Immobilization of penicillin G acylase on paramagnetic polymer microspheres with epoxy groups

Paramagnetic polymer microspheres were synthesized by the inverse suspension polymerizationmethod through polymerization of glycidyl methacrylate,ally glycidyl ether and methacrylamide onthe surface of silica‐coated Fe3O4nanoparticles using N,N’‐methylene‐bis(acrylamide)as across‐linking agent.Penicillin G acylase(PGA)was covalently immobilized on the surface of theparamagnetic microspheres by reacting the amino groups of the PGA molecules with the epoxygroups of the paramagnetic polymer microspheres.The effect of the SiO2coating and the amount ofparamagnetic Fe3O4nanoparticles on the initial activity and the operational stability of the immobilizedPGA was investigated.The results indicated that SiO2played an important role in the polymerization process and paramagnetic polymer microspheres with a SiO2‐coated Fe3O4nanoparticles mass content of7.5%are an optimal support material for PGA immobilization.Immobilized PGA on the paramagnetic polymer microspheres shows a high initial activity of430U/g(wet)and retains99%of its initial activity after recycling10times.Furthermore,immobilized PGA exhibits high thermal stability,pH stability and excellent reusability,which can be rapidly recycled by the aid of magnet.?2018,Dalian Institute of Chemical Physics,Chinese Academy of Sciences.Published by Elsevier B.V.All rights reserved.

Highly efficient cobalt-doped carbon nitride polymers for solvent-free selective oxidation of cyclohexane

Selective oxidation of saturated hydrocarbons with molecular oxygen has been of great interest in catalysis, and the development of highly efficient catalysts for this process is a crucial challenge. A new kind of heterogeneous catalyst, cobalt-doped carbon nitride polymer(g-C_3N_4),was harnessed for the selective oxidation of cyclohexane. X-ray diffraction, Fourier transform infrared spectra and high resolution transmission electron microscope revealed that Co species were highly dispersed in g-C_3N_4 matrix and the characteristic structure of polymeric g-C_3N_4 can be retained after Co-doping, although Co-doping caused the incomplete polymerization to some extent. Ultraviolet-visible, Raman and X-ray photoelectron spectroscopy further proved the successful Co doping in g-C_3N_4 matrix as the form of Co(Ⅱ)-N bonds. For the selective oxidation of cyclohexane, Co-doping can markedly promote the catalytic performance of g-C_3N_4 catalyst due to the synergistic effect of Co species and gC_3N_4 hybrid. Furthermore, the content of Co largely affected the activity of Co-doped g-C_3N_4 catalysts, among which the catalyst with 9.0 wt%Co content exhibited the highest yield(9.0%) of cyclohexanone and cyclohexanol, as well as a high stability. Meanwhile, the reaction mechanism over Co-doped g-C_3N_4 catalysts was elaborated.

Gas-phase epoxidation of propylene by molecular oxygen over Ag-Cu-Cl/BaCO_3 catalyst:Effects of Cu and Cl loadings

Ag‐Cu‐Cl/BaCO3 catalysts with different Cl and Cu loadings, prepared by the reduction deposition impregnation method, were investigated for gas‐phase epoxidation of propylene by molecular oxygen and characterized by X‐ray diffraction, X‐ray photoelectron spectroscopy and O2 temperatureprogrammed desorption. Ag‐Cu‐Cl/BaCO3 catalyst with 0.036 wt% Cu and 0.060 wt% Cl exhibitedthe highest catalytic performance for gas‐phase epoxidation of propylene by molecular oxygen. Apropylene oxide selectivity of 83.7% and propylene conversion of 1.2% were achieved under thereaction conditions of 20% C3H6‐10% O2‐70% N2, 200 °C, 0.1 MPa and 3000 h?1. Increasing the Clloading allowed Ag to ensemble easier, whereas changing the Cu loading showed little effect on Agcrystallite size. The appropriate Cl loading of Ag‐Cu‐Cl/BaCO3 catalyst can reduce the dissociationadsorption of oxygen to atomic oxygen species leading to the combustion of propylene to CO2, whichbenefits epoxidation of propylene by molecular oxygen. Excessive Cl loading of Ag‐Cu‐Cl/BaCO3catalyst decreases propylene conversion and propylene oxide selectivity remarkably because of Clpoisoning. The appropriate Cu loading of Ag‐Cu‐Cl/BaCO3 catalyst is efficient for the epoxidation ofpropylene by molecular oxygen, and an excess Cu loading decreases propylene oxide selectivitybecause the aggregation of Cu species increases the exposed surfaces of Ag nanoparticles, whichwas shown by slight increases in atomic oxygen species adsorbed. The appropriate loadings of Cu and Cl of Ag‐Cu‐Cl/BaCO3 catalyst are important to strike the balance between molecular oxygen and atomic oxygen species to create a favorable epoxidation of propylene by molecular oxygen.

