Latest ArticlesStructural and functional biomimicking of the active site of [NiFe]-hydrogenases can provide helpful hints for designing bioinspired catalysts to replace the expensive noble metal catalysts for H2 generation and uptake. Treatment of dianion [Ni(phma)]2- [H4phma = N, N'-1, 2-phenylenebis(2-mercaptoacetamide)] with [NiCl2(dppp)] (dppp = bis(diphenylphosphino)propane) yielded a dinickel product [Ni(phma)(μ-S, S')Ni(dppp)] (1) as the model complex relevant to the active site of [NiFe]-H2ases. The structure of complex 1 has been characterized by single-crystal X-ray analysis. From cyclic voltammetry and controlled potential electrolysis studies, complex 1 was found to be a moderate electrocatalyst for the H2-evoluting reaction using ClCH2COOH as the proton source.
Zinc-based electrochemistry energy storage with high safety and high theoretical capacity is considered to be a competitive candidate to replace lithium-ion batteries. In electrochemical energy storage, multimetal oxide cathode materials can generally provide a wider electrochemical stability window and a higher capacity compared with single metal oxides cathode. Here, a new type of cathode material, MnFe2Co3O8 nanodots/functional graphene sheets, is designed and used for aqueous hybrid Zn-based energy storage. Coupling with a hybrid electrolyte based on zinc sulfate and potassium hydroxide, the asfabricated battery was able to work with a wide electrochemical window of 0.1~1.8 V, showed a high specific capacity of 660 mAh/g, delivered an ultrahigh energy density of 1135 Wh/kg and a scalable power density of 5754 W/kg (calculated based on the cathode), and displayed a long cycling life of 1000 cycles. These are mainly attributed to the valence charge density distribution in MnFe2Co3O8 nanodots, the good structural strengthening as well as high conductivity of the cathode, and the right electrolyte. Such cathode material also exhibited high electrocatalytic activity for oxygen evolution reaction and thus could be used for constructing a Zn-air battery with an ultrahigh reversible capacity of 9556 mAh/g.
In order to boost power conversion efficiency (PCE) and operation stability of organic solar cells (OSCs), we propose a new idea of phase junction materials (PJMs) used as a photoactive layer component to improve device performance and stability. For this purpose, a novel PJM of H-TRC8 based on rhodanine unit was designed with a conjugated AH-D-A framework. Here, AH is a hydrogen-donating electron acceptor unit, D-A is an electron donor-acceptor unit. It is found that H-TRC8 has a good carriertransporting ability, as well as definite hydrogen-bond and D-A interaction with donor/acceptor materials. While H-TRC8 is added into the PBDB-T/PC60BM blend film with 1.0 vol% DIO (1, 8-diiodooctane), the resulting blend film exhibited an enhanced absorption and improved morphology. The intermolecular hydrogen bond between H-TRC8 and PBDB-T plays an important role for them, which is confirmed via FT-IR spectra and 2D 1H NMR. As a result, the PBDB-T/PC60BM-based devices with 1.25 wt% H-TRC8 and 1.0 vol% DIO exhibit a significantly improved PCE of 8.06%, which is increased by 20.6% in comparison to that in the binary devices with 1.0 vol% DIO only (PCE = 6.68%). Furthermore, the device stability is significantly enhanced with only 43% PCE roll-off at 150 ℃ for 120 h. This work indicates that AH-D-A-type PJMs are promising photovoltaic materials used as photoactive-layer components to achieve high-performance fullerene OSCs with high device stability.
By integrating the merits of lanthanide elements and quantum dots, we firstly design CeO2 quantum dots doped Ni-Co hydroxide nanosheet via a controllable synthetic strategy, which exhibits a large specific capacitance (1370.7 F/g at 1.0 A/g) and a good cyclic stability (90.6% retention after 4000 cycles). Moreover, we assemble an aqueous asymmetric supercapacitor with the obtained material, which has an extremely high energy density (108.9 Wh/kg at 378 W/kg) and outstanding cycle stability (retaining 88.1% capacitance at 2.0 A/g after 4000 cycles).
Pathogen infection is the main cause of human morbidity and death. Traditional antibiotics usually sterilize bacteria in chemical ways, which tends to develop serious antibiotic resistance. Cationic polymers exhibit good bacterial inhibition with less resistance, but often face severe cytotoxicity toward normal cells. The optimization of polymeric antimicrobials for enhanced bactericidal capacity and improved biocompatibility is quite meaningful. In addition, photodynamic therapy (PDT) is a therapeutic modality with less susceptibility to develop resistance. Herein, a typical commercial polymeric antimicrobial, polyhexamethylene guanidine (PHMG) was selected for current proof-of-concept optimization due to its excellent bactericidal capacity but moderate biocompatibility. Eosin-Y (EoS) was copolymerized to afford EoS-labeled polymer conjugates, poly(2-(dimethylamino) ethyl methacrylate-co-eosin), P(DMAEMA-co-EoS), which was conjugated with PHMG to afford a novel polymeric antimicrobial, P(DMAEMA-co-EoS)-b-PHMG-b-P(DMAEMA-co-EoS), noted as PEoS-PHMG. It could efficiently kill broad-spectrum bacteria by physical damage and photodynamic therapy. Compared with PHMG, the bacterial inhibition of PEoS-PHMG was potentiated after the functionalization. Furthermore, PEoS-PHMG exhibited low cytotoxicity and minimal hemolysis, which was demonstrated by cell viability assays toward LO2 cells and RAW 264.7 cells as well as hemolytic assays against red blood cells. These results confirmed that the resultant PEoS-PHMG could act as promising alternative antibacterial materials with excellent broad-spectrum bacterial inhibition and favorable biocompatibility.
