Latest ArticlesWound healing in diabetic patients presents significant challenges due to heightened risks of bacterial infection, elevated glucose levels, and insufficient angiogenesis. Nanozymes are widely employed for wound healing, but most current nanozyme systems exhibit only moderate activity limited by incompatible reaction microenvironments including pH and hydrogen peroxide (H2O2) concentration. Herein, a glucose-activated nanozyme hydrogel was developed using bovine serum albumin (BSA)-modified gold nanoparticles (Au NPs) attached to a two-dimensional (2D) metal-organic framework (MOF) (Cu-TCPP(Fe)@Au@BSA) by an in situ growth method. The Au NPs function as a glucose oxidase (GOx)-like enzyme, converting glucose to gluconic acid and H2O2, triggering the peroxidase (POD)-like activity of Cu-TCPP(Fe) to produce hydroxyl radicals (•OH), effectively eliminating bacteria. Additionally, the modification of BSA reduces the Au NP size, enhancing enzyme activity. Both in vitro and in vivo tests demonstrate that this nanozyme hydrogel can be activated by the microenvironment to lower blood glucose, eliminate bacterial infections, and promote epithelial formation and collagen deposition, thus accelerating diabetic wound healing effectively. The multifunctional nanozyme hydrogel dressing developed in this study presents a promising therapeutic approach to enhance diabetic wound healing.
Developing BiVO4 photoanode with efficient carrier transfer and fast water oxidation kinetics is the permanent pursuit to achieve the state-of-art solar-driven photoelectrochemical (PEC) water splitting. The capacity to increase the PEC activity of BiVO4 by loading oxygen evolution co-catalysts (OECs) has been proven, however it suffers from sluggish charge carriers dynamics brought on by the complicated interface between BiVO4 and OECs as well as poor long-term durability. Herein, we connected OECs (NiFeOx) and photoanode with a Al-O bridge for bettering the PEC performance of BiVO4. The Al-O bridge served as a channel to extract hole from BiVO4 to NiFeOx, thus boosting charge carriers′ separation and preventing BiVO4 from photo-corrosion. The Al-O bridging photoanode (NiFeOx/Al2O3/BiVO4) demonstrated a high photocurrent density of 5.87 mA/cm2 at 1.23 V vs. RHE and long-term photostability in comparison to NiFeOx/BiVO4 photoanode. This study proposes a unique technique to boost charge carriers′ separation between BiVO4 and OECs for high-efficiency solar-driven PEC water splitting.
A highly sensitive zinc ion fluorescent probe NOD-NY with controlled release of nitric oxide was designed, synthesized and used for tracking intracellular zinc ions in living A549 cells. NOD-NY was prepared from naphthalimide as the fluorophore and N,N-bis(2-pyridylmethyl)amine as the zinc ion recognition receptor, the amide N atom of the naphthalimide was connected to n-butylamine. Under the irradiation of ultraviolet light, NOD-NY can quantitatively release nitric oxide and generate a highly sensitive zinc ion probe Zn-HN, accompanied by a red-shift process of maximum ultraviolet absorption from 350 nm to 450 nm. Upon addition of Zn2+ to the solutions of Zn-HN, a remarkable fluorescence enhancement was observed, which could be attributed to the photo-induced electron transfer (PET) mechanism. By replaced the n-butylamine on NOD-NY with diethylene glycolamine or triphenylphosphine structures, NOD-AY with good biocompatibility and NOD-BY that can target mitochondria were obtained respectively. In addition, the nitric oxide released by NOD-NY enriched in lysosome can diffuse into mitochondria. The released nitric oxide can stimulate metallothionein to release zinc ions, and the light-induced in situ generated zinc ion probe Zn-HN can have a highly sensitive fluorescence response to free zinc ions in living A549 cells.
Pt(Ⅱ)−salophen complexes (S-1~S-4) and 9,10-diphenylanthracene (DPA) tethering pillar[5]arene derivatives (A-1 and A-2) were synthesized to act as sensitizers and annihilators for triplet-triplet annihilation upconversion (TTA-UC), respectively. It turned out that the pyridine cation served as a mask for the excited state of the sensitizer, the triplet states of S-2 and S-3 were significantly quenched by photo-induced electron transfer (PET) with phosphorescence quantum yield quenched from 24.4% for S-4 to 9.3% for S-3, and therefore, both S-2 and S-3 led to negligible UC emissions when traditional annihilator DPA was used as the annihilator. Delightfully, when supramolecular annihilator A-1 and A-2 were employed to include the pyridine cation, PET was significantly inhibited and the triplet states of the sensitizers were activated, TTA-UC emission was therefore boosted. The UC quantum yield of A-2/S-3 system was up to 130 times higher than that of DPA/S-3 system, and the UC emission was switchable by the addition of competitive guests.
A decomposable and sono-enzyme co-triggered nanoparticle (pTCP-CR NP) with “AND gate” logic was synthesized, combining a meso‑carboxyl-porphyrin-based sonosensitizer (5,10,15,20-tetrakis(carboxyl)porphyrin, TCP) and a thiophenyl-croconium (2,5-bis[(2-(2-(2-hydroxyethoxy)ethoxy)ethyl-4-carboxylate-piperidylamino)thiophenyl]-croconium, CR) via ester groups. TCP releases carbon monoxide (CO) under ultrasound (US) irradiation, offering both sonodynamic and gas therapy. CR decomposes into stronger reactive oxygen species (ROS) compared to oxygen-based radicals. The Förster resonance energy transfer (FRET) effect between TCP and CR inhibits ROS and CO generation until triggered by tumor cell overexpressed carboxylesterase (CEs). pTCP-CR NPs “AND gate” logic ensures activation only in the presence of both CEs and US, targeting tumor cells while safety in normal tissues. The ROS and CO generation abilities, as well as the releasing of SO4•− have been systemically examined. pTCP-CR can be thoroughly decomposed into low-toxic molecules post the treatment, showing the safety with negligible phototoxic reactions. In vivo anti-cancer therapy has been evaluated using mice bearing hepatocellular carcinoma.
