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The wide application of lithium-ion batteries (LIBs) for electric vehicles forebodes a future decommissioning tide of spent LIBs. Therefore, the recycling of spent LIBs has garnered significant attention, primarily due to the scarcity of resources and the detrimental effects of environmental pollution. However, traditional recycling technologies such as pyrometallurgy and hydrometallurgy methods are limited by their high energy consumption, high pollution, and complicated separation processes. Herein, we propose a novel and general approach to convert a series of spent LiNi1−x−yCoxMnyO2 (NCM) cathodes into Ni–Co–Mn hydroxide (NCM-OH) catalysts for the oxygen evolution reaction (OER) using deep eutectic solvents to extract valuable metals, followed by an in situ precipitation process using oxalic acid and a final self-templating process in an alkaline solution. The NCM-OH catalyst obtained from the spent LiNi0.33Co0.33Mn0.33O2 cathode is found to possess a nanoflake-assembled microrod structure with a large surface area (385.8 m2 g−1) and high porosity, which is endowed with abundant active sites and gas channels for the electrocatalytic reaction and mass transfer process. As a result, the NCM-OH catalyst for the oxygen evolution reaction exhibits a low overpotential of 273 mV at a current density of 10 mA cm−2 with a Tafel slope of 50.46 mV dec−1 as well as satisfactory stability. The effect of the composition on the catalytic performance is also evaluated by comparing different Ni1−x−yCoxMny hydroxide catalysts derived from commercially prevailing spent cathodes. This work provides a promising strategy for recycling spent LIBs into electrocatalyst materials for the OER. [ABSTRACT FROM AUTHOR]

Establishing efficient synthetic pathways for microbial production of biochemicals is often hampered by competing pathways and insufficient precursor supply. Compartmentalization in cellular organelles can isolate biosynthetic pathways from competing pathways, and thus provide a more compact and conducive environment for biosynthesis. Herein, the farnesyl diphosphate biosynthetic pathway and α-bisabolene synthase were compartmentalized in the yeast Yarrowia lipolytica peroxisome to enable high-level α-bisabolene production. Along with compartmentalization of the α-bisabolene biosynthesis pathway, a systems metabolic engineering approach that comprises mediating product export with an efflux pump, optimizing the gene copy numbers of rate-limiting enzymes, balancing the distribution of the common precursor acetyl-CoA between native lipid biosynthesis and heterologous α-bisabolene production, improving ATP and acetyl-CoA supply, and dynamic regulation of peroxisomes was then employed to further enhance the bisabolene production. Consequently, the optimized engineered strain produced 3028.9 mg L−1 α-bisabolene from waste cooking oil as the sole carbon source through shake flask cultivation. Finally, fed-batch fermentation was performed to accomplish α-bisabolene production at 15.5 g L−1, the highest ever reported for α-bisabolene from an engineered microbe. Taken together, this work lays the foundation for peroxisome engineering of Y. lipolytica, towards the production of α-bisabolene in a highly sustainable manner. [ABSTRACT FROM AUTHOR]

The exploitation of two-dimensional (2D) ferrovalley materials is of great significance in promoting the development of novel information storage devices, which is garnering increasing interest nowadays. However, the currently discovered 2D ferrovalley materials are very limited, and some of them still suffer from the drawback of small valley splitting, which seriously hinders their application in valleytronics. Herein, using first-principles calculations, we predict a promising 2D ferrovalley material, Janus monolayer GdBrI, which harbors sizable valley splitting and the anomalous valley Hall effect (AVHE). Monolayer GdBrI is a stable ferromagnetic semiconductor with an easy magnetization plane and magnetic transition temperature of 264.5 K. When the magnetization orientation is toward the z direction, valley polarization with a large splitting of 120.4 meV is achieved in the valence band due to the synergetic effect between the magnetic exchange interaction and spin–orbit coupling. The valley-contrasting Berry curvature gives rise to the AVHE in the monolayer. The magnitude of valley splitting can be continuously tuned by varying the magnetization orientation, biaxial strain and perpendicular electric field. These findings offer Janus monolayer GdBrI as a potential candidate for spintronic and valleytronic applications. [ABSTRACT FROM AUTHOR]

