Latest ArticlesImproving the surface atoms utilization efficiency of catalysts is extremely important for large-scale H2 production by electrochemical water splitting, but it remains a great challenge. Herein, we reported two kinds of MoO3-polyoxometalate hybrid nanobelt superstructures (MoO3-POM HNSs, POM= PW12O40 and SiW12O40) using a simple hydrothermal method. Such superstructure with highly uniform nanoparticles as building blocks can expose more surface atoms and emanate increased specific surface area. The incorporated POMs generated abundant oxygen vacancies, improved the electronic mobility, and modulated the surface electronic structure of MoO3, allowing to optimize the H* adsorption/desorption and dehydrogenation kinetics of catalyst. Notably, the as-prepared MoO3-PW12O40 HNSs electrodes not only displayed the low overpotentials of 108 mV at 10 mA/cm2 current density in 0.5 mol/L H2SO4 electrolyte but also displayed excellent long-term stability. The hydrogen evolution reaction (HER) performance of MoO3-POM superstructures is significantly better than that of corresponding bulk materials MoO3@PW12O40 and MoO3@SiW12O40, and the overpotentials are about 8.3 and 4.9 times lower than that of single MoO3. This work opens an avenue for designing highly surface-exposed catalysts for electrocatalytic H2 production and other electrochemical applications.
Herein, the Cu(Ⅲ) synthesized from copper plating effluent was developed for the first time to evaluate the onsite degradation performance of heavy metal complexes in the wastewater, thus achieving the purpose of "treating waste with waste". The results indicated that synthetic Cu(Ⅲ) presented the excellent decomplexation performance for Cu(Ⅱ)/Ni(Ⅱ)-organic complexes. The removal efficiency of Cu(Ⅱ)/Ni(Ⅱ)-EDTA significantly increased with increasing Cu(Ⅲ) dosage, and the degradation of Cu(Ⅱ)/Ni(Ⅱ)-EDTA by synthetic Cu(Ⅲ) system displayed highly pH-dependent reactivity. The radical quencher experiments confirmed that Cu(Ⅲ) direct oxidation were mainly involved in the degradation of Cu(Ⅱ)-EDTA. Additionally, the continuous decarboxylation process was proven to be the main degradation pathway of Cu(Ⅱ)-EDTA in Cu(Ⅲ) system. The coexisting substances (SO42−, Cl− and fulvic acids) showed little impacts at low level for the removal of Cu(Ⅱ)/Ni(Ⅱ)-EDTA, while retarded the degradation of Cu(Ⅱ)-EDTA slightly at high level, which features high selective oxidation. Encouragingly, it was also effective to remove Cu(Ⅱ)/Ni(Ⅱ)-EDTA from in treating actual Cu/Ni-containing wastewater through synthetic Cu(Ⅲ) treatment.
Pyridyl-based ketones and 1, 6-diketones are both attractive and invaluable scaffolds which play pivotal roles in the construction and structural modification of a plethora of synthetically paramount natural products, pharmaceuticals, organic materials and fine chemicals. In this context, we herein demonstrate an unprecedented, robust and generally applicable synthetically strategy to deliver these two crucial ketone frameworks via visible-light-induced ring-opening coupling reactions of cycloalcohols with vinylazaarenes and enones, respectively. A plausible mechanism involves the selective β-C-C bond cleavage of cycloalcohols enabled by proton-coupled electron transfer and ensuing Giese-type addition followed by single electron reduction and protonation. The synthetic methodology exhibits broad substrate scope, excellent functional group compatibility as well as operational simplicity and environmental friendliness.
Ln-containing polyoxoniobates (PONbs) have appealing applications in luminescence, information encryption and magnetic fields, but the synthesis of PONbs containing high-nuclearity Ln-O clusters is challenging due to the easy hydrolysis of Ln3+ ions in alkaline environments. In this paper, we are able to integrate CO32− and high-nuclearity Ln-O clusters into PONb to construct an inorganic giant Eu19-embedded PONb H49K16Na13(H2O)63[Eu21O2(OH)7(H2O)5(Nb7O22)10(Nb2O6)2(CO3)18]·91H2O (1), which contains the highest nuclearity Eu-O clusters and the largest number of Eu3+ ions among PONbs. In addition, the film that was prepared by mixing 1 with gelatin and glycerol, exhibits reversible luminescence switching behavior under acid/alkali stimulation and has been used to create a fluorescence-encoded information approach. This work paves a feasible strategy for the construction of high-nuclearity Ln-O cluster-containing PONbs and the expansion of the application of Ln-containing PONbs in information encryption.
