Latest ArticlesWater pollution caused by global population growth, urban expansion and industrialization development is one of the urgent issues that need to be addressed in the 21st century. Up to now, it was challenging for metal-organic frameworks (MOFs) to be used in the actual water treatment due to that the powder MOFs suffered from difficult reuse, poor water stability and easy corrosion. It is an effective strategy to immobilize MOFs powder onto porous sponge foam carriers for accomplishing large flux, facile recycling, easy processing water treatment setups. In this review article, the fabrication approaches and applications of different MOFs/sponge composites were highlighted, in which the fluorescence detection of pollutants, adsorption and separation of pollutants, catalytic reduction and oxidation of pollutants were included. Finally, the future challenges and opportunities of MOF/sponge for water treatment are proposed, aiming to provide in-depth guidance for the future design and manufacture of the immobilized MOFs onto sponge foams.
Electrocatalytic synthesis of ammonia as an environment-friendly and sustainable development method has received widespread attention in recent years. Two-dimensional (2D) materials are a promising catalyst for ammonia synthesis due to their large surface area. In this work, we have constructed a series of 2D metal borides (MBenes) with transition metal (TM) defects (TMd-MBenes) and comprehensively calculated the reactivity of electrocatalytic synthesis of ammonia-based on density functional theory. The results have demonstrated that the TMd-MBenes can effectively activate nitrogen oxide (NO) and nitrogen (N2) molecules thermodynamically. Particularly interesting, the co-chemisorption of O atoms, dissociated from NO, can facilitate the spilled of the inert N2 molecules into single N atoms, which can further hydrogenate into ammonia easily with an ultralow limiting potential of 0.59 V on TMd-MnB. Our research has not only provided clues for catalyst design for experimental study but also paved the way for the industrial application of electrocatalytic ammonia synthesis.
The virtual cocrystal screening approach based on molecular electrostatic potential surface (MEPS) maps is a fast and feasible computational method to estimate the probability of cocrystal formation by calculating the difference in the interaction site pairing energies of monomers and that of their assemblies prior to experimental screening. In this paper, we report 12 cocrystal forms of temozolomide with mono-, di-, and trihydroxy benzoic acids, namely, 3-hydroxy-, 2,4-dihydroxy-, 2,5-dihydroxy-, 2,6-dihydroxy-, 3,4-dihydroxy-, and 3,4,5-trihydroxy-benzoic acids, as well as benzoic acid, as pharmaceutical coformers for the first time. 10 single crystals out of the 12 cocrystal forms were obtained and unequivocally determined by single-crystal X-ray diffraction, which clarified spatial arrangements, molecular conformations, and supramolecular synthons. MEPS further gains some insights into the sites of hydrogen bonding interactions for exploring combination patterns in these assemblies. Modulated stability of TMZ was successfully achieved by cocrystallization with these acids.
Commercial V2O5-based catalysts have been successfully applied in NH3 selective catalytic reduction (NH3-SCR) of NOx from power stations, but their poor alkali-resistance restrains the wider application in nonelectrical industries. In this study, NOx reduction against alkali poisoning over V2O5/TiO2 is greatly improved via Ce(SO4)2 modification. It has been originally demonstrated that Ce4+–SO42− pair sites play crucial roles in improving NOx reduction against alkali poisoning over V2O5/TiO2 catalysts. The strong interaction between V species and Ce sites of Ce4+–SO42− pairs triggers the reaction between NH4+species and gaseous NO via Eley-Rideal (E-R) reaction pathway. After K-poisoning, the SO42− sites of Ce4+–SO42− pairs as protective sites strongly bond with K and thus maintain the high reaction efficiency via the E-R reaction pathway. This work demonstrates an effective strategy to enhance NOx reduction against alkali poisoning over catalysts via constructing Ce4+–SO42− pair sites, contributing to developing alkali-resistant SCR catalysts for practical application in nonelectrical industries.
Nanoplastics (NPs) in aqueous environment have become a category of emerging pollutants on account of their potential risks to both human health and environment. The detection of NPs is a great challenge due to the lack of sensitive and selective sensing materials with fast response time and wide sensing range of particle sizes. Herein, a Tb-based coordination polymer has been synthesized for luminescent detection of nanopolystyrene with different particle sizes in aqueous solutions, showing a low limit of detection, fast response time within 10 s and high selectivity in the presence of other plastics. The “turn-on” sensing mechanism is studied in detail. This work provides a facile method for the fast detection of NPs.
