Latest ArticlesThe Z-scheme heterostructure for photocatalyst can effectively prolong the lifetime of photogenerated carriers and retain a higher conduction/valence band position, promoting the synergistic coupling of photocatalysis and peroxymonosulfate (PMS) activation. In order to fully utilize the luminous energy and realize the efficient activation of PMS, this work achieved successful construction of NiCo2O4/BiOCl/Bi24O31Br10 ternary Z-scheme heterojunction by simultaneously synthesizing BiOCl and NiCo2O4 with NiCl2 and CoCl2 as the precursors. The intercalated BiOCl could serve as a carrier migration ladder to further achieve the spatial separation of electron-hole pairs, so that the oxidation and reduction processes separately occurred in different regions. Compared with the reported catalysts, the as-prepared composites exhibited the enhanced removal efficiency for tetracycline hydrochloride (TCH) in the visible light/PMS system, with a degradation efficiency of 85.30% in 2 min, and possessed good stability. Z-scheme heterojunction was shown to be beneficial for maximizing the superiority of photo-assisted Fenton-like reaction system. The experimental and characterization results confirmed that both non-radicals (1O2) and radicals (SO5•− and SO4•−) were involved in the reaction process and the SO5•− generated by the oxidation of PMS played a crucial role in the TCH degradation. The possible reaction mechanism was finally proposed. This study provided new insight into the Z-scheme heterostructure to promote the photo-assisted Fenton-like reaction.
During the past few years, the construction of BODIPY-based supramolecular fluorescent metallacages through coordination-driven self-assembly has gained increasing interest due to their unique photophysical properties and applications in catalysis, sensing, and bioimaging. In consideration of the rapid development of this field, it is time to summarize recent developments involving BODIPY-based metallacages. In this review, a comprehensive summary of the construction of BODIPY-based metallacages as well as their photophysical properties and applications will be presented.
The strong intrinsic Coulomb interactions of Frenkel excitons in crystalline carbon nitride (CCN) greatly limits their dissociation into electrons and holes, resulting in unsatisfactory charges separation and photocatalytic efficiency. Herein, we propose a strategy to facilitate excitons dissociation by molecular regulation induced built-in electric field (BIEF). The electron-rich pyrimidine-ring into CCN changes the charge density distribution over heptazine-rings to induce BIEF between melon chains. Such BIEF is sufficient to overcome the considerable exciton binding energy (EBE) and reduce it from 38.4 meV to 16.4 meV, increasing the excitons dissociation efficiency (EDE) from 21.5% to 51.9%. Our results establish a strategy to facilitate excitons dissociation through molecular regulation induced BIEF, targeting the intrinsic high EBE and low EDE of polymer photocatalysts.
Nitric oxide (NO) gas therapy has been regarded as a promising strategy for cancer treatment. However, its therapeutic efficiency is still unsatisfying due to the limitations of monotherapy. Previous preclinical and clinical studies have shown that combination therapy could significantly enhance therapeutic efficiency. Herein, a graphene oxide (GO)-L-arginine (L-Arg, a natural NO donor) hybrid nanogenerator is developed followed by surface functionalization of soybean lecithin (SL) for synergistic enhancement of cancer treatment through photothermal and gas therapy. The resultant GO-Arg-SL nanogenerator not only exhibited good biocompatibility and excellent endocytosis ability, but also exhibited excellent photothermal conversion capability and high sensitivity to release NO within tumor microenvironment via inducible NO synthase (iNOS) catalyzation. Moreover, the produced hyperthermia and intracellular NO could synergistically kill cancer cells both in vitro and in vivo. More importantly, this nanogenerator can efficiently eliminate tumor while inhibiting the tumor recurrence because of the immunogenic cell death (ICD) elicited by NIR laser-triggered hyperthermia and the immune response activation by massive NO generation. We envision that the GO-Arg-SL nanogenerator could provide a potential strategy for synergistic photothermal and gas therapy.
The exploration of novel photo/thermal-responsive nonvolatile memorizers will be beneficial for energy-saving memories. Herein, new <110> -oriented perovskites using single template melamine, i.e., [(MLAI-H2)(PbX4)] (X = Br (α-1), Cl (α-2), MLAI = melamine) have been prepared and their structures upon irradiation of visible light have been investigated. They have been fabricated as nonvolatile memory devices with structures of ITO/[(MLAI-H2)(PbX4)]/PMMA/Ag (device-1: X = Br, device-2: X = Cl), which can exhibit unique visible light-triggered binary nonvolatile memory performances. Interestingly, the silent or working status can be monitored by visible chromisms. Furthermore, the light-triggered binary resistive switching mechanisms of these ITO/[(MLAI-H2)(PbX4)]/PMMA/Ag memory devices have been clarified in terms of EPR, fluorescence, and single-crystal structural analysis. The presence of light-activated traps in <110> -oriented [(MLAI-H2)(PbX4)] perovskites are dominated in the appearance of light-triggered resistive switching behaviors, based on which the inverted internal electrical fields can be established. According to the structural analysis, the more distorted PbX6 octahedra, higher corrugated <110> -oriented perovskite sheets, and more condensed organic-inorganic packing in Br-containing perovskite are beneficial for the stabilization of light-activated traps, which lead to the better resistive switching behavior of device-1. This work can pave a new avenue for the establishment of novel energy-saving nonvolatile memorizers used in aerospace or military industries.
