Fluorophore Label-Free Light-up Near Infrared Deoxyribonucleic Acid Nanosensor for Monitoring Extracellular Potassium Levels.

Fluorescent DNA nanosensors have been widely used due to their unique advantages, among which the near-infrared (NIR) imaging mode can provide deeper penetration depth and lower biological background for the nanosensors. However, efficient NIR quenchers require ingenious design, complex synthesis, and modification, which severely limit the development of NIR DNA nanosensors. Label-free strategies based on G-quadruplex (G4) and NIR G4 dyes were first introduced into in situ extracellular imaging, and a novel NIR sensing strategy for the specific detection of extracellular targets is proposed. The strategy avoids complex synthesis and site-specific modification by controlling the change of the NIR signal through the formation of a G4 nanostructure. A light-up NIR DNA nanosensor based on potassium ion (K+)-sensitive G4 chain PS2.M was constructed to verify the strategy. PS2.M forms a stable G4 nanostructure in the presence of K+ and activates the NIR G4 dye CSTS, thus outputting NIR signals. The nanosensor can rapidly respond to K+ with a linear range of 5-50 mM and has good resistance to interference. The nanosensor with cholesterol can provide feedback on the changes in extracellular K+ concentration in many kinds of cells, serving as a potential tool for the study of diseases such as epilepsy and cancer, as well as the development of related drugs. The strategy can be potentially applied to the NIR detection of a variety of extracellular targets with the help of functional DNAs such as aptamer and DNAzyme.

Surface change of microplastics in aquatic environment and the removal by froth flotation assisted with cationic and anionic surfactants.

Microplastics (MPs) are increasingly released into the environment due to the widespread usage and improper management of plastics. Considerable research efforts have been devoted to the remediation of MPs. Froth flotation has been demonstrated as an effective method to remove MPs in water and sediment. However, there is a lack of knowledge on the regulation of the hydrophobicity/hydrophilicity of MPs surfaces. We found that exposure to the natural environment resulted in the increased hydrophilicity of MPs. The flotation efficiencies of polyvinyl chloride (PVC), polypropylene (PP), polystyrene (PS), and polyethylene glycol terephthalate (PET) MPs decreased to zero after six months of natural incubation in rivers. According to various characterizations, the hydrophilization mechanism is mainly correlated with surface oxidation and the deposition of clay minerals. Inspired by surface wettability conversion, we applied surfactants (collectors) to enhance MPs hydrophobicity and flotation efficiency. Anionic sodium oleate (NaOL) and cationic dodecyl trimethyl ammonium chloride (DTAC) were used to regulate surface hydrophobicity. The effects of collector concentration, pH, conditioning time, and metal ions on MPs flotation were thoroughly elucidated. Characterizations and adsorption experiments were performed to describe the heterogeneous adsorption of surfactants on MPs surfaces. The interaction between surfactants and MPs was explained through density functional theory (DFT) simulations. The dispersion energy between hydrophobic hydrocarbon chains attracts collectors on the MPs surface, and the collector molecules wrap and laminate to MPs surfaces. Flotation using NaOL exhibited a higher removal efficiency, and NaOL was environmentally friendly. Subsequently, we investigated the activation of Ca2+, Fe3+, and Al3+ to further improve the collecting efficiency of NaOL. Under the optimized conditions, MPs in natural rivers could be removed by froth flotation. This study shows the great promise of froth flotation for the application of MPs removal.

Rational design of cobalt sulfide anchored on nitrogen-doped carbon derived from cyanobacteria waste enables efficient activation of peroxymonosulfate for organic pollutants oxidation.