The present study reported fabrication of novel carbon quantum dots-MnFe2O4@ZIF-8 (CQDs-MFO@ZIF-8) by using co-precipitation hydrothermal method for activation of peroxydisulfate (PDS) to degrade bisphenol A (BPA), one of important emerging organic pollutants in water environment. CQDs-MFO@ZIF-8 served as a highly efficient thermal activated PDS catalyst with high catalytic degradation efficiency, reusability and stability. The catalyst achieved almost completely removal of 20.0 mg/L BPA within 5.0 min, and the degradation efficiency remained higher than 83% after 5 consecutive cycles. Free radicals (•OH, SO4•− and •O2−) and non-free radicals (1O2) were generated in the thermal PDS-activation system, in which singlet oxygen (1O2) played a dominant role in the degradation of BPA. The potential toxicity of BPA degradation intermediates was analyzed upon the culture of E. coli and Chlorella sorokiniana by using Ecological Structure-Activity Relationship Model (ECOSAR) program. The catalytic performances of BPA degradation by CQDs-MFO@ZIF-8 were evaluated for treatment of different practical water samples to further verify the feasibility of practical applications. This study provides proof-in-concept demonstration of new nanomaterials for enhanced catalytic water decontamination.
Staphylococcal enterotoxin A (SEA) derived from Staphylococcus aureus, as a superantigen, shows potential for cancer immunotherapy, but systemic immunotoxicity restricts its clinical application. Targeted delivery of SEA to tumor site provides a promising option for reducing the systemic toxicity. Here, we constructed an iRGD peptide (H-[Cys-Arg-Gly-Asp-Lys-Gly-Pro-Asp-Cys]-NH2) modified nanoparticle (iDPP) to deliver plasmids encoding SEA for melanoma treatment. The iDPP/SEA nanocomplexes efficiently mediated SEA expression in B16-F10 cells in vivo and in vitro and induced the activation of lymphocytes and maturation of murine bone marrow-derived dendritic cells (BMDCs) in vitro. In the subcutaneous B16-F10 melanoma model, the iDPP/SEA nanocomplexes could effectively enhance immune response and T lymphocytes infiltration in tumor site after intravenous administration, thereby considerably decreased melanoma growth. Meanwhile, no obvious adverse effect was observed after intravenous administration of the iDPP/SEA nanocomplexes in vivo. Our findings demonstrated that gene therapy of SEA is a potential candidate for melanoma treatment.
We reported the characterization of a novel brassicicene diterpene biosynthetic gene cluster, which contains a unique α-ketoglutarate-dependent dioxygenase (αKGD) enzyme, AbnI. Our findings revealed that AbnI demonstrates remarkable substrate promiscuity and is capable of activating multiple sites on both 5–8–5 and 5–9–5 brassicicene skeletons, resulting in skeleton modifications and an unexpected ring system rearrangement. These results suggested the potential utility of AbnI as an enzymatic tool for terpene CH functionalization. In addition, the catalytic mechanism of AbnI and its potential ecological implications were discussed.
Alginate is a natural polysaccharide polymer. Hydrogel filtration membranes prepared from alginate show excellent fouling resistance and controllable separation performance, but poor mechanical properties limit the use of algae hydrogels. In this study, Ba2+/Ca2+ co-crosslinked alginate (Ba/CaAlg) hydrogel membrane was prepared by cross-linking sodium alginate with a blend aqueous solution of barium ions and calcium ions, and the membrane was applied to the separation of dyes/salts from dyeing wastewater. Compared with the CaAlg membrane, the Ba/CaAlg hydrogel membrane exhibited more stable structure, and the mechanical properties and salt tolerance of the membrane were significantly improved. The flux of Ba/CaAlg membrane for methyl blue/sodium chloride mixed solution reached 43.5 L m−2 h−1, which was significantly higher than that of CaAlg membrane. Besides, the Ba/CaAlg membrane showed higher dye rejection (>99.6%) and lower salt rejection (<8.2%). The structure of Ba/CaAlg membrane was preliminarily simulated by molecular dynamics, and the pore size and distribution of the membrane were calculated. The Ba/CaAlg membrane has a broad application prospect in dyes/salts separation.
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