Developing a heterostructure for alloying-based anode for sodium-ion batteries (SIBs) is an efficient solution to accommodate volume change upon sodiation/desodiation and boost sodium storage since it combines the merits of each component. Herein, we report a metallic and microphone-like Sn-Zn0.9Mn0.1O heterostructure via an in-situ Mn doping strategy. Based on theoretical calculations and experimental results, the introduction of Mn into ZnO (a small amount of Mn also diffuses into the Sn lattice) can not only enhance intrinsic electronic conductivity but also reduce the Na+ diffusion barrier inside the Sn phase. When evaluated as anode for SIBs, the obtained heterostructures show a high reversible capacity of 395.1 mAh/g at 0.1 A/g, rate capability of 332 mAh/g at 5 A/g, and capacity retention of almost 100% after 850 cycles at 5 A/g, indicating its great potential for high-power application of SIBs.
In this paper, low-temperature dielectric-blocked discharge plasma (DBD) was employed for the first time to treat silica-doped H4PMo11VO40 (HPAV) catalysts (DBD(Ar/x)-MF-Catal) and apply them in the catalytic methacrolein (MAL) selective oxidation to produce methacrylic acid (MAA). This work investigates in detail the controllable regulation of the concentration of oxidation states on silica-doped HPAV catalysts by adjusting the DBD discharge with controlled changes in voltage, current, treatment time, and treatment medium. It reports the intrinsic correlation between oxidation states and MAL oxidation performance. The research results indicated that the catalytic performance was related to the presence of oxygen vacancies and oxygen species (VO2+), and are the main reason for the selective oxidation of MAL to MAA. Besides, the generation of oxygen vacancies and VO2+ altered localized electrons, which resulted in the easier activation of O2. Theoretical calculations of DFT also proved the formation mechanism of oxygen vacancies and VO2+ and electron properties on high-performance polymers, which elucidated the intrinsic influence of catalyst components. The DBD(Ar/10)-MF-Catal catalysts with suitable VO2+ and oxygen vacancy concentrations exhibited the highest catalytic performance with 90% MAL conversion and 70% MAA selectivity and showed good stability (500 h).
The nano-MOF-303 synthesized by microwave method exhibited efficient adsorption capacity (232 mg/g) toward Ag+, in which the adsorption behaviors were fitted by the pseudo-second-order kinetic and the Freundlich isotherm model. The outstanding Ag+ sorption ability of nano-MOF-303 could be contributed to electrostatic interactions, weak coordination interaction of Ag-N, and AgCl precipitates originating from the stored Cl− in nano-MOF-303. Besides the adsorbent regeneration, the formed Ag/AgCl onto nano-MOF-303 could produce Ag/AgCl/MOF-303 as a photocatalyst for sulfamethoxazole degradation under visible light. In this work, both the adsorption and photocatalysis mechanisms were clarified, which might provide insight to develop more effective adsorbents for mining the critical resource from the wastewater.
Up to now, numerous emerging methods of cancer treatment including chemodynamic therapy, photothermal therapy, photodynamic therapy, sonodynamic therapy, immunotherapy and chemotherapy have rapidly entered a new stage of development. However, the single treatment mode is often constrained by the complex tumor microenvironment. Recently, the nanomaterials and nanomedicine have emerged as promising avenues to overcome the limitation in cancer theranostics. Especially, metal-organic frameworks (MOFs) have gained considerable interests in cancer therapy because of their customizable morphologies, easy functionalization, large specific surface area, and good biocompatibility. Among these MOFs, iron-based MOFs (Fe-MOFs) are particularly promising for cancer treatment due to their properties as nano-photosensitizers, peroxidase-like activity, bioimaging contrast capabilities, and biodegradability. Utilizing their structural regularity and synthetic tunability, Fe-MOFs can be engineered to incorporate organic molecules or other inorganic nanoparticles, thereby creating multifunctional nanoplatforms for single or combined theranostic modes. Herein, the minireview focuses on the recent advancements of the Fe-MOFs-based nanoplatforms for self-enhanced imaging and treatment at tumor sites. Furthermore, the clinical research development of Fe-MOFs-based nanoplatforms is discussed, addressing key challenges and innovations for the future. Our review aims to provide novice researchers with a foundational understanding of advanced cancer theranostic modes and promote their clinical applications through the modification of Fe-MOFs.
Excited-state intramolecular proton-transfer (ESIPT) based fluorescence probes are particularly attractive due to their unique properties including environmental sensitivity, a large Stokes shift, and potential for ratiometric sensing. In general, ESIPT-based fluorophore incorporates an intramolecular hydrogen bonding interaction between a hydrogen bond donor (–OH and NH2 are common) and a hydrogen bond acceptor (C=N and C=O). More, protection–deprotection of hydroxyl group as hydrogen bond donor could induce an off-on switch of ESIPT-based emission. Therefore, protection–deprotection of hydroxyl group has been the widely used strategy to design fluorescent probes, where the potential key issue is selecting a protective group that can specifically leave in the presence of the target analyte. In this review, we mainly summarize the specific protecting groups (sites) and deprotection mechanisms for biologically important species (including reactive sulfur species (RSS), reactive oxygen species (ROS), enzymes, etc.), and analyze the advantages and disadvantages of different protection mechanisms from some aspects including probe stability, selectivity, response rate and assay system, etc. Based on the aforementioned, we further point out the current challenges and the potential future direction for developing ESIPT-based probes.
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