Advancement in Layered Transition Metal Dichalcogenide Composites for Lithium and Sodium Ion Batteries

With an ever increasing energy demand and environmental issues, many state-of-the-art nanostructured electrode materials have been developed for energy storage devices and they include batteries, supercapacitors and fuel cells. Among these electrode materials, L-TMD （layered transition metal dichalcogenide） nanosheets （especially, S （sulfur） and Se （selenium） based dichaleogenides） have received a lot of attention due to their intriguing layered structure for enhanced electrochemical properties. L-TMD composites have recently been investigated not only as a main charge storage specie but also, as a substrate to hold the active specie. This review highlights the recent advancements in L-TMD composites with 0D （0-dimensional）, 1 D, 2D, 3D and various forms of carbon structures and their potential applications in LIB （lithium ion battery） and SIB （sodium ion battery）.

Enhanced high-temperature mechanical properties of laser-arc hybrid additive manufacturing of Al-Zn-Mg-Cu alloy via microstructure control

Recently,rapid and cost-effective additive manufacturing solutions for lightweight aluminum alloys with excellent high-temperature mechanical properties have been increasingly in demand.In this study,we combined laser-arc hybrid additive manufacturing with solution and artificial aging treatments to achieve Al-Zn-Mg-Cu alloy with favorable high-temperature strength via microstructure control.Hydrogen pores became the major defect in the as-deposited and heat-treated specimens.The continuous distribution of eutectics with hard-brittle characteristics at the grain boundaries was destructed following heat treat-ment.High-densityηprecipitates were uniformly dispersed in the heat-treated Al-Zn-Mg-Cu alloy,whereas appeared coarsened and dissolved at 473 K,owing to the rapid diffusion of Zn and Mg.The average 0.2%yield strength(318±16 MPa)and ultimate tensile strength(362±20 MPa)at 473 K af-ter heat treatment were enhanced by approximately 58%and 51%,respectively,compared to those of the as-deposited specimen.In addition,theηprecipitates contributed to lattice distortions and strain fields,which prevented dislocation motion and increased slip deformation resistance at high temper-atures.The as-deposited specimen exhibited intergranular fracture at 473 K,with cracks preferring to propagate along the aggregated eutectics.However,crack propagation proceeded in the sections with more pores in the heat-treated specimen.Our approach may provide a valid option for achieving alu-minum alloys with excellent high-temperature mechanical properties.

Research of cycloaliphatic epoxy resin and silicone rubber composite insulator interface based on four-electrode system and temperature rise model

Interface degradation between mandrel and sheath can cause a decrease in insulation performance and mechanical strength of composite insulators.In this study,the interface ageing properties of cycloaliphatic epoxy resin and silicone rubber composite insulator were compared.A water diffusion test was adopted to simulate the composite insulator ageing in a hot and humid environment.A four-electrode system was built to detect leakage current at different locations(mandrel,sheath and interface),which is an important basis for evaluating insulator performance.The ageing degree of insulator could be quantitatively characterised by leakage current change.It was found that the infiltrated moisture had a great effect on insulation performance.Based on the water absorption test result,the interface performance of two insulators was mainly influenced by their sheath sealing quality.As an auxiliary evaluation method,temperature rise during the test was recorded using an infrared camera.The experiment results showed that interface degradation was the main factor for the insulation performance decrease of silicone rubber composite insulators.However,insulation level reduction of the cycloaliphatic epoxy resin was caused by the wet sheath.In addition,a model for temperature rise of cycloaliphatic epoxy resin insulators was proposed based on good correspondence between sheath material and insulation.The model incorporated multiple processes such as ageing and heating of insulators,and it can predict the early temperature rise well.