With the increasing of eutrophication in water body, algae blooms have become one of the global environmental problems. The cyanobacteria waste has placed a severe burden on the environment and transforming cyanobacteria into functional materials may be a wise approach. Herein, cobaltous sulfide/nitrogen-doped biochar (N-BC/CoSx) composite was synthesized by pyrolysis of cyanobacteria waste. The N-BC/CoSx showed excellent performance in peroxymonosulfate (PMS) activation for enrofloxacin (ENR) degradation, which could remove more than 90% ENR within 60 min. The influencing factors of pH and catalyst dosage on ENR removal efficiency were studied. The N-BC/CoSx showed good recyclability in the cycle runs. The radicals (O2•-, OH andSO4•-) and the non-radical species (charge transfer and 1O2) were generated in the ENR degradation. The cycle of Co(II)/Co(III) m ay contribute to the radical generation process. This work proved that metal sulfide modified cyanobacteria biochar has a specific application value in water pollution control and provides a new method for resource utilization of cyanobacteria.

Self-assembly of DNA nanospheres with controllable size and self-degradable property for enhanced antitumor chemotherapy.

Controllable size, self-degradability and targeting property are important for a precise improvement of anticancer effects and reduction of side effects of drug vehicles. Here, a series of DNA nanospheres with controllable size and self-degradation ability were constructed through the hybridization of two i-motif strands and two linker strands for targeted cancer therapy. DNA nanospheres with different sizes were fabricated by regulating the linker sequence, and their pH-responsive self-degradation property was realized by the introduction of the i-motif strand. Moreover, the ZY11 aptamer was introduced to endow the DNA nanospheres with targeting property toward SMMC-7721 cancer cells. The results revealed that the appropriate size of DNA nanospheres (80 nm) highly promoted the internalization by mammalian cells. The results of DLS, AFM and CD spectra showed that the DNA nanospheres were stable in a physiological environment but they self-degraded in a slightly acidic environment due to the existence of the i-motif strand. Moreover, the fluorescence of DOX@AP-NSs2 was triple at pH = 5.0 than at pH = 7.4, which further confirmed the pH-responsive drug release performance. The above results proved that the use of DOX@AP-NSs2 is a promising approach to accelerate the rapid release of drugs into the tumors and avoid drug leakage into the normal tissue. The results at a cellular level and in vivo confirmed the pH-responsive targeted antitumor effect. Hence, the novel DNA nanospheres with controllable size and self-degradable property represent a potential tool for targeted drug delivery and cancer therapy.

Anti-tumor immunity and ferroptosis of hepatocellular carcinoma are enhanced by combined therapy of sorafenib and delivering modified GO-based PD-L1 siRNAs.

Programmed cell death receptor ligand 1 (PD-L1)/PD-1 signaling has been exploited to design inhibitors that deliver promising clinical outcome albeit with limited efficacy. Herein, we prepare graphene oxide (GO)-PEI-PEG with low cytotoxicity and long stability and GO-PEI-PEG delivers PD-L1 siRNAs to hepatocellular carcinoma (HCC) cells by the endocytosis-lysosome pathway. The functional GO-PEI-PEG/PD-L1 siRNAs decrease PD-L1 and PD-1 abundance, increase pro-inflammation cytokine IFN-γ and TNF-α release, and improve the proliferation activity of Jurkat T cells. Since GO-PEI-PEG targets the mouse liver effectively, the intrahepatic tumors in C57BL/6 mice are treated with GO-PEI-PEG/Pd-l1 siRNAs via the tail vein, resulting in shrinkage of the HCC tumors and boosting the anti-tumor efficacy in combination with oral sorafenib. A single treatment improves the total CD3+ and cytotoxic CD8+ T cell infiltration in the HCC tumor tissues and even spleen and upregulates the expression of Perforin, Gzmb, Ifng, Il-1b and Tnfa in the tumors after the combined treatment. Both the single and combined treatments enhance reactive oxygen species (ROS) accumulation, and improved HCC ferroptosis. The results suggest that GO-PEI-PEG delivered PD-L1 siRNAs combined with oral sorafenib can activate the adaptive immunity and tumor ferroptosis and reveal an effective therapy to treat advanced HCC patients.

Fabrication, GSH-responsive drug release, and anticancer properties of thioctic acid-based intelligent hydrogels.

