Latest ArticlesDefects can strongly affect the lattice, strain, and electronic structures of nanomaterials photocatalysts, like a double-edged sword of both positive significance and negative influence on photocatalytic performances. To date, most studies into defects only partially elucidated their beneficial or detrimental roles in photocatalysis. However, a quantitative understanding of the photocatalytic performances modulated by defect concentration still needs to be discovered. Here, a series of TiO2−X mesoporous spheres (MS) with different oxygen vacancy concentrations for photocatalytic applications were prepared by high-temperature chemical reduction. The link between oxygen vacancy concentration and photocatalytic performance was successfully established. The localization of carriers dominated by the Stark effect is first enhanced and then weakened with increasing oxygen vacancy concentration, which is a crucial factor in explaining the double-edged sword role of defect concentration in photocatalysis. As the reduction temperature rises to 300 ℃, carrier localization dominated by the quantum-confined Stark effect maximizes the separation ability of photo generated electron hole pairs, thus exhibiting the best catalytic performance for photocatalytic hydrogen production and the degradation of organic pollutants, as demonstrated by a hydrogen evolution rate of 523.7 µmol g-1 h-1 and a ninefold higher RhB photodegradation rate compared to TiO2 MS. The work offers excellent flexibility for precisely constructing high-performance photocatalysts by understanding vacancy engineering.
1-(4-(1,1-Dimethylethyl)phenyl)-3-(4-methoxyphenyl)-1,3-propanedione (known as Avobenzone/AVB), widely used throughout the world as a highly effective UVA absorber, can prevent the progression of photoaging in skin, and is also known for the disadvantage of having a reduced capability to absorb UVA when exposed to sunlight for long periods. To address this challenge, ZnTi-CO3-LDH with a two-dimensional layered structure was used to improve stability and synergistically enhance UV absorption of AVB. A novel AVB loaded ZnTi-CO3-LDH (AVB@ZnTi-LDH) material was synthesized by reconstruction method and the loading content (LC) was about 46.8% investigated by high-performance liquid chromatography (HPLC). A possible mechanism for the binding of AVB with the ZnTi-LDH surface was proposed. X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) calculations were used to confirm further the coordination between Zn on the layer and the oxygen atom of the carbonyl group of AVB. UV absorption and critical wavelength of AVB@ZnTi-LDH were superior to those of AVB and ZnTi-LDH precursors. Compared with pure AVB, the photodegradation rate was reduced from 15.06% to 4.06%. Especially in titanium dioxide, the decomposition rate was reduced from 29.75% to 7.92%. Furthermore, pure AVB often reacts with multivalent metal ions to induce an unpleasant color (light yellow to reddish brown), which is greatly mitigated with AVB@ZnTi-LDH. In this study, avobenzone was combined with hydrotalcite to prepare an organic-inorganic composite with excellent UV resistance and better stability, the composite has great promise for application in sunscreen cosmetics.
SnO2 is a potential anode material with high theoretical capacity for lithium-ion batteries (LIBs), however, its applications have been limited by the severe volume expansion during charging-discharging process. In this work, an inverse opal TiO2/SnO2 composite with an interconnect network nanostructure was designed to confine SnO2 nanoparticles in the porous TiO2. Due to this nanoconfinement structure, the volume expansion in the process was effectively alleviated, therefore the safety performance and cycling stability of the battery were effectively improved. At the same time, with a large number of microporous structures in the framework, the appearance of pseudocapacitance improves the rate performance and reversible capacity. In terms of electrochemical kinetics, its framework provides the connected path for charge migration, effectively reducing the charge transfer impedance, meanwhile, quantities of micropores in its skeleton could provide a smoother channel for lithium ions, thus greatly improving the diffusion rate of LIBs. The design of this nanostructure provides a new idea for the research of SnO2-based anode with effectively enhanced electrochemical performance, which is promising anode for practical application.