ZnIn2S4, a typical n-type semiconductor, has received intensive attention due to its suitable bandgap, excellent visible light absorption performance, and simple and flexible preparation methods. However, its application is curbed by photo-generated carrier recombination and photo corrosion. Although constructing S-scheme heterojunctions by combining ZnIn2S4 with other semiconductors can solve these problems, the photocatalytic activity of S-scheme heterojunctions can be further improved. Therefore, this short review summarizes modification strategies of ZnIn2S4-based S-scheme heterojunctions. This article also introduces the concept, design principles, and characterization methods of ZnIn2S4-based S-scheme heterojunction. Finally, current challenges and future research focuses related to ZnIn2S4-based S-scheme heterojunctions are discussed and summarized, including the utilization of advanced in-situ characterization techniques to further illuminate the photocatalytic mechanism, the DFT-assisted design of catalysts to increase the selectivity of products during photocatalytic CO2 reduction, and extending the photo-response of ZnIn2S4-based S-scheme heterojunction to near-infrared range, etc.
Black phosphorus (BP), as a rising star of 2D nanomaterials has drawn considerable attention in cancer therapy. However, the poor stability under ambient conditions limits their practical applications. Herein, a multiple supramolecular assembly composed of adamantane-modified hyaluronic acid (HAADA), ferrocene-modified cinnamaldehyde (Fc-CA), guanidinium-functionalized β-cyclodextrin (Guano-CD), and black phosphorus (BP) nanosheets was successfully fabricated through cooperative host-guest and electrostatic interactions. Owing to the cooperative contribution of these building blocks, the obtained supramolecular assembly simultaneously possesses multiple functions including excellent stability, good biocompatibility and targeting property, and a high inhibition effect toward cancer cells. We believe that this work might provide new insights into designing a new generation of cancer theranostic protocols for potential clinical applications.
A strategy for copper-catalyzed and biphosphine ligand controlled boracarboxylation of 1,3-dienes and CO2 with 3,4-selectivity was developed. The CuCl coupled with DPPF (1,1′-bis(diphenylphosphino)ferrocene) was assigned to be the best catalyst, with 84% yield and exclusive 3,4-selectivity. The ligand effect on both catalytic activity and regioselectivity of boracarboxylation was disclosed, which is rarely reported in any copper catalyzed boracarboxylation. The borocupration process is revealed to be a vital step for the biphosphine participated boracarboxylation of 1,3-dienes with CO2. The minimal substrate distortion occurring in 3,4-borocupration favors the 3,4-regioselectivity of boracarboxylation. The “pocket” confinement and suitable βn (92°–106°) of bisphosphine ligands are demonstrated to be in favour of the interaction between LCu-Bpin complex (the catalytic precursor) and 1,3-diene substrate to decrease their interaction energy ∆Eint(ζ) in 3,4-borocupration, thus promoting the 3,4-boracarboxylation.
Although inductively coupled plasma mass spectrometry (ICP-MS) retains high sensitivity and has been intensively used for the measurement of 99Tc, it usually suffers from tedious, expensive, and time-consuming sample pretreatments due to the isobaric interferences from 99Ru and 98Mo1H. Herein, capillary electrophoresis (CE) was applied as sample introduction system for the sensitive, and interference-free determination of 99TcO4- from RuO4-, and MoO42- by ICP-MS with a simple sample treatment. Compared to the conventional methods, the hyphenated CE-ICP-MS avoids the use of expensive separation resins and reduces the consumption of mineral acid, representing a simpler, more efficient and environmentally benign approach. Moreover, the proposed method exhibits higher accuracy compared with the mathematical correction method using the natural isotope ratio of 99Ru and 101Ru, and significantly reduces sample consumption and the amount of waste, thus remarkably alleviating the radioactive exposure to operators and the pressure of radioactive waste treatment. Under the optimized conditions, the detection limits of 25 µg/L and 0.06 µg/L were obtained for RuO4- and ReO4- (Tc was replaced by Re), respectively, with relative standard deviation (RSD) lower than 5%. In addition, efficient recoveries of RuO4-, ReO4-, and 99TcO4- from simulated Hanford site groundwater were achieved. The method is expected to be a promising candidate for sensitive and accurate analysis of 99Tc from contaminated environmental samples.
A general process for the construction of azaaryl alkanes was achieved by employing the photoredox/palladium dual catalysis under mild visible light irradiation. The palladium catalyst ligated with a diphosphamide ligand exhibited high effectiveness in facilitating the modular three-components transformation. Furthermore, the cascade transformation was not restricted to constructing tertiary carbon centers; it also encompassed the synthesis of more challenging quaternary carbon centers with sixteen representative azaarene-derived substrates as reactants. In addition, alkyl 1,4-dihydropyridines (DHP), alkyl BF3K, and alkyl carboxylic acids were identified as precursors for alkyl radicals. Mechanistic investigations revealed the involvement of two different active benzylic nucleophiles in the cascade transformation. One is azabenzylic radical, which generate the terminal product through an “inner sphere” reductive elimination process. The other is azabenzylic anions, generated through visible light induced radical anion cross-over, leading to the formation of terminal products via an “outer sphere” reaction pathway. The efficiency of current modular transformation was also demonstarted by the concise of oliceridine, a prominent USFDA drug for pain management.
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