Latest ArticlesDeveloping high-efficiency, inexpensive, and steady non-precious metal oxygen reduction reaction (ORR) catalysts to displace Pt-based catalysts is significant for commercial applications of Al-air battery. Here, we have prepared the Cu/Cu2O-NC catalyst with excellent ORR performance and high stability, due to the synergistic effect of Cu and Cu2O nanoparticles. The half-wave potential (0.8 V) and the limiting-current density (5.20 mA/cm2) of the Cu/Cu2O-NC are very close to those of the 20% Pt/C catalyst (0.82 V, 5.10 mA/cm2). Besides, it exhibits excellent performance with a maximal power density of 250 mW/cm2 and a stable continuous discharge for more than 90 h in the Al-air battery test. The promoting effects of Cu2O towards Cu-based ORR catalysts are illustrated as follows: (i) Cu2O is the major ORR active site by the redox of Cu(Ⅱ)/Cu(Ⅰ), which provides excellent ORR activities; (ii) Cu can stabilize the location of Cu2O by assisting the electron transfer to Cu(Ⅱ)/Cu(Ⅰ) redox, which is conducive to the high stability of the catalyst. This work provides a useful strategy for enhancing the ORR performance of Cu-based catalysts.
Semiconductor-mediated photocatalysis is a promising photochemical process for harvesting inexhaustible solar energy to address the energy crisis and environmental issues. However, the low solar-light response and poor carrier migration are severe drawbacks that limit its practical application. Herein, we propose a convenient pathway for improving electron-hole separation and solar energy utilisation by engineering defective ZnIn2S4 with doping of carbon dots. The optimum ZnIn2S4/CD200 nanosheet exhibited 100% diclofenac (DCF) degradation within 12 min under visible-light. The estimated photocatalytic efficiency under natural sunlight was 98.2%. Scavenging experiments and electron spin resonance (ESR) analysis indicated that the superoxide radical (O2∙−), photoelectron (e−), hole (h+) and hydroxyl radical (∙OH) were the predominant contributions in the ZnIn2S4/CD200/DCF/visible light system. Furthermore, ZnIn2S4/CD200 exhibited excellent reusability and stability after 4 times recycling. The photodegradation routes mainly involved hydroxylation, decarboxylation, CN bond cleavage, dechlorination, ring closure, and ring-opening. The ecological risk assessment and total organic carbon (TOC) tests exhibited desirable toxicity reduction and mineralization results. These observations not only offer a facile strategy for the construction of defective ZnIn2S4, but also pioneer the direct utilisation of natural light for highly efficient environmental remediation.
In the crystal engineering area, it is important to clearly demonstrating the relationship of structure and certain functionality. Herein, we present the study of the relationship of structure with phosphorescent nature for two new room temperature phosphorescence (RTP) coordination polymers (CPs). [Pb(FDA)(H2O)] (1) and [NH3(CH3)NH2(CH3)2][Pb4(FDA)5] (2), where H2FDA is 2, 5-furandicarboxylic acid, have been synthesized by solvothermal method using different solvents and Pb2+ sources and characterized by microanalysis, powder X-ray diffraction (PXRD), thermogravimetric (TG), IR and UV–vis spectra. The Pb2+ ions adopt bicapped triangle prism coordination sphere in 1 and 2, which are connected together via FDA2− ligands into bilayer structure in 1 while pillared-layer framework in 2. The FDA2− ligands show different bridging modes in 1 and 2, leading to distinct coordination interactions between Pb2+ ion and FDA2− ligand in both CPs. Both 1 and 2 emit ligand-centered RTP due to the heavy atom of Pb2+ ion, with a lifetime and quantum yield of 0.62 ms and 14.9% in 1 versus 1.69 ms and 15.7% in 2. The emission peak shows significant redshift (79 nm) in 2 regarding 1, which arises from their distinction of coordination interactions between Pb2+ ion and FDA2− ligand in both CPs.
Electrochemical water splitting is a facile and effective route to generate pure hydrogen and oxygen. However, the sluggish kinetics of hydrogen evolution reaction (HER) and especially oxygen evolution reaction (OER) hinder the water splitting efficiency. Meanwhile, the high-cost of noble-metal catalysts limit their actual application. It is thus highly urgent to exploit an economical and earth-abundant bifunctional HER and OER electrocatalyst to simplify procedure and reduce cost. Herein, we synthesize the three-dimensionally ordered macro-/mesoporous (3DOM/m) NixCo100-x alloys with distinctive structure and large surface area via a dual-templating technique. Among them, the 3DOM/m Ni61Co39 shows the lowest overpotentials of 121 mV and 241 mV at 10 mA/cm2 for HER and OER, respectively. Furthermore, when employed for water splitting, the Ni61Co39 only requires 1.60 V to approach 10 mA/cm2 and presents excellent stability. These encouraging performances of the Ni61Co39 render it a promising bifunctional catalyst for overall water splitting.
Extensive research has been performed on cell membrane camouflaged-based drug delivery systems in recent years. Herein, we provide an overview of the challenges in system preparation, functional design, continuous industrial production of these systems, and solution strategies for these challenges. Further, we analyze and discuss the frontier medical applications of cell membrane-camouflaged drug delivery systems in anti-inflammatory, anti-pathogenic microorganisms, and biological detoxification. This review takes a challenge-oriented perspective and seeks innovative strategies, provides a literature review of research into cell membrane-camouflaged drug delivery systems, and promotes the development of personalized clinical treatments.