Poly(ethylene glycol)-poly(lactic acid) block copolymer (PEG-PLA) is one of the most widely used biomedical polymers in clinical drug delivery owing to its biocompatibility and biodegradability. However, endowing PEG-PLA micelles with high drug loading, self-assembly stability and fast intracellular drug release is still challenging. Redox-responsive diblock copolymers (MPEG-SS-PMLA) of poly(ethylene glycol) and phenyl-functionalized poly(lactic acid) with disulfide bond as the linker are synthesized to prepare PLA-based micelles that demonstrate excellent colloidal stability and high Ru loading. Notably, MPEG-SS-PMLA achieved a remarkably high Ru loading efficiency of 84.3% due to the existence of strong π-π stacking between phenyl and Ru complex. MPEG-SS-PMLA exhibited good colloidal stability in physiological condition but quickly destabilized by reductive tumor microenvironment. Interestingly, about 74% of Ru complex was released under 10 mmol/L GSH concentration. Ru-loaded MEPG-SS-PMLA showed efficient delivery and release of Ru complex into MCF-7 cancer cells, achieving enhanced in vitro and in vivo antitumor activity of photodynamic therapy. This feasible functionalization method of MPEG-PLA has appeared to be a clinically viable platform for controlled delivery therapeutic agents and enhanced phototherapy.
The regulation of the basic properties of atom-economic catalysts at the atomic scale and atomic-level insights into the underlying mechanism of catalysis are less explored. We engineer the surface of vertical immobilized MoS2 on dispersible TiO2 nanofibers via atomic subtraction to precisely manipulate active sites at the atomic level. The photocatalytic performances of TiO2@MoS2 after H2 reduction towards the hydrogen production under visible light irradiation (> 420 nm) are about 4 times that of TiO2@MoS2 before H2 reduction. Importantly, the enhanced stability of TiO2@MoS2 lasts for at least 30 h. Promising catalytic activity that is attributed to omnidirectional exposed active sites located defects, edges, corners that are transformed from the subtractive atomic sites could be exhumed comprehensively. This work will provide an intriguing and effective approach on tuning electronic structures for optimizing the catalytic activity at the atomic level by atom elimination strategy. To get rid of a few atomics on the surface of atomically-thin MoS2 nanosheet could be a prudent avenue for enabling the basal plane of MoS2 catalytically active.
Development of sensitive and accurate methods for sialic acid (SA) determination is of great significance in early cancer diagnosis. Here, a colorimetric-assisted Photoelectrochemical (PEC) sensor was constructed for SA detection based on the two pairs of cis-diol groups in SA molecule. With the specific recognition of SA via the two pairs of cis-diol groups, the prepared gold-modified Bi2S3 (Au NPs@Bi2S3) and metal organic framework (Au@PCN-224) were introduced to the electrode and formed a sandwich structure. Based on the properties of inert electroconductivity and nanozyme of the PCN-224, dual-readout of photocurrent and visualization was achieved with the presence of 3, 3′, 5, 5′-tetramethylbenzidine (TMB). Moreover, to intensify the visualization signal, Ce3+ was employed as the mediator to boost the catalysis capability by transferring energy from PCN-224 surface to the whole system. With the unique SA recognition and the mediation of Ce3+, both the photocurrent and the visualization signals sensitively responded with the SA concentration linearly. The present method showed greatly high sensitivity, selectivity and accuracy for SA detection with a limit of detection of 1.44 µmol/L and a wide linear range of 5–1000 µmol/L. This method provided a new promising platform for SA detection and a potential strategy for design of novel biosensors with dual-model readout.
A variety of luminol derivatives with N- and O-substitution have been synthesized with broad functional group tolerance. O-esterification has been demonstrated for the first time as a promising way to prepare enhanced CL reagents for sensing hemin, bloodstain and horseradish peroxidase (HRP). The most effective analogue with a deuterated acetyl group exhibited greater potential than luminol for bloodstain imaging and HRP imaging in western blotting (WB). In addition, O-etherification can greatly suppress CL signal that has been applied to design a CL probe for β-glucosidase (β-Glu). This study offers important and useful information regarding the luminol modification and shows great potential to use O-substituted analogues for enhanced CL analysis.
Devising a desirable adsorbent for efficiently selective capture of Ag(Ⅰ) from wastewater has attracted much attention but faced with huge challenges. Herein, a novel linear o-phenanthroline-based polymer l-PRL was prepared via chemical oxidative polymerization for the adsorption of Ag(Ⅰ). The maximum adsorption capacity for Ag(Ⅰ) by l-PRL is 325.8 mg/g at pH 0. In addition, l-PRL owes ascendant selectivity for Ag(Ⅰ) from aqueous solutions containing various interfering metal ions of Pb(Ⅱ), Co(Ⅱ), Ni(Ⅱ), Cd(Ⅱ) and Fe(Ⅲ). Multiple characterizations of FT-IR and XPS uncover that the N groups on l-PRL act as adsorption sites to coordinate with Ag(Ⅰ). Density functional theory (DFT) calculations further evidence the mechanism that l-PRL is provided with the admirable adsorptivity and selectivity for Ag(Ⅰ). It is mainly attributed to the most stable complexes of l-PRL with Ag(Ⅰ), which possesses shortest Ag-N bond length compared with other heavy metal ions. Furthermore, 93.5% of initial adsorption capacity is reserved after four continuous regeneration cycles, indicating that l-PRL is equipped with superior recyclability and durability, and l-PRL is capable of removing Ag(Ⅰ) in low-concentration actual Ag(Ⅰ)-containing wastewater completely. This study shed light on the rational design of polymer adsorbents and in-depth insight into selective removal of aqueous Ag(Ⅰ).
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