Injectable hydrogels are potential local drug delivery systems since they contain plenty of water and soft like biological tissues. Such hydrogels could be injected directly into the tumor site where the drug is released under the tumor microenvironment. However, drug loaded hydrogels for cancer treatment based on lipoic acid (natural small molecule) have not been exploited. Here, a novel poly(lipoic acid)-poly(ethylene glycol) (PEG-PTA) hydrogels were prepared through a two-step reaction. The hydrogels contained disulfide bonds, so they could be degraded via the thiol exchange reaction with the abundant GSH in the tumor microenvironment, and subsequently release the drug. The results in vitro and at cellular level showed that the hydrogels were degraded and released the drugs only in the presence of GSH. Therefore, the injectable GSH-responsive hydrogels are promising to be served as an intelligent drug delivery system for cancer treatment.

Waste coal cinder catalyst enhanced electrocatalytic oxidation and persulfate advanced oxidation for the degradation of sulfadiazine.

Waste coal cinder, a kind of waste cinder discharged from coal combustion of thermal power plants, industrial and civil boilers, and other equipment, was rich in metal oxides with catalytic activity. In this work, waste coal cinder was used to enhance electrochemical coupling peroxymonosulfate (PMS) advanced oxidation degradation of sulfadiazine (SD). The surface morphology, elemental composition, and electrocatalytic activity of waste coal cinder were characterized by various characterization instruments. The results show that compared with simple electrocatalytic oxidation, electrocatalytic oxidation + waste coal cinder and electrocatalytic coupled persulfate oxidation, electrocatalytic oxidation + PMS advanced oxidation + waste coal cinder has the largest removal efficiency (99.95%) and mineralization rates (90.16%) of SD in 90 min, indicating that the introduction of waste coal cinder greatly increases the degradation efficiency. •OH and SO4-• were detected during the process of degradation. The optimal degradation process parameters were explored through different voltage, pH, plate spacing, aeration flow rate, potassium peroxymonosulfate sulfate complex salt dose, and Na2SO4 dosage. Cycling experiments show waste coal cinder has good structural stability. Through the analysis of triple quadrupole liquid chromatography-mass spectrometry (LC-MS), we put forward three possible ways of SD degradation. This research will provide a novel vision for water treatment.

Bimetallic modified halloysite particle electrode enhanced electrocatalytic oxidation for the degradation of sulfanilamide.

The treatment of antibiotics wastewater by electrocatalytic oxidation has attracted much attention. In the paper, a novel halloysite bimetallic (HLS-Cu-Mn) particle electrode material was prepared and a bench-scale electrocatalytic reaction tank was designed. A three-dimensional electrocatalytic oxidation reactor composed of HLS-Cu-Mn and a bench-scale electrocatalytic reaction tank was used to degrade Sulfanilamide (SA) wastewater. Characterization of the synthesized material was conducted with Scanning electron microscopy (SEM), X-ray polycrystalline powder diffractometer (XRD), X-ray photoelectron spectroscopy (XPS), and Brunauer-Emmett-Teller (BET). The electron spin resonance spectroscopy test results confirmed that HLS-Cu-Mn produced a large number of •OH. The electrochemical workstation confirmed that HLS-Cu-Mn had strong electrocatalytic activity and repolarization ability. Under the optimum preparation conditions and degradation process parameters, the removal efficiency of SA and TOC was 99.84% and 88.95% respectively. The method also has good degradation efficiency for aniline, phenol, herbicides, antibiotics, and dyeing wastewater. It was found that 4 main intermediates appeared in the degradation process by Ultra-high performance liquid chromatography/triple tandem quadrupole mass spectrometry (LC-MS). In sum, it was believed that this work provides a new vision and idea for water treatment.

Discovery of the Rnase activity of CRISPR-Cas12a and its distinguishing cleavage efficiency on various substrates.

