Latest ArticlesAromatic compounds such as phenols presented widely in coal chemical industry wastewater (CCW) render the treatment facing great challenge due to their biorefractory characteristics and potential risks to the environment and human health. Ozone-based advanced oxidation processes show promising for these pollutants removal, but the mineralization via ozonation alone is unsatisfactory and not cost-effective. Herein, a hybrid peroxi-coagulation/ozonation process (denoted as PCO) was developed using sacrificial iron plate as an anode and carbon black modified carbon felt as cathode in the presence of ozonation. An enhanced phenol removal of ~100% within 20 min and phenol mineralization of ~80% within 60 min were achieved with a low energy consumption of 0.35 kWh/g TOC. In this novel process, synergistic effect between ozonation and peroxi-coagulation was observed, and beside O3 direct oxidation, peroxone played a dominant role for phenol removal. In the PCO process, the hydrolyzed Fe species enhanced the generation of reactive oxygen species (ROS), while •OH was dominantly responsible for pollutant degradation. This process also illustrated high resistance to high ionic strength and better performance for TOC removal in real wastewater when compared with ozonation and peroxi-coagulation process. Therefore, this process is more cost-effective, being very promising for CCW treatment.
NaClO has been widely used to restore membrane flux in practical membrane cleaning processes, which would induce the formation of toxic halogenated byproducts. In this study, we proposed a novel heat-activated peroxydisulfate (heat/PDS) process to clean the membrane fouling derived from humic acid (HA). The results show that the combination of heat and PDS can achieve almost 100% recovery of permeate flux after soaking the HA-fouled membrane in 1 mmol/L PDS solution at 50 ℃ for 2 h, which is attributed to the changes of HA structure and enhanced detachment of foulants from membranes. The properties of different treated membranes are characterized by scanning electron microscopy (SEM), atomic force microscope (AFM), attenuated total reflection Fourier transform infrared spectroscopy (ATR-FTIR), and X-ray photoelectron spectroscopy (XPS), demonstrating that the reversible and irreversible foulants could be effectively removed by heat/PDS cleaning. The filtration process and fouling mechanism of the cleaned membrane were close to that of the virgin membrane, illustrating the good reusability of the cleaned membrane. Additionally, heat/PDS which can avoid the generation of halogenated byproducts shows comparable performance to NaClO on membrane cleaning and high performance for the removal of fouling caused by sodium alginate (SA), HA-bovine serum albumin (BSA)-SA mixture and algae, further suggesting that heat/PDS would be a potential alternative for membrane cleaning in practical application.
Triple-negative breast cancer (TNBC) lacks specific regimens for targeted therapy. Repeat chemotherapy promotes the evolution of TNBC into highly chemo-resistant tumors that metastasize to multiple organs simultaneously. Herein, polyacrylic acid-coated ultrasmall superparamagnetic iron-oxide nanoparticles (PAA@IONs) and dual-targeting doxorubicin liposomes achieved chemo–immunotherapy through intermittent administration. They inhibited tumor-drug resistance and multiorgan-specific metastasis significantly by targeting tumors and the microenvironment. We deciphered an immunosuppressive pre-metastatic niche and discovered that PAA@IONs could target tumors, tumor-draining lymph nodes (TDLNs), the liver, bone, and lungs. They promoted the polarization of macrophages into M1 macrophages in these organs and tissues. This action remodeled the immunosuppressive microenvironment and induced a sustained immune response, thereby reducing organ-specific metastasis. Overcoming the disadvantages of doxorubicin-induced cardiotoxicity as well as low tumor specificity, dual peptide-modified liposomes could target CD206 and CD13 simultaneously, and reverse chemo-resistance. These properties resulted in a significant decrease in the numbers of myeloid-derived suppressor cells (MDSCs) and cancer stem cells (CSCs) in the liver, lungs, and bone, thereby reducing protein expression of Ki-67 in TDLNs, and dramatically increasing the number of cluster of differentiation (CD)8+T cells and CD8+ T cell/T-regulatory-cell ratio in tumors and TDLNs (P < 0.0001). Compared with the control (P < 0.05 and P < 0.01, respectively) or free drug (P < 0.0001 and P < 0.01, respectively), multi-organ metastases were suppressed significantly, tumor-growth rate reduced, and survival prolonged. Our drug-delivery system overcame TNBC chemo-resistance and inhibited multiorgan-specific metastases. It circumvents the lack of effective therapeutic targets, the problem of patient selection due to a low mutation rate, and can simultaneously offer the possibility of avoiding surgery and considerable postoperative complications.
