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Direct sustainable conversion of hydrogen sulfide (H2S) enables collaborative recovery of H and S resources via a metal-enhanced microwave plasma strategy, avoiding the hydrogen waste in the traditional Claus process. However, the metal size effect on microwave plasma property, the optimal process parameters, and the enhancement mechanism remain unclear in H2S conversion. Herein, the optimal tungsten needle (diameter: 1 mm, length: 60 mm, and tip angle: 10°) is experimentally proven for intensifying microwave discharge in multi-mode cavities. Theoretical calculations and plasma distribution reveal that the optimized tungsten needle achieves the ideal coupling with the microwave field, exhibiting extreme electric field augmentation around the needle tip. Tungsten-needle intensifies microwave-sustained plasma, realizing 40.2 % (90.1 %) conversion of 100 % (10 %) concentration H2S to H2 at a low microwave power of 300 W with a good stability of 30 hrs. Low power, large flow rate, and high H2S concentration are beneficial for improving energy efficiency. The excitation of microwave plasma is accompanied by a massive generation of highly energetic electrons. The direct high-energy electron-H2S collision contributes a lot to H2S splitting, especially for high-concentration H2S. In-situ optical emission spectroscopy confirms the vital S and H radicals in the plasma. The free radical reactions triggered by electron collisions are responsible for the production of H2 and S. This work opens an avenue to sustainable and low-carbon hydrogen production from the direct conversion and utilization of H2S.
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Faced with the increasing volume of retired lithium-ion batteries (LIBs), recycling and reusing the spent graphite (SG) is of great significance for resource sustainability. Here, a facile method for transforming the SG into a carbon framework as well as loading Fe2O3 to form a composite anode with a sandwich structure is proposed. Taking advantage of the fact that the layer spacing of the spent graphite naturally expands, impurities and intercalants are eliminated through microwave thermal shock to produce microwave-puffed graphite (MPG) with a distinct three-dimensional structure. Based on the mechanism of microwave-induced gasification intercalation, a Fe2O3-MPG intercalation compound (Fe2O3-MPGIC) anode material was constructed by introducing iron precursors between the framework layers and subsequently converting them into Fe2O3 through annealing. The Fe2O3-MPGIC anode exhibits a high reversible capacity of 1000.6 mAh g-1 at 200 mA g-1 after 100 cycles and a good cycling stability of 504.4 mAh g-1 at 2000 mA g-1 after 500 cycles. This work can provide a reference for the feasible recycling of SG and development of high-performance anode materials for LIBs.
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The corrosion behavior of 20G and TP347H materials was investigated in molten LiCl-NaCl-KCl salt. The corrosion rates of these materials in molten chloride salt are high and are strongly affected by the alloying surface oxide formation. The 20G shows uniform surface corrosion with almost no protective oxide formation on the surface. In contrast, the austenitic steel TP347H exhibits better corrosion resistance in molten chloride salts due to its high Cr content. Owing to the highly corrosive nature of molten chloride salts, the Cl- in molten salt could react with oxides and alloy, inducing intergranular corrosion of austenitic steel in molten chloride salt environments.
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It needs to be improved the conversion efficiency and stable operation of conventional pyrolysis with high-temperature flue gas heating (HFH). Herein, a new radiative heating (RH) pyrolysis method is proposed. Experimental studies are carried out on a self-made radiation pyrolysis pilot plant to investigate the effects of different factors (pyrolysis final temperature, residence time, and carrier gas volume) on product distribution. The results show that with the increase of pyrolysis temperature, the yield of the gas phase consistently increases, and the proportion of CH4 and H2 in the pyrolysis gas reaches 62.31% at 700 °C. The yield of the liquid phase increases and then decreases. The recovery rate of pyrolysis oil achieves 68.07% when the pyrolysis temperature is 600 °C with main components of ketones and unsaturated hydrocarbon compounds. The yield of the solid phase consistently decreases. The RH in this work generates more pyrolysis gas in the pyrolysis process and alleviates the effects of fouling layers on the continuous operation of the equipment which has guiding significance for the efficient resource utilization of oil sludge.
