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Titanium silicalite-1 (TS-1) zeolites are the efficient and clean catalysts for producing the important epoxidized products in the epoxidation of alkenes. Herein, the size-controlled synthesis of the TS-1 (TS-1#ACh) catalysts was carried out by introducing acetylcholine (ACh) as a crystal growth regulator. Large-sized TS-1#0.1ACh catalysts show excellent tetrahedrally coordinated framework Titanium, which provides good catalytic performance and stability in the epoxidation of [Detail] ...
Wave energy is inexhaustible renewable energy. Making full use of the huge ocean wave energy resources is the dream of mankind for hundreds of years. Nowadays, the utilization of water wave energy is mainly absorbed and transformed by electromagnetic generators (EMGs) in the form of mechanical energy. However, waves usually have low frequency and uncertainty, which means low power generation efficiency for EMGs. Fortunately, in this slow current and random direction wave case, the triboelectric nanogenerator (TENG) has a relatively stable output power, which is suitable for collecting blue energy. This article summarizes the main research results of TENG in harvesting blue energy. Firstly, based on Maxwell’s displacement current, the basic principle of the nanogenerator is expounded. Then, four working modes and three applications of TENG are introduced, especially the application of TENG in blue energy. TENG currently used in blue energy harvesting is divided into four categories and discussed in detail. After TENG harvests water wave energy, it is meaningless if it cannot be used. Therefore, the modular storage of TENG energy is discussed. The output power of a single TENG unit is relatively low, which cannot meet the demand for high power. Thus, the networking strategy of large-scale TENG is further introduced. TENG’s energy comes from water waves, and each TENG’s output has great randomness, which is very unfavorable for the energy storage after large-scale TENG integration. On this basis, this paper discusses the power management methods of TENG. In addition, in order to further prove its economic and environmental advantages, the economic benefits of TENG are also evaluated. Finally, the development potential of TENG in the field of blue energy and some problems that need to be solved urgently are briefly summarized.
The massive conversion of resourceful biomass to carbon nanomaterials not only opens a new avenue to effective and economical disposal of biomass, but provides a possibility to produce highly valued functionalized carbon-based electrodes for energy storage and conversion systems. In this work, biomass is applied to a facile and scalable one-step pyrolysis method to prepare three-dimensional (3D) carbon nanotubes/mesoporous carbon architecture, which uses transition metal inorganic salts and melamine as initial precursors. The role of each employed component is investigated, and the electrochemical performance of the attained product is explored. Each component and precise regulation of their dosage is proven to be the key to successful conversion of biomass to the desired carbon nanomaterials. Owing to the unique 3D architecture and integration of individual merits of carbon nanotubes and mesoporous carbon, the as-synthesized carbon nanotubes/mesoporous carbon hybrid exhibits versatile application toward lithium-ion batteries and Zn-air batteries. Apparently, a significant guidance on effective conversion of biomass to functionalized carbon nanomaterials can be shown by this work.
Cellulose has a wide range of applications in many fields due to their naturally degradable and low-cost characteristics, but few studies can achieve cellulose-nanofibers by conventional electrospinning. Herein, we demonstrate that the freestanding cellulose-based carbon nanofibers are successfully obtained by a special design of electrospinning firstly, pre-oxidation and high-temperature carbonization (1600 °C), which display a superior electrical conductivity of 31.2 S·cm–1 and larger specific surface area of 35.61 m2·g–1 than that of the polyacrylonitrile-based carbon nanofibers (electrical conductivity of 18.5 S·cm–1, specific surface area of 12 m2·g–1). The NiCo2O4 nanoflake arrays are grown uniformly on the cellulose-based carbon nanofibers successfully by a facile one-step solvothermal and calcination method. The as-prepared cellulose-based carbon nanofibers/NiCo2O4 nanoflake arrays are directly used as electrodes to achieve a high specific capacitance of 1010 F·g–1 at 1 A·g–1 and a good cycling stability with 90.84% capacitance retention after 3000 times at 10 A·g–1. Furthermore, the all-solid-state symmetric supercapacitors assembled from the cellulose-based carbon nanofibers/NiCo2O4 deliver a high energy density of 62 W·h·kg–1 at a power density of 1200 W·kg–1. Six all-solid-state symmetric supercapacitors in series can also power a ‘DHU’ logo consisted of 36 light emitting diodes, confirming that the cellulose-based carbon nanofiber is a promising carbon matrix material for energy storage devices.