Aliphatic C(sp3)–H moieties are ubiquitous in numerous organic compounds. Direct functionalization of inert C(sp3)–H bonds is a powerful and straightforward approach for the efficient construction of diverse carbon–carbon or carbon–heteroatom bonds. Chelating group directed metal-catalyzed remote functionalization of readily available alkenes has emerged as an appealing strategy for rapidly accessing various value-added aliphatic molecules. With the aid of directing groups, various α-, β- and γ-functionalized alkanes could be synthesized smoothly with excellent regioselectivity. The preferred formation of a stable five- or six-membered metallacycle intermediate terminates the chain-walking at a specific methylene site, which serves as the driving force for excellent site-selective migratory functionalization. This review herein is aimed at summarizing the recent progress on the metal-catalyzed regiodivergent functionalization of unactivated alkenes by merging alkene isomerization and cross-coupling with the assistance of directing auxiliary. Last but not least, the current situations and future directions in this field are highlighted and discussed.
Antibiotic resistance poses a critical threat to human healthcare, largely driven by bacterial biofilms. These biofilms resist the immune system and antibiotics, rendering enclosed microbial cells 10–1000 times more antibiotic-resistant than planktonic cells, leading to severe infections. Therefore, there is an urgent need to develop innovative tools for investigating biofilm regulators and devising novel antibacterial strategies. In this study, we developed Cy-NEO-PA, a near-infrared (NIR) fluorescent probe responsive to penicillin G acylase (PGA), with bacteria-targeting ability. This probe was designed to visualize the influence of environmental factors on biofilm formation in Acinetobacter baumannii (A. baumannii). Our findings demonstrated that glucose suppressed PGA production, leading to enhanced biofilm formation, whereas phenylacetic acid (PAA) stimulated PGA production and inhibited biofilm formation in A. baumannii. These observations highlight the remarkable capability of Cy-NEO-PA to accurately measure PGA dynamics, shedding light on the critical role of PGA in biofilm development. Additionally, Cy-NEO-PA exhibited excellent biocompatibility, potent reactive oxygen species (ROS) generation, efficient photothermal conversion, and bacteria-targeting abilities, making it a promising agent for combating bacterial infections and promoting wound healing through photothermal (PTT)/photodynamic (PDT) therapy. These discoveries emphasize the significant role of PGA in antibacterial therapy and offer valuable insights for the design of effective strategies targeting PGA to combat biofilm-associated infections.
In 2023, The MOE Key Laboratory of Macromolecular Synthesis and Functionalization in Zhejiang University had achieved several important results in the five research directions. First, for controllable catalytic polymerization, a new silicon-centered organoboron binary catalyst was developed for copolymerization of epoxides, and a series of cooperative organocatalysts were proposed for ring-opening copolymerization of chalcogen-rich monomers. Second, with respect to microstructure and rheology, axially encoded metafiber demonstrated its capacity for integrating multiple electronics, while artificial nacre materials showed improved strength and toughness due to interlayer entanglement. Third, concerning separating functional polymers, interfacial polymerization was monitored via aggregation-induced emission, and vacuum filtration was applied to assist interfacial polymerization. Fourth, in terms of biomedical functional polymers, we designed antibacterial materials such as a novel quaternary ammonium salt that enables polyethylene terephthalate recycling and its antibacterial function, nanozyme-armed phage proved its efficiency in combating bacterial infection, and also transition metal nanoparticles showed capacities in antibacterial treatments. We also made achievements in biomedical materials, including polymeric microneedles for minimally invasive implantation and functionalization of cardiac patches, as well as ROS-responsive/scavenging prodrug/miRNA balloon coating to promote drug delivery efficiency. Besides, methods and mechanisms of RNA labeling has been developed. Fifth, about photo-electro-magnetic functional polymers, through-space conjugation was successfully manipulated by altering subunit packing modes, room-temperature phosphorescent hydrogels were synthesized via polymerization-induced crystallization of dopant molecules, and single crystals of both fullerene and non-fullerene acceptors were grown in crystallized organogel, with their photodetection performance further explored. The related works are reviewed in this paper.