Carbon nanofiber-based supercapacitors have broad prospects in powering wearable electronics owing to their high specific capacity, fast charge/discharge process, along with long-cycling life. Herein, a poly(acrylonitrile-co-β-methylhydrogen itaconate) copolymer was prepared and used to synthesize flexible hollow carbon nanofibers (HCNFs) via an electrospinning method without breaking after multiple bending. Subsequently, the inner and outer surfaces of HCNFs were evenly covered with ordered needle-like polyaniline (PANI) through in-situ polymerization methods to obtain three-dimensional flexible HCNFs/PANI composites, which exhibited a high capacity 1196.7 F/g at 1 A/g and good cycling stability (90.1% retention at 5 A/g after 3000 cycles). The symmetrical supercapacitor based on the HCNFs/PANI composites also delivered an outstanding electrochemical performance with high energy/power density (60.28 Wh/kg at 1000 W/kg) and superior cycling durability (90% capacitance retention after at 5 A/g 3000 cycles), which confirmed that the HCNFs/PANI composites had a wide application potential in flexible energy storage devices.
Gold nanovesicles (GVs) with unique plasmonic property and large cavity hold great potential as a stimuli-responsive nanocarrier to deliver drugs for efficient tumor chemotherapy and other therapies synergistically. Herein, we developed doxorubicin-loaded gold nanovesicles (DGVs), offering infrared thermal (IRT) and photoacoustic (PA) dual-modal imaging guided mild hyperthermia-enhanced chemo-photothermal cancer synergistic therapy. The DGVs are self-assembled by gold nanoparticles modified with amphiphilic copolymer in a predetermined concentration of doxorubicin through film rehydration method. Under the influence of laser excitation, the as-prepared DGVs exhibited good photothermal effect, which triggered the structural disruption of GVs and thus, allowed the efficient release of encapsulated DOX to enhance cell uptake for fluorescence imaging and tumor chemotherapy, respectively. In addition, DGVs also showed a strong PA and IRT signals in vivo. Our study demonstrated the potential of DGVs as stimuli-responsive drug delivery systems and cancer theranostics.
Environmental risks posed by discharge of the emerging contaminant antimony (Sb) into water bodies have raised global concerns recently. The toxicity of Sb has been shown to be species-dependent, with Sb(III) demonstrating much greater toxicity than Sb(V). Here, we proposed an electrochemical filtration system to achieve rapid detoxification of Sb(III) via a non-radical pathway. The key to this technology was an electroactive carbon nanotube filter functionalized with nanoscale Ti-Ce binary oxide. Under an electric field, in situ generated H2O2 could react with the Ti-Ce binary oxide to produce hydroperoxide complexes, which enabled an efficient transformation of Sb(III) to the less toxic Sb(V) (τ < 2 s) at neutral pH. The impact of important operational parameters was assessed and optimized, and system efficacy could be maintained over a wide pH range and long-term operation. An optimum detoxification efficiency of > 90% was achieved using lake water spiked with Sb(III) at 500 μg/L. The results showed that Ti/Ce-hydroperoxo surface complexes were the dominant species responsible for the non-radical oxidation of Sb(III) based on extensive experimental evidences and advanced characterizations. This study provides a robust and effective strategy for the detoxification of water containing Sb(III) and other similar heavy metal ions by integrating state-of-the-art advanced oxidation processes, electrochemistry and nano-filtration technology.
A series of multi-(phenylthio)porphyrinato Ni(ò) compounds were synthesized without the participation of transition metal catalysts. All of these products were well characterized by 1H NMR, 13C NMR and HRMS. Structures of three typical compounds were further confirmed by X-ray single crystal diffraction. Remarkable red shifts were observed in UVɃvis absorption spectra of multi-(phenylthio)porphyrinato Ni(ò) compounds which meet well with the electrochemical data. DFT calculation indicates that the phenylthio groups have strong effects on the frontier orbitals of these molecules. The order of a1u-like and a2u-like orbitals mainly distributed in porphyrin moiety is often inversed in energy when multi-phenylthio groups are attached.
Bimetallic nanoparticles modified hollow-structured nanoporous carbons (NPCs) have been fabricated via a convenient one-step carbonizing strategy derived from covalent organic framework. The Pd/Fe/NPCs, Pt/Fe/NPCs and Rh/Fe/NPCs were obtained and can be used as Fenton-like catalysts with good stability and reusability. The catalytic activity was evaluated by the degradation of 2, 4-dichlorophenl (2, 4-DCP). These fabricated bimetallic catalysts exhibited much higher catalytic activity than Fe/NPCs at room temperature. The enhancement of catalytic ability was benefited from synergetic catalytic effect of bimetallic nanoparticles and accelerated mass transfer of hollow structure. Additionally, the enhanced catalytic mechanism of bimetallic catalysts was studied in detail and the reasonable reaction pathway was proposed. Besides, the bimetallic catalysts were successfully used for degradation of 2, 4-DCP in actual industrial wastewater and the removal efficiency could reach 74.3% within 120 min, which demonstrated the promising potential application of bimetallic catalysts in the removal of pollutants in environment.
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