The multifunctional films was prepared by blending chitosan and nano-ZnO with purple tomato anthocyanins or black wolfberry anthocyanins. The properties of films functioned by anthocyanins source and nano-ZnO content were studied. It was found purple tomato anthocyanins showed more significant color change against pH than black wolfberry anthocyanins. The nano-ZnO were widely dispersed in matrix and enhanced the compatibility of anthocyanins with chitosan. However, the anthocyanins source influenced the properties of the films more slightly than nano-ZnO addition. The tensile strength, antioxidant and antibacterial effects of the chitosan films dramatically increased after cooperated by nano-ZnO and anthocyanins, which also enhanced with increase of nano-ZnO content, whereas the elongation at break of the composite films decreased. Especially, the anthocyanin and nano-ZnO promoted the antibacterial activity of films synergistically. Composite films made from black wolfberry anthocyanins exhibited higher mechanical performance than those made from purple tomato anthocyanins but weaker antibacterial effects. The purple tomato anthocyanins/chitosan and nano-ZnO/purple tomato anthocyanins/chitosan films effectively reflected pork spoilage, changing their colors from dark green to brown, indicating the potential for applications in active and intelligent food packaging.
A Fe2O3−Bi2MoO6 heterojunction was synthesized via a hydrothermal method. Scanning electron microscopy, transmission electron microscopy, energy-dispersive X-ray, powder X-ray diffraction, Fourier transform infrared spectroscopy and ultra-violet−visible near-infrared spectrometry were performed to measure the structures, morphologies and optical properties of the as-prepared samples. The various factors that affected the piezocatalytic property of composite catalyst were studied. The highest rhodamine B degradation rate of 96.6% was attained on the 3% Fe2O3−Bi2MoO6 composite catalyst under 60 min of ultrasonic vibration. The good piezocatalytic activity was ascribed to the formation of a hierarchical flower-shaped microsphere structure and the heterostructure between Fe2O3 and Bi2MoO6, which effectively separated the ultrasound-induced electron–hole pairs and suppressed their recombination. Furthermore, a potential piezoelectric catalytic dye degradation mechanism of the Fe2O3−Bi2MoO6 catalyst was proposed based on the band potential and quenching effect of radical scavengers. The results demonstrated the potential of using Fe2O3−Bi2MoO6 nanocomposites in piezocatalytic applications.
Designing advanced and cost-effective electrocatalytic system for nitric oxide (NO) reduction reaction (NORR) is vital for sustainable NH3 production and NO removal, yet it is a challenging task. Herein, it is shown that phosphorus (P)-doped titania (TiO2) nanotubes can be adopted as highly efficient catalyst for NORR. The catalyst demonstrates impressive performance in ionic liquid (IL)-based electrolyte with a remarkable high Faradaic efficiency of 89% and NH3 yield rate of 425 μg·h−1·mgcat.−1, being close to the best-reported results. Noteworthy, the obtained performance metrics are significantly larger than those for N2 reduction reaction. It also shows good durability with negligible activity decay even after 10 cycles. Theoretical simulations reveal that the introduction of P dopants tunes the electronic structure of Ti active sites, thereby enhancing the NO adsorption and facilitating the desorption of *NH3. Moreover, the utilization of IL further suppresses the competitive hydrogen evolution reaction. This study highlights the advantage of the catalyst−electrolyte engineering strategy for producing NH3 at a high efficiency and rate.
In this study, a simple and effective method was proposed to improve the electrocatalytic ability of overoxidized poly(3,4-ethylenedioxythiophene)-overoxidized polypyrrole composite films modified on glassy carbon electrode for rutin and luteolin determination. The composite electrode was prepared by cyclic voltammetry copolymerization with LiClO4-water as the supporting electrolyte. The peak current of rutin and luteolin on the composite electrode gradually decreased or even disappeared with the increase in the positive potential limit. After incubation in NaOH–ethanol solution with a volume ratio of 1:1, the composite electrodes prepared at positive potential limit greater than 1.5 V exhibited enhanced differential pulse voltammetry peak currents, reduced charge transfer resistance, larger effective specific surface area and higher electron transfer rate constant. The composite electrode prepared in the potential range of 0–1.7 V showed optimal electrocatalytic performance. The X-ray photoelectron spectroscopy results indicated that the content of –SO2/–SO and –C=N– groups in the composite film increased significantly after incubation. Further, the Raman spectra and Fourier transform infrared spectra revealed that the thiophene ring structure changed from benzene-type to quinone-type, and the quinone-type pyrrole ring was formed. The electrocatalytic mechanism of the composite film was proposed based on the experimental results and further verified by Density Functional Theory calculation.