We, herein, indicated for the first time the Rnase activities of LbCas12a on linear ssRNA above 11 bases, and hairpin RNA substrates. Meanwhile, the LbCas12a bound to ssDNA or ssRNA exhibited different cleavage efficiencies on various substrates, including short ssDNA, hairpin DNA, linear ssRNA and hairpin RNA. With hairpin DNA as a reporter, we attained a detection limit of 5 pM and 50 pM for the ssDNA and ssRNA targets, respectively. We believe that these findings will pave a new avenue for expanding the reporter toolbox for Cas12a-based diagnostics in biosensing and biochemistry.

Capsule-like molecular imprinted polymer nanoparticles for targeted and chemophotothermal synergistic cancer therapy.

Selective cancer cell targeting, controlled drug release, easy construction and multiple therapeutic modalities are some of the desirable characteristics of drug delivery systems. We designed and built simple capsule-like molecular imprinted polymer (MIP)-based nanoparticles for targeted and chemo-photothermal synergistic cancer therapy. Using dopamine (DA) as functional monomer, cross-linking agent as well as photo-thermal agent, ZIF-8 (zeoliticimidazolate framework-8) as drug carrier, epitope of EGFR (epidermal growth factor receptor) as template molecules, molecular imprinted polymer (MIP) drug carrier was constructed. The ability of MIP layer to bind to EGFR epitope endowed the MD (DOX@MIP) particles to recognize EGFR-overexpressing cancer cells, while the pH-responsiveness and photothermal conversion ability of PDA (polydopamine) achieved chemo-photothermal synergistic effects upon NIR irradiation. Taken together, the MD nanoparticles integrated cancer cell targeting recognition, intelligent drug release, biocompatibility and chemo-photothermal effects, and is therefore a promising tool for targeted cancer therapy with minimal toxicity to normal cells, as well as tumor imaging.

O, S-Dual-Vacancy Defects Mediated Efficient Charge Separation in ZnIn2S4/Black TiO2 Heterojunction Hollow Spheres for Boosting Photocatalytic Hydrogen Production.

Defective ZnIn2S4 nanosheets/mesoporous black TiO2 heterojunction hollow spheres (H-ZIS/b-TiO2) are prepared through hydrothermal and surface low-temperature hydrogenation strategies, which show broad-spectrum response and excellent charge separation efficiency. This H-ZIS/b-TiO2 flower-like heterojunction hollow spheres with a narrow band gap of ∼1.88 eV expand the light response to visible light and show excellent photocatalytic hydrogen evolution rate (278 µmol h-1 50 mg-1) under visible-light irradiation, which is 1.5 times as high as that of ZnIn2S4/black TiO2 heterojunction hollow spheres (ZIS/b-TiO2) (181 µmol h-1 50 mg-1). The excellent photocatalytic performance is due to the formation of O, S dual vacancies in b-TiO2 and H-ZIS providing more active sites for photocatalytic reaction and improving the charge separation efficiency, heterojunctions promoting transport of photogenerated carriers, and the hollow structure increasing light utilization by reflecting light. The novel heterojunction hollow sphere with high performance has broad application prospects in the field of energy.

Current methods and prospects of coronavirus detection.

SARS-COV-2 is a novel coronavirus discovered in Wuhan in December 30, 2019, and is a family of SARS-COV (severe acute respiratory syndrome coronavirus), that is, coronavirus family. After infection with SARS-COV-2, patients often experience fever, cough, gas prostration, dyspnea and other symptoms, which can lead to severe acute respiratory syndrome (SARS), kidney failure and even death. The SARS-COV-2 virus is particularly infectious and has led to a global infection crisis, with an explosion in the number of infections. Therefore, rapid and accurate detection of the virus plays a vital role. At present, many detection methods are limited in their wide application due to their defects such as high preparation cost, poor stability and complex operation process. Moreover, some methods need to be operated by professional medical staff, which can easily lead to infection. In order to overcome these problems, a Surface molecular imprinting technology (SM-MIT) is proposed for the first time to detect SARS-COV-2 virus. For this SM-MIT method, this review provides detailed detection principles and steps. In addition, this method not only has the advantages of low cost, high stability and good specificity, but also can detect whether it is infected at designated points. Therefore, we think SM-MIT may have great potential in the detection of SARS-COV-2 virus.