Latest ArticlesSupramolecular transformations of coordination cage or capsule have received much attention recently, which help elucidate this natural self-assembly behavior in biological systems. The current study describes the first supramolecular transformation of titanium–organic coordination capsule triggered by phenol (and H3PO3). The structural alterations are accompanied by the reconstruction of 5-coordinated Ti centers to 6-coordinated ones. Meanwhile, different amounts of encapsulated phenol guest molecules can be identified, dependent on the sizes of the obtained cavities. In addition, they display much better visible light absorption and air stability than the isopropanol stabilized ones.
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.
In this study, Mn catalysts have been designed based on manganese oxide octahedral molecular sieve (OMS-2) supports to optimize the catalytic activity in the degradation of organic pollutants. Herein, two different synthetic strategies: Pre-incorporation vs. wet-impregnation have been employed to synthesize [PW]-OMS-2 and [PW]/OMS-2. For [PW]-OMS-2, energy dispersive X-ray spectroscopy (EDX) confirmed that dispersed granular phosphotungstic acid attached and located at the surface of OMS-2, meanwhile some W atoms have been doped into frameworks of OMS-2. However, for [PW]/OMS-2, the W atoms cannot enter the OMS-2 frameworks. A correlation has been established between the different synthetic strategies and catalytic activities. The [PW]-OMS-2 is the most highly effective and stable over than [PW]/OMS-2 and OMS-2 itself for the organic pollutants removal. This may be caused not only by the synergetic effect of [PW] and OMS-2, but also by doping W into frameworks of OMS-2. Therefore, this work provides a new environmentally-friendly and heterogeneous PMS activator and it may be put into practice to degrade organic pollutants.
In power storage technology, ion exchange is widely used to modify the electronic structures of electrode materials to stimulate their electrochemical properties. Here, we proposed a multistep ion exchange (cation exchange and anion exchange) strategy to synthesize amorphous Ni-Co-S and β-Co(OH)2 hybrid nanomaterials with a hollow polyhedron structures. The synergistic effects of different components and the remarkable superiorities of hollow structure endow Ni-Co-S/Co(OH)2 electrode with outstanding electrochemical performance, including ultra-high specific capacity (1440.0 C/g at 1 A/g), superior capacitance retention rate (79.1% retention at 20 A/g) and long operating lifespan (81.4% retention after 5000 cycles). Moreover, the corresponding hybrid supercapacitor enjoys a high energy density of 58.4 Wh/kg at the power density of 0.8 kW/kg, and a decent cyclability that the capacitances are maintained at 80.8% compared with the initial capacitance. This research presents a high-performance electrode material and provides a promising route for the construction of electrode materials for supercapacitors with both structural and component advantages.
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.
Fabrication of well-designed heterojunctions is an extraordinarily attractive pathway for boosting the photocatalytic activity toward CO2 photoreduction. Herein, a novel kind of nanosheet-based intercalation hybrid coupled with CdSe quantum dots (QDs) was successfully fabricated by a facile solvothermal method and served as photocatalyst for full-spectrum-light-driven CO2 reduction. Ultra-small CdSe QDs were rationally in-situ introduced and coupled with lamellar ZnSe-intercalation hybrid nanosheet, resulting in the formation of CdSe QDs/ZnSe hybrid heterojunction. Significantly, the concentration of Cd2+ could change directly the crystallinity and micromorphology of ZnSe intercalation hybrid, which in turn would impact on the photocatalysis activity. The optimized CdSe QDs/ZnSe hybrid-5 composite demonstrated a considerable CO yield rate of the 25.6 μmol g-1 h-1 without any additional cocatalysts or sacrificial agents assisting, making it one of the best reported performance toward CO2 photoreduction under full-spectrum light. The elevated CO2 photoreduction activity could be attributed to the special surface heterojunction, leading to improving the ability of light absorption and promoting the separation/transfer of photogenerated carriers. This present study developed a new strategy for designing inorganic-organic heterojunctions with enhanced photocatalyst for CO2 photoreduction and provided an available way to simultaneously mitigate the greenhouse effect and alleviate energy shortage pressure.
Hydrogen sulfide (H2S) is a signaling molecule that plays important roles in biological systems. The exploration of H2S as a new drug release trigger and its related fluorescent theranostic system is crucial for cancer bio-imaging and therapy. Herein, we designed a new two-photon ratiometric fluorescent theranostic prodrug (compound 1) and studied its spectroscopic properties and application in in vivo imaging. Compound 1 specifically reacted with H2S and released the free active therapeutic component of 7-ethyl-10-hydroxycamptothecin, which was accompanied with a red-shift fluorescence emission signal from 460 nm to 545 nm. The exogenous and endogenous H2S in living cells were imaged by compound 1 under one-photon and two-photon excitation. Furthermore, compound 1 monitored the H2S concentration changes in Caenorhabditis elegans by fluorescence imaging. Additionally, it showed effective drug release activation in situ tumor with exogenous and endogenous H2S as the trigger. The H2S-sensitive activation and drug-release properties highlight the potential of theranostic compound 1 in future cancer treatment and therapy.
Prussian whites (PWs) with a three-dimensional framework can accommodate the insertion and extraction of ions with large radius, which have been widely used in potassium ion batteries. However, PWs show the poor cycling performance and inferior rate ability because of high coordinated water. In this work, PWs with different water content were synthesized via a coprecipitation method by controlling the reaction temperature. The sample with low-coordination water prohibits the best electrochemical performance. It shows a high capacity of 120.5 mAh/g at 100 mA/g for potassium-ion batteries (KIBs). It also exhibits a good rate performance, displaying a capacity of 73.2 mAh/g at 500 mA/g.
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.
Constructing a heterojunction photocatalyst is a significant method to enhance photocatalytic activity because it can promote the separation of photogenerated carriers. Herein, amorphous/crystalline contact Bi2S3/Bi4O7 heterostructure was successfully synthesized by in-situ sulfidation of Bi4O7. The amorphous Bi2S3 is diffused on the surface of Bi4O7 rod, enhancing the visible light response and improving the transport of photogenerated carriers. Various characterizations confirm that the rapid separation of photogenerated carriers leads to increased photocatalytic performance. The optimized Bi2S3/Bi4O7 heterostructure photocatalyst (BiS-0.15) exhibits the highest Cr(VI) reduction (0.01350 min−1) and RhB oxidation (0.08011 min−1) activity, which is much higher than that of pure Bi4O7 and Bi2S3/Bi4O7 mixture under visible light irradiation. This work provides new insights into the construction of efficient novel photocatalysts.
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