The appearance and spread of antibiotic-resistant pathogens known as antimicrobial resistance (AMR) is one of the major worldwide health crises that humanity have to deal with over the next decades. One of the main methods for addressing AMR is the effective screening for antimicrobial insensitivity in clinical and environmental monitoring. Current clinical laboratory procedures use traditional culture-based antibiotic susceptibility testing (AST) methods, which can take up to 24h to identify which drug is suitable for the infection inhibition. Therefore, it is vital to develop novel strategies that offer quick, simple, affordable, reliable, sensitive and accurate AMR monitoring. Sensors for AMR markers detection could possess the essential qualities for quickly identifying resistant microorganisms and could give vital data for the selection of antibacterial drugs administration. This review offers a summary of the innovative application of these AMR markers detection strategies focusing on healthcare and environmental surveillance for the AMR genotypic or phenotypic assessment.
Carbon dots (CDs), a new building unit, have been revolutionizing the fields of biomedicine, bioimaging, and optoelectronics with their excellent physical, chemical, and biological properties. However, the difficulty of preparing excitation-dependent full-spectrum fluorescent CDs has seriously hindered their further research in fluorescence emission mechanisms and biomedicine. Here, we report full-spectrum fluorescent CDs that exhibit controlled emission changes from purple (380 nm) to red (613 nm) at room temperature by changing the excitation wavelength, and the excitation dependence was closely related to the regulation of sp2 and sp3 hybrid carbon structures by β-cyclodextrin-related groups. In addition, by regulating the content of β-cyclodextrin, the optimal quantum yields of full-spectrum fluorescent CDs were 8.97%, 8.35%, 7.90%, 9.69% and 17.4% at the excitation wavelengths of 340, 350, 390, 410 and 540 nm, respectively. Due to their excellent biocompatibility and color tunability, full-spectrum fluorescent CDs emitted bright and steady purple, blue, green, yellow, and red fluorescence in MCF-7 cells. Moreover, we optimized the imaging conditions of CDs and mitochondrial-specific dyes; and realized the mitochondrial-targeted co-localization imaging of purple, blue and green fluorescence. After that, we also explored the effect of full-spectrum fluorescent CDs in vivo fluorescence imaging through the intratumorally, subcutaneously, and caudal vein, and found that full-spectrum fluorescent CDs had good fluorescence imaging ability in vivo.
CRISPR/Cas system has been utilized to rationally manipulate intracellular genes, and it has been engineered as versatile and efficient gene editing tools with precise site-specificity and excellent targeting ability for therapeutics, diagnostics, and bioimaging. Here, the evolution and application of CRISPR/Cas systems were sketched chronologically. Landmark works were exemplified to illustrate the design principles of CRISPR/Cas systems. Furthermore, the delivery vectors of CRISPR/Cas system especially DNA nanomaterials-based vectors were categorized and illuminated. DNA nanomaterials are suitable for CRISPR/Cas system delivery via base pairing due to its sequence programmability and biocompatibility. Then the applications of CRISPR/Cas in diagnosis and genomic imaging were highlighted. At the end of the review, the challenges and opportunities of CRISPR/Cas systems were deeply discussed. We envision that the grant advances on CRISPR/Cas systems will promote the development of interdisciplinary fields in chemistry, biology and medicine.