A two-dimensional (2D) multifunctional material, which couples multiple physical properties together, is both fundamentally intriguing and practically appealing. Here, based on first-principles calculations and tight-binding (TB) model analysis, the possibility of regulating the valley-contrasting physics and nontrivial topological properties via ferroelectricity is investigated in monolayer AsCH2OH. Reversible electric polarization is accessible via the rotation operation on the ligand. The broken inversion symmetry and the spin–orbit coupling (SOC) would lead to valley spin splitting, spin–valley coupling and valley-contrasting Berry curvature. More importantly, the reversal of electric polarization can realize the nonvolatile control of valley-dependent properties. Besides, the nontrivial topological state is confirmed in the monolayer AsCH2OH, which is robust against the rotation operation on the ligand. The magnitude of polarization, valley spin splitting and bulk band gap can be effectively modulated by the biaxial strain. The H-terminated SiC is demonstrated to be an appropriate candidate for encapsulating monolayer AsCH2OH, without affecting its exotic properties. These findings provide insights into the fundamental physics for the coupling of the valley-contrasting phenomenon, topological properties and ferroelectricity, and open avenues for exploiting innovative device applications. [ABSTRACT FROM AUTHOR]

Molybdenum selenide (MoSe2), a promising anode material for sodium ion batteries (SIBs), has generated intensive scientific interest due to its high theoretical capacity and favorable conversion kinetics. Nevertheless, its practical applications are seriously restricted by the volume variation, inferior structural stability and dissolved poly-selenides. Herein, we report dual carbon protected MoSe2 (MoSe2@NC@rGO) and the intrinsic mechanism for its enhanced sodium storage performance. Organic–inorganic hybrid Mo3O10(C2H10N2) (MoOx-EDA) is used as a self-sacrificing precursor. The synthesis process involves self-assembly of MoOx-EDA with functionalized graphene oxide (GO) and subsequent thermal selenization. The dual protection carbon layers can block the poly-selenide shuttling, promote electron transfer and buffer the huge volume change. When evaluated as an anode material for SIBs, the optimized MoSe2@NC@rGO-200 electrode delivers a high reversible specific capacity of 447 mA h g−1 at 100 mA g−1 and maintains an appreciable capacity of 281 mA h g−1 at 5 A g−1. Moreover, a capacity of 360 mA h g−1 is retained after 200 cycles at 1 A g−1 with no obvious capacity decay. A full-battery configuration coupled with the Na3V2(PO4)2/C cathode exhibits an average operating potential of 1.8 V and good cycling performance. Such a dual carbon-confined approach can also be extended to other electrode materials with large volume swelling. [ABSTRACT FROM AUTHOR]

A versatile coating strategy, which is suitable for the anti-corrosion and anti-fouling modification of chemically distinct substrates, is crucial in many industries. The immobilization of zwitterionic polymers onto the surface has been proven to be an excellent approach for the improvement of antibiofouling potency. However, the anti-corrosion property has not always been considered simultaneously. Herein, a layer-by-layer (LBL) zwitterionic surface modification strategy was proposed: the surface was first coated with a polydopamine (PDA) layer for anti-corrosion; then, by self-assembling a monolayer of 3-aminopropyl triethoxysilane (APTES), the anti-corrosion ability was further enhanced and the efficiency of grafting was improved; thereafter, by immobilizing the zwitterionic polysulfobetaine (PSB) polymer brush layer, the surface could effectively repel biofouling. The surface chemical composition and morphology characterization was performed by using attenuated total reflectance Fourier transform infrared (ATR-FTIR) spectroscopy, scanning electron microscopy (SEM), atomic force microscopy (AFM), and water contact angle measurements, demonstrating that the modification was stepwise introduced onto the surface. The thickness of coating was observed and measured by SEM cross-sectional analysis. In vitro studies revealed that the PSB coated surfaces dramatically reduced the adhesion of bovine serum albumin (BSA), bovine plasma fibrinogen (Fg), bovine γ-globulin (γ-GL), the mixture of these proteins, fibroblasts, E. coli and S. aureus with superior cytocompatibility and hemocompatibility. Moreover, the electrochemical impedance spectroscopy and acidic corrosion studies indicated that an excellent and durable anti-corrosion property was established successfully on the surfaces of stainless steel, cotton textile and wood plates, confirming the feasibility of the LBL surface modification strategy. Significantly, this LBL surface chemistry may be widely applied for the modification of other materials, such as biosensors, biomedical implants and/or devices, and marine equipment. [ABSTRACT FROM AUTHOR]