Eleven new fluorine-containing FDA-approved drugs have been profiled and details of their discovery and preparation are discussed. Therapeutic areas include schizophrenia, migraine, multiple sclerosis, insomnia, rheumatoid arthritis, anti-tuberculosis, breast cancer, lymphoma kinase inhibitor, serotonin receptor antagonist. New pharmaceuticals feature four examples of aromatic fluorine, three aromatic CF3 group, three aliphatic CF3 and one compound with aromatic CF3O group. Furthermore, among the new compounds, six are chiral and seven are derived from tailor-made amino acids.
An iron (Ⅲ) cluster, namely [Fe10(μ3-O)8L8(NO3)6] (1), has been synthesized by treatment of Fe (NO3)3·9H2O with 3, 5-dimethyl-1-(hydroxymethyl)-pyrazole (HL) under ambient temperature. The core skeleton of {FeⅢ10} can be regarded as a pear-like cage with eight triangular {FeⅢ3(μ3-O)} units, in which each three FeⅢ centers is held together by one μ3-O2- group with FeⅢ centers as corner-sharing triangle units. Importantly, {FeⅢ10} cluster is not only stable in solid state but also in solution, which is confirmed by powder X-ray diffraction (PXRD) pattern and electrospray ionization mass spectrometry (ESI-MS), respectively. Furthermore, 1 shows antiferromagnetic exchange behavior arising from the interactions between the iron(Ⅲ) centers.
Ru and Co are highly dispersed on the surface of TiO2 nanoparticles with an easy coprecipitation method to fabricate a novel Ru-based catalyst (Ru/Co-TiO2). The fabricated Ru/Co-TiO2 catalyst exhibits superior catalytic performance for promoting NaBH4 hydrolysis in alkaline medium, showing an impressive hydrogen generation rate per gram Ru as high as 172 L min-1 gRu-1, which is better than most of recently reported Ru-based catalysts. In addition, the fabricated Ru/Co-TiO2 catalyst also shows excellent durability in cycle use, with only 2.9% activity loss after being used for 5 cycles.These advantages make the developed Ru/ Co-TiO2 catalyst a potential choice for promoting hydrogen generation from NaBH4 hydrolysis.
Developing a fast, sensitive and convenient method for the detection of hydroxyl radicals (·OH) in the atmosphere could help us know the precursor levels of atmospheric species and control air pollution. In this work, the carbon fiber paper (CFP) functionalizing with a kind of covalent organic frameworks (COFs), formed from 1, 3, 5-triformylphloroglucinol (Tp) and benzidine (BD) (COF(TpBD)), was firstly used a new platform for ·OH trapping and detection. The COF(TpBD) modified CFP was acted as a filter to impregnate salicylic acid (SA) and a detector to detect 2, 5-dihydroxybenzoic acid (2, 5-DHBA) which was produced from the reaction between the impregnated SA and ·OH in the atmosphere. This method provided a linearity for 2, 5-DHBA from 5.0×10-14 mol/L 1.0×10-9 mol/L with a detection limit of 6.9×10-15 mol/L, which is corresponding to the amount of ·OH from 3.0×107 to 6.0×1011 molecules/cm3 with the detection limit of 4.1×106 molecules/cm3. This COF(TpBD)-CFP platform has been successfully applied for the detection of ·OH concentration under different conditions of Yangzhou when the sampling time was shortened to 30 min. This work has provided a new method for atmospheric ·OH detection with excellent sensitivity, simplicity, and high speed.
In addition to the theoretical research, direct ethanol fuel cells have great potential in practical applications. The performance of direct ethanol fuel cells largely depends on the electrocatalysts. Pt-based electrocatalysts have been promising candidates for advancing direct ethanol fuel cells for its high catalytic activity and great durability. Here, a PtSn catalyst with unique three-dimensional porous nanostructure has been designed and synthesized via a two-step liquid phase reduction reaction. Sn formed a self-supporting framework in PtSn alloy particles (~3.5 nm). In ethanol electro-oxidation reaction, the PtSn catalyst exhibited high mass activity and excellent recycling time compared with that of Pt/C. After the morphology characterization before and after potential cycling, the PtSn alloy-based nano-catalyst showed good stability. The PtSn catalysts effectively avoid structural instability due to the external carriers, and prolong the leaching time of Sn. In addition, the introduction of a certain amount of Sn can also solve the poisoning phenomenon of active sites on Pt surface. The design strategy of porous alloy nano-catalyst sheds light on its applications in direct ethanol fuel cells.
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