High-performance Li-ion batteries based on graphene quantum dot wrapped carbon nanotube hybrid anodes

Since Akira Yoshino first proposed the usage of the carbonaceous materials as an anode of lithium ion batteries(LIBs)in 1985,carbonaceous materials such as graphite and graphene have been widely considered as LIB anodes.Here,we explored the application of novel carbonaceous UB anodes incorporating graphene quantum dots(GQDs).We fabricated a freestanding all-carbon electrode based on a porous carbon nanotube(CNT)sponge via a facile in-situ hydrothermal deposition technique,creating coaxial structure of GQD-coated CNTs(GQD@CNTs)through electrostatic interaction and n-n stacking with tunable loading and functionalization.This hybrid structure combined conductive CNTs with highly active GQDs,in which GQDs with predesigned functional groups provided massive storage sites for Li ions and the 3D CNT frameworks avoided the agglomeration of GQDs,together contributing to a high specific capacity(700 mAh·g^-1 at 100 mA·g^-1 after 100 cycles)and rate performance.Even at a high current density of 1,000 mA·g^-1,the reversible specific capacity remained at 483 mAh g-1 after 350 cycles.In particular,the mechanism study demonstrated the important role of oxygen functional groups of GQDs in promoting the performance of the LIB anodes by controlled grafting of GQDs onto various porous-carbon and metal-foam based structures.

Analysis of photoluminescence behavior of high-quality single-layer MoS2

The ability to tailor and enhance photoluminescence (PL) behavior in two-dimensional (2D) transition metal dichalcogenides (TMDCs) such as molybdenum disulfide (MoS2) is significant for pursuing optoelectronic applications.To achieve this,it has been essential to obtain high-quality single-layer MoS2 and fully explore its intrinsic PL performance.Here,we fabricate single-layer MoS2 by a thermal vapor sulfurization method in which a pre-deposited molybdenum trioxide (MoO3) thin film is sulfurized over a short period (for several minutes) to turn into MoS2.These as-grown MoS2 crystals show quite strong PL,which is about one order of magnitude higher than that of chemical-vapor-deposited MoS2.Temperature- and power-dependent spectroscopy measurements disclose the apparent influence of sulfur (S) vacancies on the PL behavior and the noticeable free-to-bound exciton recombinations in the luminescence process.The fact that PL intensity of the sample in vacuum sharply lowered down relative to in air reveals that the high PL is facilitated by molecular adsorption on S vacancies in air.And multi-channel decay processes coupled with S vacancies are revealed in the time-resolved PL spectroscopy.In our work,single-layer MoS2 with high PL is synthesized and its defect-induced PL features are analyzed,which is of great importance for developing advanced nano-electronics and optoelectronics based on 2D structures.

Catalytic wet oxidation of N,N-dimethyl formamide over ruthenium supported on CeO_2 and Ce_(0.7)Zr_(0.3)O_2 catalysts

A series of Ru supported on CeO_2 and Ce_(0.7)Zr_(0.3)O_2(CeZrO) was prepared by incipient-wet impregnation method and investigated in the catalytic wet oxidation of N,N-dimethyl formamide(DMF) in batch reactor. The physicochemical property of the catalysts was characterized by Brunauer-Emmett-Teller(BET), X-ray diffraction(XRD), H_2 temperature-programmed reduction(H_2-TPR), X-ray photoelectron spectroscopy(XPS) and thermogravimetry(TG). Compared with 3%Ru/CeO_2, 3%Ru/Ce_(0.7)Zr_(0.3)O_2 catalyst exhibits much higher performance for DMF degradation due to the promotion of Ru dispersion and the transfer of active oxygen, and 99% DMF conversion and 97% COD elimination are obtained at 453 K,2.5 MPa oxygen pressure after 5 h. The reaction mechanism of DMF degradation was suggested. The carbonaceous species deposition and oxidation of Ru can be responsible for catalyst deactivation. And the catalyst activity can be recovered by air calcination and H_2 reduction.

Al2O3 supported hybrid Pd-CeO2 colloidal spheres and its enhanced catalytic performances for methane combustion

Fabrication of novel nano-catalyst with improved activity and stability has been a hot topic in heterogeneous catalysis. Herein a novel approach was designed to synthesize Pd-CeO2 colloidal assembled spheres(CASs) in one-pot fashion. The Pd clusters were encompassed by the CeO2 nanocrystals with a high dispersity. Based on this hybrid structure, the Pd/ceria interface area can be greatly improved. After Pd-CeO2 CASs was supported on γ-Al2O3, its catalytic activity for CH4 combustion was evaluated. The result shows that Al2O3 supported Pd-CeO2 CASs exhibits an improved catalytic activity and stability,compared to the Pd/CeO2 catalyst prepared by impregnation method. The results of several characterization techniques indicate that the enhanced catalytic activity of Al2O3 supported Pd-CeO2 CASs can be attributed to the more interfacial Pd-O-Ce species and the more surface active oxygen species.