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Calor , Aguas del Alcantarillado , Calefacción , Pirólisis , TemperaturaRESUMEN
To understand the physical phase structural variation and activation pathway of the active component during the catalytic reduction of pyrite (FeS2)-based catalysts, multiple methods, including X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and high-temperature in situ XRD, were applied to characterize the catalyst and reaction process. The reaction mechanism was simulated and verified using density functional theory. The results indicated that pyrite-based catalysts promote the CO reduction of SO2 to S through the dynamic transformation of three phases (FeS2, Fe7S8, and FeS), in which S-vacancy formation is the most important step. As the critical temperature for the reaction of FeS2 and CO was initiated at approximately 525 °C, the active component's physical phase structure and activation pathway could be controlled by adjusting the temperature.
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Hierro , Azufre , Temperatura , CatálisisRESUMEN
CO emission is a critical issue of industrial processes such as steel-smelting, cement manufacturing, and waste incineration. Catalytic oxidation based on Cu-Mn binary catalysts shows great potential for efficient removal of CO, whereas their practical applicability is limited by the inferior low-temperature catalytic activity and the high catalyst cost owing to a substantial quantity of Cu. In this study, doping graphene is designed to adjust the electron transfer capability to improve the low-temperature catalytic activity as well as reduce the amount of Cu, and thereby Cu1Mn10 catalysts doped with slight amounts of graphene (x%G-Cu1Mn10, x is 1â¼5) were fabricated. It was found that the introduction of graphene could form effective electron transport channels to enhance the intermetallic interaction and oxygen vacancy generation, thus improving the low-temperature catalytic performance of the Cu1Mn10 catalyst. Among all the catalysts, 4%G-Cu1Mn10 exhibited the highest activity, achieving CO conversion of 92% at 110 °C at a weight hourly space velocity of 120,000 mL/(gâh). The introduction of graphene also enabled the catalyst with excellent catalytic activity and stability at a relative humidity of 70%. Attractively, 4%G-Cu1Mn10 can be further loaded into the polyester fabric, presenting great application potentials in the effective elimination of CO during the dust removal process since the flue gas temperature in the dust collector is just around the T90% and the catalyst that is inside of fabric fiber rather than on the fabric surface can be rarely influenced by the dust. In general, doping graphene provides a facile method to enhance the low-temperature activities of the Cu-Mn binary catalysts and cut down the use of valuable Cu, showing great application potential.
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A large amount of pharmaceutical industry waste (PIW) was inevitably produced every year, and the PIW can be degraded by high temperature reaction to form porous structures. The study proposed an innovative pathway to valorize PIW with hydrothermal carbonization (HTC) coupled with alkali etching (AE). Without adding any additives, magnetic hydrochar could be generated with rough surface topography and suitable specific surface area (SBET) by this method. Effects of HTC conditions and alkaline solution concentrations on the physicochemical and adsorption properties of PIW were investigated, and adsorption mechanism was explored. Based on evaluations of the magnetism, cyclic regeneration, and heavy metal leaching properties of the products, the feasibility of preparing magnetic adsorbents with solid waste by HTC coupled AE was established. The alkaline etching pharmaceutical industry waste (AEPIW) hydrochar showed the highest SBET (54.64 m2/g) after the PIW was treated by 260 °C for 2 h plus 1 mol/L KOH. The removal rate of methylene blue (MB) could exceed 90% and the saturated magnetization was ~8 emu/g. The proposed new method was able to convert the low-value solid industrial waste into high-performance hydrochar-based magnetic adsorbents, which was tested to have a capability to efficiently and sustainably remove organic pollutants from water.