Near-infrared (NIR) irradiation responsive drug delivery systems have many advantages, which have attracted extensive interest from researchers. In this study, a NIR-triggered drug release system was established by grafting upper critical solution temperature (UCST) polymers on the surface of hollow mesoporous silica nanoparticles (HMSNs) followed by treatment with the photothermal conversion agent indocyanine green (ICG). The as-prepared UCST polymers showed the clearing temperature of 45 °C, which were advantageous to serve as gatekeepers in the physiological environment (37 °C). Under NIR irradiation, the temperature of the solution was elevated above the clearing point due to the presence of ICG; consequently, the collapsed UCST polymer chains became more hydrophilic; this resulted in the exposure of the mesoporous channels of the HMSNs and achievement of a burst drug release. Moreover, this NIR-responsive delivery system showed good biocompatibility and high anticancer efficiency towards the MCF-7 cancer cells upon exposure to NIR irradiation. In addition, a synergistic effect of thermal and chemo treatment has been achieved by the application of NIR irradiation since cancer cells are more vulnerable to high temperatures than normal cells. [ABSTRACT FROM AUTHOR]

As a promising conversion-type anode material, iron sulfide has been widely studied. However, due to its huge volume expansion during repeated lithiation/delithiation, iron sulfide tends to pulverize and form aggregates upon cycling, which greatly hinders its application in high performance lithium ion batteries as a durable anode material. Herein, a strategy for synthesizing and stabilizing iron sulfide nanosheets with a robust titanium oxide nanofiber interior support is proposed. The hierarchical nanostructured composite anode material was successfully synthesized by the electrospinning technique and subsequent sulfurization. The size of the iron sulfide nanosheets can be easily tuned by adjusting the composition of the reacting agents and/or the sulfurization temperature. Electrochemical results reveal that the composite delivers a reversible capacity of 591 mA h g−1 at a current density of 0.1 A g−1 after 100 cycles and exhibits excellent long-term cycling stability at 0.5 A g−1 and 1 A g−1 as well. Furthermore, when being paired with LiFePO4, the as-synthesized composite also delivers promising full-cell performance, showing its potential in serving as a competitive candidate anode material in lithium-ion batteries for power applications. Moreover, this method also opens up an avenue for modifying and improving other conversion-type anode materials. [ABSTRACT FROM AUTHOR]

Realizing simultaneous high breathability and humidity stability of on-skin devices is still a critical challenge. Herein, we develop a breathable, humidity-ultrastable and degradable sensory skin by using cowskin as a skin-friendly substrate. Cowskin has similar constituents and hierarchical structure to human skin, which supplies the sensory skin with remarkable breathability and exceptional water-vapor permeability as high as 3714 g m−2 d−1, two orders of magnitude larger than conventional polydimethylsiloxane film (80 g m−2 d−1). Sensory skin features a distinct sensing mechanism that employs cowskin as a cross-scale deformable 3D sensory substrate for achieving high skin-conformability, detection sensitivity (0.144 kPa−1), fast response (200 ms), high operational stability (15 000 cycles) and wide sensory range from human physiological signals to high strain movements. Because sensory skin relies on a 3D sensory structure, its sensing ability is, therefore, free from a localized structure damage, including scratches, cuts and abrasions. Sensory skin is further processed to be superhydrophobic, gaining unaffected sensory capability under extremely humid conditions (50 °C and relative humidity of 82%) with exceptional breathability (1087 g m−2 d−1). The collagenous substrate of sensory skin is fully degradable. These outstanding advantages make sensory skin a powerful skin-friendly on-skin device. [ABSTRACT FROM AUTHOR]

