility of fabricating novel light-emitting materials for device fabrication and research.
PubMed: 38953487
DOI: 10.1021/acsami.4c03180 -
The Chinese Journal of Dental Research Jun 2024To evaluate the effect of different adhesives and veneering resins on the shear bond strength (SBS) of polyetheretherketone (PEEK).
OBJECTIVE
To evaluate the effect of different adhesives and veneering resins on the shear bond strength (SBS) of polyetheretherketone (PEEK).
METHODS
A total of 138 PEEK specimens were randomly divided into 6 groups according to adhesive material application: Control (C, no application), Adhese Universal (A) (Ivoclar Vivadent, Schaan, Liechtenstein), Gluma Bond Universal (G) (Heraeus Kulzer, South Bend, IN, USA), G-PremioBOND (P) (GC Corporation, Tokyo, Japan), Single Bond Universal (S) (3M, Saint Paul, MN, USA) and visio.link (V) (Bredent, Senden, Germany). Each adhesive group was divided into two subgroups according to the type of veneering material: Estenia direct composite (D) and Gradia Plus indirect composite (IN) (both GC Corporation). After the veneering process, the specimens were aged by thermal cycling. Kruskal-Wallis and Mann-Whitney U tests were used for SBS analysis (P < 0.05).
RESULTS
The highest SBS results were obtained in the VIN group, followed by the VD, PD, GIN, AIN, AD, SIN, SD, PIN, GD, CIN and CD groups, respectively (P = 0.001). There were no significant differences in terms of the type of veneering composite when the same adhesive was applied (P > 0.05), except for Gluma Bond Universal (P = 0.009). All the adhesives tested showed clinically acceptable SBS results.
CONCLUSION
Visio.link offered the highest adhesion to PEEK, whereas the tested universal adhesives may be used as an alternative to visio.link in clinical settings. It was determined that changing the veneer type has no statistical difference when the same adhesive material is used.
Topics: Benzophenones; Polyethylene Glycols; Ketones; Composite Resins; Polymers; Dental Veneers; Shear Strength; Materials Testing; Dental Bonding; Humans; Resin Cements; Dental Stress Analysis; Bisphenol A-Glycidyl Methacrylate
PubMed: 38953481
DOI: 10.3290/j.cjdr.b5459601 -
The Chinese Journal of Dental Research Jun 2024As the biological mechanisms of orthodontic tooth movement have been explored further, scholars have gradually focused on the remodelling mechanism of the extracellular... (Review)
Review
As the biological mechanisms of orthodontic tooth movement have been explored further, scholars have gradually focused on the remodelling mechanism of the extracellular matrix (ECM) in the periodontal ligament (PDL). The ECM of the PDL consists of various types of collagens and other glycoproteins. The specific process and mechanism of ECM remodelling during orthodontic tooth movement remains unclear. Collagen I and III, which constitute major components of the PDL, are upregulated under orthodontic force. The changes in the contents of ECM proteins also depend on the expression of ECM-related enzymes, which organise new collagen fibre networks to adapt to changes in tooth position. The matrix metalloproteinase family is the main enzyme that participates in collagen hydrolysis and renewal and changes its expression under orthodontic force. Moreover, ECM adhesion molecules, such as integrins, are also regulated by orthodontic force and participate in the dynamic reaction of cell adhesion and separation with the ECM. This article reviews the changes in ECM components, related enzymes and adhesion molecules in the PDL under orthodontic force to lay the foundation for the exploration of the regulatory mechanism of ECM remodelling during orthodontic tooth movement.
Topics: Extracellular Matrix; Humans; Tooth Movement Techniques; Periodontal Ligament; Periodontium; Matrix Metalloproteinases; Integrins; Collagen
PubMed: 38953477
DOI: 10.3290/j.cjdr.b5459583 -
Journal of the American Chemical Society Jul 2024Direct air capture (DAC) shows considerable promise for the effective removal of CO; however, materials applicable to DAC are lacking. Among metal-organic framework...
Direct air capture (DAC) shows considerable promise for the effective removal of CO; however, materials applicable to DAC are lacking. Among metal-organic framework (MOF) adsorbents, diamine-Mg(dobpdc) (dobpdc = 4,4-dioxidobiphenyl-3,3'-dicarboxylate) effectively removes low-pressure CO, but the synthesis of the organic ligand requires high temperature, high pressure, and a toxic solvent. Besides, it is necessary to isolate the ligand for utilization in the synthesis of the framework. In this study, we synthesized a new variant of extended MOF-74-type frameworks, M(hob) (M = Mg, Co, Ni, and Zn; hob = 5,5'-(hydrazine-1,2-diylidenebis(methanylylidene))bis(2-oxidobenzoate)), constructed from an azine-bonded organic ligand obtained through a facile condensation reaction at room temperature. Functionalization of Mg(hob) with -methylethylenediamine, -ethylethylenediamine, and ,'-dimethylethylenediamine (mmen) enables strong interactions with low-pressure CO, resulting in top-tier adsorption capacities of 2.60, 2.49, and 2.91 mmol g at 400 ppm of CO, respectively. Under humid conditions, the CO capacity was higher than under dry conditions due to the presence of water molecules that aid in the formation of bicarbonate species. A composite material combining mmen-Mg(hob) and polyvinylidene fluoride, a hydrophobic polymer, retained its excellent adsorption performance even after 7 days of exposure to 40% relative humidity. In addition, the one-pot synthesis of Mg(hob) from a mixture of the corresponding monomers is achieved without separate ligand synthesis steps; thus, this framework is suitable for facile large-scale production. This work underscores that the newly synthesized Mg(hob) and its composites demonstrate significant potential for DAC applications.
PubMed: 38953459
DOI: 10.1021/jacs.4c05318