The rechargeable Li-O2 battery endowed with high theoretical specific energy density has sparked intense research interest as a promising energy storage system. However, the intrinsic high activity of Li anode, especially to moisture, usually leads to inferior electrochemical performance of Li-O2 battery in humid environments, hindering its widespread application. To settle the trouble of poor moisture tolerance, fabricating a water-proof layer on the Li-metal anode could be an effective tactic. Herein, a facile strategy for constructing an ibuprofen-based protective layer on the Li anode has been proposed to realize highly rechargeable Li-O2 battery in humid atmosphere. Due to the in-situ reaction between ibuprofen reagent and metallic Li, the protective layer with a thickness of ~30 μm has been uniformly deposited on the surface of Li anode. Particularly, the protective layer, consisting of a large amount of hydrophobic alkyl group and benzene ring, can significantly resist water ingress and enhance the electrochemical stability of Li anode. As a result, the Li-O2 battery based on the protected Li anode achieves a long cycle life of 210 h (21 cycles at 1000 mAh/g, 200 mA/g) in highly moist atmosphere with relative humidity (RH) of 68%. This convenient and efficient strategy offers novel design concept of water-resistant metal anode, and paves the way to the promising future prospect for the high-energy Li-O2 battery implementing in the ambient atmosphere.
Regenerating spent graphite (SG) from retired lithium-ion batteries (LIBs) can effectively avoid resource waste. However, the technology is challenged by the impurity content and energy consumption. In this study, micro-expanded graphite (MEG) was synthesized by one-step oxidation method using waste LIBs anode graphite as material and perchloric acid as intercalation and oxidant agent. Then, its performance as a LIBs anode material were investigated as well as the greenhouse gas (GHG) emissions of the whole process were calculated. Perchloric acid was successfully embedded in the SG during the reaction, which effectively removed the impurities in the graphite. Defects introduced during intercalation and delamination, such as nanopores and intercrystalline cracks. Both provide additional space for Li ions during charging and discharging, thereby promoting capacity enhancement. The prepared MEG expresses a rate capability as high as 340.32 mAh/g at a current density of 0.1 C and still retains 81.73% of the capacity after 100 cycles at a current density of 1 C. Additionally, the GHG emissions of the synthesis process of this article and other literatures are compared. The results demonstrated that perchloric acid treatment process provides a low-carbon, time- and energy-saving approach for regenerated SG as battery grade material.
This report describes the oxidative cyclopalladation activation of a C≡C bond during the Pd-catalyzed hydroalkylation of alkynes and analyzes potential reaction pathways based on density functional theory calculations. The more favorable pathway in-volves an oxidative cyclopalladation to generate a palladacyclopropene intermediate, which is rarely examined in Pd-catalyzed alkyne transformations. The reaction pathway proposed herein is kinetically favorable relative to the commonly proposed alkyne insertion mode. Furthermore, the Laplacians of the electron density, interaction region indicators, Mayer bond orders, and localized orbital bonding are evaluated to determine the reaction processes and characterize the key intermediates. Theoretical calculations indicate covalent bonding between a Pd(Ⅱ) center and the two C-atoms in three-membered palladacycle species. Finally, electrostatic potential analysis reveals that the regioselectivity is governed by the charge distribution on the palladacycle moiety during the protonation step.
The construction of an integrated nanoplatform with controlled fungicide delivery features in the specific microenvironment produced by fungal pathogens is a highly desirable strategy to improve the utilization of fungicides. Herein, we report a supramolecular fungicide delivery system based on benzimidazole-modified NH2-MIL-101(Fe) metal–organic frameworks (B-MIL-101(Fe) MOFs) as carriers loaded with osthole (OS), and β-cyclodextrin (β-CD) as nanovalves to form β-CD@B-MIL-101(Fe)-OS. The nanoplatform can release the loaded OS for fungus control through self-degradation of the MOFs skeleton in an oxalic acid microenvironment produced by Botrytis cinerea. The experimental results exhibit that the constructed supramolecular fungicide delivery system could effectively inhibit mycelial growth and protect the tomatoes from infection by B. cinerea during the ripening stage. This strategy constructs a facile and integrated supramolecular drug delivery system for B. cinerea control and opens up a new avenue for the sustainable development of modern agriculture.
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