Since lithium iron phosphate cathode material does not contain high-value metals other than lithium, it is therefore necessary to strike a balance between recovery efficiency and economic benefits in the recycling of waste lithium iron phosphate cathode materials. Here, we describe a selective recovery process that can achieve economically efficient recovery and an acceptable lithium leaching yield. Adjusting the acid concentration and amount of oxidant enables selective recovery of lithium ions. Iron is retained in the leaching residue as iron phosphate, which is easy to recycle. The effects of factors such as acid concentration, acid dosage, amount of oxidant, and reaction temperature on the leaching of lithium and iron are comprehensively explored, and the mechanism of selective leaching is clarified. This process greatly reduces the cost of processing equipment and chemicals. This increases the potential industrial use of this process and enables the green and efficient recycling of waste lithium iron phosphate cathode materials in the future.
This work introduces a deep-learning network, i.e., multi-input self-organizing-map ResNet (MISR), for modeling refining units comprised of two reactors and a separation train. The model is comprised of self-organizing-map and the neural network parts. The self-organizing-map part maps the input data into multiple two-dimensional planes and sends them to the neural network part. In the neural network part, residual blocks enhance the convergence and accuracy, ensuring that the structure will not be overfitted easily. Development of the MISR model of hydrocracking unit also benefits from the utilization of prior knowledge of the importance of the input variables for predicting properties of the products. The results show that the proposed MISR structure predicts more accurately the product yields and properties than the previously introduced self-organizing-map convolutional neural network model, thus leading to more accurate optimization of the hydrocracker operation. Moreover, the MISR model has smoother error convergence than the previous model. Optimal operating conditions have been determined via multi-round-particle-swarm and differential evolution algorithms. Numerical experiments show that the MISR model is suitable for modeling nonlinear conversion units which are often encountered in refining and petrochemical plants.
Development of a titanium silicalite-1 (TS-1) catalyst with good crystallinity and a four-coordinate Ti framework is critical for efficient catalytic oxidation reaction under mild conditions. Herein, a size-controlled TS-1 zeolite (TS-1 0.1ACh (acetylcholine)) was synthesized via steam-assisted crystallization by introducing acetylcholine as a crystal growth modifier in the preparation process, and TS-1 0.1ACh was also employed in epoxidations of different substrates containing C=C double bonds. The crystalline sizes of the as-synthesized TS-1 0.1ACh catalysts were controlled with the acetylcholine content, and characterization results showed that the particle sizes of highly crystalline TS-1 0.1ACh zeolite reached 3.0 μm with a good Ti framework. Throughout the synthetic process, the growth rate of the crystals was accelerated by electrostatic interactions between the connected hydroxyl groups of the acetylcholine modifier and the negatively charged skeleton of the pre-zeolites. Furthermore, the TS-1 0.1ACh catalyst demonstrated maximum catalytic activity, good selectivity and high stability during epoxidation of allyl chloride. Importantly, the TS-1 0.1ACh catalyst was also highly versatile and effective with different unsaturated substrates. These findings may provide novel, easily separable and large TS-1 catalysts for efficient and clean industrial epoxidations of C=C double bonds.
In situ encapsulation is an effective way to synthesize enzyme@metal–organic framework biocatalysts; however, it is limited by the conditions of metal–organic framework synthesis and its acid-base stability. Herein, a biocatalytic platform with improved acid-base stability was constructed via a one-pot method using bismuth-ellagic acid as the carrier. Bismuth-ellagic acid is a green phenol-based metal–organic framework whose organic precursor is extracted from natural plants. After encapsulation, the stability, especially the acid-base stability, of amyloglucosidases@bismuth-ellagic acid was enhanced, which remained stable over a wide pH range (2–12) and achieved multiple recycling. By selecting a suitable buffer, bismuth-ellagic acid can encapsulate different types of enzymes and enable interactions between the encapsulated enzymes and cofactors, as well as between multiple enzymes. The green precursor, simple and convenient preparation process provided a versatile strategy for enzymes encapsulation.