Stannous based anode materials have been extensively studied for sodium ion batteries due to their high theoretical capacities. However, the large volume changes upon repeated cycling always cause their structural pulverization and capacity fading. Herein, we report the fabrication of S-doped porous hollow carbon confined SnS nanospheres particles and their good electrochemical performance as an anode material for sodium ion batteries. Unlike previous reports, stanniferous solid carbonaceous nanospheres are novelly prepared by a hydrothermal process, and they can be converted into yolk–shell structured Sn@C nanospheres after thermal annealing in a H2/Ar atmosphere. The subsequent sulfidation process can produce S-doped carbon confined SnS hollow nanospheres with high porosity. The obtained SnS@SPC nanospheres possess a large Brunauer–Emmett–Teller (BET) surface area of 135.8 m2 g−1. As an anode material for sodium ion batteries, the obtained yolk–shell SnS@SPC exhibits a high reversible capacity of 512 mA h g−1 at 100 mA g−1 and good cycling stability. The void space between the carbon shell and the SnS yolk can accommodate the volume changes during the charge/discharge process. Meanwhile, the porous carbon shell can serve as a conductive skeleton and a reservoir for the electrolyte. [ABSTRACT FROM AUTHOR]

Simultaneous removal of emulsified water and surfactant from surfactant-stabilized emulsions remains challenging. In the present investigation, we developed a new conceptual emulsion separation membrane by using multiple walled carbon nanotubes (MWCNTs) as heterogeneous competitive adsorption-type demulsifying sites, and a 3D hierarchically fibrous structured collagen fiber membrane (CFM) as a nonporous substrate with high flux and strong mechanical strength. The MWCNTs inside the CFM served as heterogeneous demulsifying sites responsible for competitive adsorption to surfactants stabilized with emulsion droplets, which not only realized effective demulsification but also completely solved the problem of surfactant contamination in the filtrate. The nonporous substrate of the CFM ensured high separation flux and also suppressed the fouling problem frequently observed in conventional size-sieving porous membranes, which successfully separated a variety of mixed nonionic surfactant-stabilized water-in-oil nano- and micro-emulsions under gravity, with separation efficiency high up to 99.994% and flux high up to 1051 L m−2 h−1, which showed apparent advantage compared with commercial polyamide and polytetrafluoroethylene porous membranes with low fluxes of 64 and 35 L m−2 h−1, respectively. The membrane also retained high separation efficiency and flux after 10 cycles of separation or 30 cycles of strong abrasion with sandpaper. Notably, our membrane successfully separated mixed nonionic surfactant-stabilized emulsions with an extremely high viscosity of 33.2–76.2 mPa s, with separation efficiency higher than 99.98% and a high flux of 395–1299 L m−2 h−1 bar−1, while the polyamide and polytetrafluoroethylene porous membranes failed to separate these viscous emulsions. [ABSTRACT FROM AUTHOR]

Flexible hybrid electrodes with high electronic conductivity and porosity have attracted great attention for energy storage and conversion systems. Herein, we report the fabrication of a porous graphitic carbon wrapped MnO/Ni microsphere network (MnO/Ni/CNF) by a combined solvothermal and electrospinning method followed by stabilization and carbonization processes. Carbon nanofibers which link porous MnO/Ni/C microspheres function as both a 3D conductive network and a current collector for the flexible composite electrode. Meanwhile, the porous MnO/Ni microspheres are coated with porous graphene-like carbon layers, further improving the electronic conductivity and facilitating the electrolyte penetration. When directly utilized as an anode material for LIBs, the MnO/Ni/CNF electrode exhibits excellent electrochemical performances, including high reversible capacity, good cycle stability and rate capability. The as-prepared flexible electrode delivers a capacity of 534.5 mA h g−1 at 200 mA g−1 after 100 cycles (based on the whole electrode mass) and possesses a capacity retention of 95.7% even after long-term 600 cycles at 1 A g−1, suggesting its promising applicability in lithium ion batteries as a flexible binder-free anode. [ABSTRACT FROM AUTHOR]

A Sb-containing Anderson-based polyoxomolybdate cluster, [(CH3)4N]4H8[Na5Sb3(Sb2Mo12O57)]·17H2O [1; (CH3)4N+ = TMA+], has been successfully synthesized by using an aqueous solution method and structurally characterized. In particular, UV-Vis spectroscopy has been employed to elucidate the stability of the polyoxoanions. Under mild conditions, the catalyst demonstrates high activity and selectivity for the sulfoxidation of various sulfides in the presence of hydrogen peroxide. For example, thioanisole undergoes up to 100% conversion and 100% sulfone selectivity at 25 °C in aqueous solution. [ABSTRACT FROM AUTHOR]