Lithium–sulfur (Li–S) batteries are considered one of the most promising next-generation secondary batteries owing to their ultrahigh theoretical energy density. However, practical applications are hindered by the shuttle effect of soluble lithium polysulfides (LiPSs) and sluggish redox kinetics, which result in low active material utilization and poor cycling stability. Various copper-based materials have been used to inhibit the shuttle effect of LiPSs, owing to the strong anchoring effect caused by the lithiophilic/sulphilic sites and the accelerated conversion kinetics caused by excellent catalytic activity. This study briefly introduces the working principles of Li–S batteries, followed by a summary of the synthetic methods for copper-based materials. Moreover, the recent research progress in the utilization of various copper-based materials in cathodes and separators of Li–S batteries, including copper oxides, copper sulfides, copper phosphides, copper selenides, copper-based metal-organic frameworks (MOFs), and copper single-atom, are systematically summarized. Subsequently, three strategies to improve the electrochemical performance of copper-based materials through defect engineering, morphology regulation, and synergistic effect of different components are presented. Finally, our perspectives on the future development of copper-based materials are presented, highlighting the major challenges in the rational design and synthesis of high-performance Li–S batteries.
3d transition metal chalcogenides have attracted much attention due to their unique magnetic properties. Although various Cr, V, and Fe-based chalcogenides have been fabricated recently, the limited Curie temperature (TC) still hinders their practical application. Based on the structural and magnetic advantages of MFe2O4 and Fe3Se4, we developed a one-pot solution synthesis method for the fabrication of NiFe2Se4 nanostructures with structural continuity, to facilitate the investigation of their magnetic properties. Notably, the morphology of NiFe2Se4 can be controlled from nano-rods to nano-platelets by controlling the growth direction. The coercivity (HC) of NiFe2Se4 with nano-cactus structure exhibits a maximum of 12.77 kOe at 5 K. The coercivity of ferrimagnetic NiFe2Se4 nano-platelets can be further adjusted to 1.52 kOe at room temperature. These results show that the magnetic properties of NiFe2Se4 can be significantly modified by controlling their morphologies. We also extend the method to the synthesis of CoFe2Se4 nano-cactus with an ultrahigh coercivity of 17.85 kOe at 5 K. Obviously, the synthesis strategy and their excellent magnetic properties of MFe2Se4 have sparked interest in ternary transition metal selenides as potential hard magnetic materials.
Heterojunction engineering is recognized as a promising strategy to modulate the photocatalytic properties of semiconductors. Herein, lead-free Cs2CuBr4 perovskite quantum dots (PQDs) were confined in a mesoporous CuO framework and a p-n type S-scheme heterojunction of Cs2CuBr4/CuO (CCB/CuO) photocatalyst was fabricated. Experimental characterizations confirmed the effective confinement of the Cs2CuBr4 PQDs in the mesoporous CuO framework, which enabled intimate contact in the interface of CCB/CuO heterojunction, thus facilitating the interfacial charge migration and separation between p-type CuO and n-type Cs2CuBr4. Owing to the outstanding charge transport property and CO2 adsorption capacity, the developed CCB/CuO heterojunction exhibited remarkably enhanced photocatalytic CO2 conversion efficiency with an electron consumption rate (Relectron) of 281.1 µmol g−1 h−1, which was approximately 2.8 times higher than that of pristine Cs2CuBr4. These findings provide some insights into the rational engineering design of lead-free perovskite-based heterostructures for efficient photocatalytic CO2 conversion.
A facile visible-light-induced 1,2,3,5-tetrakis(carbazol-9-yl)-4,6-dicyanobenzene (4CzIPN) catalyzed four-component reaction of alkenes, quinoxalin-2(1H)-ones, P4S10 and alcohols has been developed at room temperature. This tandem reaction provides an efficient strategy for the construction of various phosphorodithioate-containing quinoxalin-2(1H)-ones with moderate to good yields by using air (dioxygen) as the green oxidant. Experimental studies revealed a radical process was involved in this photochemical reaction.
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