Heterogeneous structures with binary chemical compositions could achieve unique chemical properties by modification of the components and interface engineering. Meanwhile, hollow microspheres with complex interiors have been extensively studied in energy storage and conversion systems due to their possibility of adjusting the electrochemical performances. In this work, we report the reliable preparation of heterogeneous (NiO)x(NiS)1−x (0 ≤x≤ 1) multi-shelled hollow microspheres derived from carbon sphere@nickel precursor templates. The structural evolution of the multiple shells is carefully studied. Moreover, the effect of sulfurization extent of the (NiO)x(NiS)1−x compounds on the electrochemical performance is also explored. As electrode materials for supercapacitors, the heterogeneous (NiO)0.1(NiS)0.9 multi-shelled hollow microspheres exhibit the best electrochemical performances among a series of nickel oxide/sulfide compounds. The (NiO)0.1(NiS)0.9 sample can deliver a high specific capacitance of 1063 F g−1 at 2 A g−1. Even at a high current density of 50 A g−1, the electrode can still retain a high specific capacitance of 486 F g−1 after 10 000 cycles. Furthermore, a (NiO)0.1(NiS)0.9‖active carbon asymmetric supercapacitor (ASC) exhibits a specific capacitance of 58.5 F g−1 at 2 A g−1 in 2 M KOH solution. The superior electrochemical performances can be attributed to the careful composition regulation and the stable multi-shelled structure. [ABSTRACT FROM AUTHOR]

Hollow structured vanadium pentoxide microspheres with multiple double-walled shells were fabricated from solid vanadium oxide precursors through ascorbic acid-assisted solvothermal growth. The interiors of the vanadium oxide microspheres and number of the novel double-walled shells can be readily controlled by adjusting the combustion of solid vanadium oxide precursors. The formation mechanism of the unique structures is elucidated and attributed to the diffusion controlled oxidation process in air. The obtained V2O5 hollow spheres with triple double-walled shells show improved electrochemical performance compared to single-shelled V2O5 hollow microspheres as electrode materials for lithium-ion batteries. [ABSTRACT FROM AUTHOR]

Polymeric carbon nitride quantum dots (CNQDs) with an average size of approximately 2.5 nm were prepared directly from melamine via a one-step molten salt method. The formation mechanism and photoluminescence (PL) properties of the resulting CNQDs were investigated by means of TEM, XRD and PL spectroscopy. The CNQDs can be dispersed in water to form a transparent colloidal solution and emit blue PL with excellent photostability. Interestingly, upon addition of CuCl2 and NaHCO3 in turn, the PL of CNQDs can be turned off and on accordingly. Taking advantage of the on–off–on PL response, the CNQDs can be used as a fluorescent security ink for information coding, encryption and decryption, indicating their promising application in data security and high-level anti-counterfeiting fields. [ABSTRACT FROM AUTHOR]

Herein, a new colorimetric strategy based on polymer nanoparticles (PNPs) and Au nanoparticles (AuNPs) is developed to detect heparin (Hep). The cationic PNPs can directly induce the aggregation of AuNPs, which are stabilized by negatively charged coating of citrate ions, and hence the absorption peak of AuNPs moves to 675 nm corresponding with a color change from wine red to blue. However, the negatively charged Hep competes with AuNPs and binds to PNPs, hindering the interaction between PNPs and AuNPs. As a result, the absorption band of AuNPs blue shifts and the color turns to red again. The reaction can be completed within 10 min, and the color variation produced by 150 nM of Hep can be distinguished by the naked eye. In addition, this strategy also shows good selectivity and sensitivity, and the linear range of Hep is from 10 to 400 nM with detection limit of 2.5 nM. Finally, this colorimetric assay has been applied to measure Hep in Hep sodium injection and human serum samples with satisfactory recoveries. [ABSTRACT FROM AUTHOR]

Hollow structures with complex interiors are promising to endow electroactive materials with fascinating physical properties, such as low mass density, large surface area and high permeability. Meanwhile, the construction of hollow structures with binary chemical compositions could further enhance the resultant electrochemical properties. Herein, we reported a designed synthesis of multi-shelled CoO/Co9S8 hollow microspheres by calcining a hollow microsphere precursor with S powder in argon gas (Ar). The inherent characteristic of cobalt(ii) mono-oxide can benefit the electrochemical activity, while the cobalt sulfide component could improve the electrical conductivity of this cobalt-based composite material. These multi-shelled hollow structures are proved to possess a porous texture with a relatively large specific surface area (SSA = 43.1 m2 g−1), which could provide more active sites for electrochemical reactions. As a result, the as-prepared multi-shelled CoO/Co9S8 hollow microspheres exhibit an enhanced specific capacitance and excellent rate performance when evaluated as electrode materials for hybrid supercapacitors. [ABSTRACT FROM AUTHOR]

For bulk-heterojunction polymer solar cells (BHJ-PSCs), appropriate concentration distribution and phase separation of the donor and acceptor molecules within the polymer:fullerene blends are crucial for effective exciton dissociation and charge transportation. Herein, we introduce a selectively dissolvable solvent 2-chlorophenol to finely tune the vertical concentration distribution of fullerene within the photoactive layer. The morphology of the photoactive layer is investigated by atomic force microscopy (AFM), Scanning Kelvin Probe Microscopy (SKPM), transmission electron microscopy (TEM) and water contact angle (WCA) measurements. The optimized three-dimensional concentration distribution is further investigated by time-of-flight secondary-ion mass spectroscopy (TOF SIMS). To investigate the effect of vertical concentration distribution on the photovoltaic performance, conventional and inverted structured PSCs are fabricated. Compared with the control device without modulation of the concentration distribution, the short circuit current density (Jsc) increased from 13.19 to 18.50 mA cm−2 and the power conversion efficiency (PCE) increased from 6.18% to 10.15% for the inverted device with 2-chlorophenol flush treatment due to the greatly enhanced charge transportation and reduced exciton recombination. Our findings indicate that simple 2-chlorophenol flush treatment is a feasible and effective way to acquire an optimal vertical composition profile of photoactive blends for high performance inverted PSCs. [ABSTRACT FROM AUTHOR]

Improving the light absorption of the photoactive layer is a key issue to enhance the photovoltaic performance of polymer solar cells (PSCs). Herein, the transfer-matrix method is used to model the absorption spectra and optical electric field distribution within the multilayer stack of conventional and inverted PSCs based on PBDTTT-C-T:PC70BM blends. The simulation results show that the short-circuit current density (Jsc) of the devices increases with increasing photoactive layer thickness and an oscillation can be observed for both conventional and inverted devices. By applying an inverted architecture, higher optical electric field energy dissipation in the photoactive layer can be realized, and higher Jsc can be achieved. Guided by the simulation results, high performance conventional and inverted PSCs based on PBDTTT-C-T:PC70BM are experimentally fabricated. Comparing the external quantum efficiency (EQE) with the absorption spectra for both devices, the increased Jsc for the inverted device is attributed mainly to the enhanced absorption. The conventional device shows a power conversion efficiency (PCE) of 7.09%, while the inverted device shows enhanced Jsc and FF, and the PCE reaches 8.81%, which is increased by 24.3% in comparison with that of the conventional device. The agreement between the modeling and experimental results confirms the directive function of optical modeling on device design and optimization. [ABSTRACT FROM AUTHOR]

In this work, hierarchical three-dimensional (3D) β-Na0.33V2O5 microspheres have been synthesized for the first time by a simple solvothermal reaction with subsequent annealing treatment. The hierarchical microspheres are self-assembled from nanosheet subunits during the solvothermal process. Simultaneously, various hierarchical microspheres with different subunits can be produced by altering the solvothermal solution. After annealing in air, the solvothermal product can be converted into β-Na0.33V2O5 with a well-retained structure. As cathode materials for lithium ion batteries, the as-prepared 3D microspheres exhibit high capacity and good rate capability. The superior electrochemical performance is attributed to the unique three-dimensional hierarchical microstructures, which mimic the advantages of nano- and micro-structures. [ABSTRACT FROM AUTHOR]

This study describes a general strategy using norepinephrine (NE) as a stable anchor for the immobilization of enzyme onto three-dimensionally ordered macroporous (3DOM) silica. Penicillin G acylase (PGA) was chosen as a model enzyme. The effect of pH and temperature on the activity of PGA@PN–SiO2 (PGA immobilized on poly(norepinephrine)-modified 3DOM silica) was investigated. The operational stability, storage stability and kinetic properties of the PGA@PN–SiO2 were also examined. Compared with free PGA and PGA@SiO2 (PGA immobilized on blank 3DOM silica through physical adsorption), the stabilities of PGA@PN–SiO2 were improved significantly. PGA@PN–SiO2 retained high activity during the hydrolysis in a continuous packed-bed reactor (PBR) after 30 catalytic cycles, which demonstrated that PGA@PN–SiO2 can bear endurance of continuous catalysis. The method presented in this study has broad potential for immobilizing enzymes and other biomolecules. [ABSTRACT FROM AUTHOR]

This research provides a novel approach for introducing a CF3CH2 group onto aromatic rings using Pd(OAc)2/palladacycle as a catalyst for the Suzuki cross-coupling reaction of CF3CH2OTs (OTs = 4-methylbenzene sulfonate) with arylboronic acids. [ABSTRACT FROM AUTHOR]

The water oxidation reaction is the bottleneck problem of the artificial photosynthetic system. In this work, the mechanism of water oxidation catalyzed by a mononuclear copper complex in alkaline conditions was studied by density functional calculations. Firstly, a water molecule coordinating with the copper center of the complex (Cu ii , 1) generates Cu ii -H 2 O (2). 2 undergoes two proton-coupled electron transfer processes to produce intermediate (4). The oxidation process occurs mainly on the ligand moiety, and 4 (˙L-Cu ii -O˙) can be described as a Cu ii center interacting with a ligand radical antiferromagnetically and an oxyl radical ferromagnetically. 4 is the active species that can trigger O-O bond formation via the water nucleophilic attack mechanism. This process occurs in a step-wise manner. The attacking water transfers one of the protons to the HPO 4 2- coupled with an electron transfer to the ligand radical, which generates a transient OH˙ interacting with the oxyl radical and H 2 PO 4 - . Then the O-O bond is formed through the direct coupling of the oxo radical and the OH radical. The triplet di-oxygen could be released after two oxidation processes. According to the Gibbs free energy diagram, the O-O bond formation was suggested to be the rate-limiting step with a calculated total barrier of 19.5 kcal mol -1 . More importantly, the copper complex catalyzing water oxidation with the help of a redox non-innocent ligand and HPO 4 2- was emphasized., Competing Interests: The authors declare no competing financial interest., (This journal is © The Royal Society of Chemistry.)

A novel tungstophosphate H 12 Na 4 K 3 [{Fe 5 O 5 (OH) 2 (OAc) 2 } 2 {W 2 -O 2 (OH)}{P 2 W 14 O 54 } 2 ]·36H 2 O (1) containing an unprecedented [{Fe 5 O 5 (OH) 2 (OAc) 2 } 2 {W 2 O 2 (OH)}] unit has been successfully obtained and characterized by IR, TGA, magnetic susceptibility measurements and single-crystal X-ray diffraction. It shows a decameric Fe III molecular assembly formed through two {Fe 5 O 23 } subunits bridged by a {W 2 O 3 } motif.

This research provides a novel approach for introducing a CF3CH2 group onto aromatic rings using Pd(OAc)2/palladacycle as a catalyst for the Suzuki cross-coupling reaction of CF3CH2OTs (OTs = 4-methylbenzene sulfonate) with arylboronic acids.

The first TiCl(4)-mediated condensation of secondary amides with aldehydes and ketones has been achieved. The reaction proceeds at room temperature and is complete within 5 h in most cases. The optimized procedure used 5 equiv of an amine base hinting that the in situ activation of both the amide and the Lewis acid is required. The reaction affords polysubstituted (E)-enamides.

LiCoO(2) material is recovered from spent lithium-ion batteries and investigated as anode materials for Ni/Co power batteries for the first time. LiCoO(2) electrodes with a small amount of S-doping display excellent electrochemical properties. The electrochemical reactions occurring on M0 electrodes during the first several cycles and after being activated are proposed, respectively. A function mechanism of S powder on M10 electrode is also proposed.

Chiral, non-racemic 1,2,3-trisubstituted ferrocene derivatives are accessible from monosubstituted ferrocenes through two sequential ortho-deprotonation reactions; removal of the central substituent gives 1,3-disubstituted ferrocenes.