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Colorantes , Residuos Industriales , Temperatura , Residuos Sólidos , Álcalis , Fenómenos Magnéticos , CarbonoRESUMEN
The reutilization of spent cathode materials plays a key role in the sustainable development of Li-ion battery technology. However, current recycling approaches generally based on hydro-/pyrometallurgy fail to cater to Co-free cathodes (e.g., LiFePO4, or LFP) owing to high consumption and secondary contamination. Here, a sustainable process is proposed for the revival of defective LFP cathodes through the synergy of defect-targeted healing and surface modification. Li deficiency and Fe oxidation of cathodes are precisely repaired by solution-based relithiation; meanwhile, 3D-interconnected porous carbon networks (3dC) are in-situ constructed with the intervention of salt template during annealing, which enhances the rate performance and electronic/ionic conductivity, by providing more convenient migration channels for Li ions and controlling carbon hybridization. Nitrogen is also doped via induction of urea to fabricate advanced nanohybrid rLFP@3dC-N. New cells using rLFP@3dC-N as cathode exhibit a reversible capacity of up to 169.74 and 141.79 mAh g-1 at 0.1 and 1C, respectively, with an excellent retention rate of over 95.7% at 1C after 200 cycles. Impressively, a high capacity of 107.18 mAh g-1 is retained at 5C. This novel concepts for Li replenishment and the construction of ion-transfer channels as well as conductive networks facilitate the regeneration of spent LFP and the optimization of its high-rate performance.
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Carbono , Porosidad , Conductividad Eléctrica , ElectrodosRESUMEN
MnOx has received widespread attention in low-temperature catalytic oxidation of VOCs, however, the synergy effect of MnOx and support on the VOCs catalytic ozonation were rarely studied. In this study, five different MnOx/X (X: MCM-41, 13X, ZSM-5, HY, USY) were synthesized and found their support greatly affect the catalytic oxidation activity. MnOx/MCM-41 presents the largest specific surface area, pore volume and unique surface morphology, and thereby provides more sites for MnOx loading and VOCs adsorption. Moreover, MnOx/MCM-41 presents a high proportion of Mn3+, which helps to enhance the ion exchange capability, and thus promotes the regeneration of oxygen vacancies. Furthermore, a part of Mn was proved to be introduced into the MCM-41 lattice, which can promote the electron transfer between the active components and the support, and thereby effectively improve the surface electronic properties of the catalyst. The toluene catalytic experiments showed that MnOx/MCM-41 exhibited the best catalytic activity, presenting complete degradation of O3 and VOCs at room temperature. In addition, 5 wt%MnOx/MCM-41 exhibited better catalytic activity than other loading, and its higher surface oxygen species endowed it with strong water resistance and stability. In-situ DRIFTs indicated that toluene was initially oxidized into benzyl alcohol during the adsorption process, and then decomposed to intermediate products (benzaldehyde, phenolate, etc.) during the catalytic ozonation process, and finally oxidized to carbon dioxide. In conclusion, the supply of loading sites and the improvement of interfacial electron transfer are the manifestations of the synergy between the support and MnOx, leading to the promotion of the catalytic ozonation of VOCs.
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Ozono , Tolueno , Adsorción , Catálisis , Oxidación-Reducción , OxígenoRESUMEN
Highly active mesoporous Fe-Mn-Ce catalysts with high specific surface area (SBET) were synthesized by a modified precipitation process for catalyzing toluene oxidation. The Fe0.85Mn0.1Ce0.05 catalyst presents richer surface oxygen species (OS), a higher proportion of Mn4+ and Ce4+, a higher concentration of lattice defects and oxygen vacancies, the highest Oads/Olatt ratio, and a superior low-temperature redox property compared with the Fe-Mn binary oxide and Fe2O3 and MnO2 catalysts. The properties contribute to a high catalytic activity to achieve T90% of toluene conversion at 264 °C and 185 °C with a gas hourly space velocity (GHSV) at 180,000 and 20,000 mL/(gâh), respectively. The introduction of a slight quantity of Ce and Mn onto the Fe2O3 catalyst is the key to enhancing the synergistic effect of the lattice OS and surface-adsorbed oxygen, contributing to the activation oxidation procedure of toluene. In-situ DRIFTS analysis reveals that the rich oxygen vacancy concentration of catalysts accelerates the key steps for the generation and activation of oxidized products. These catalysts with rich oxygen vacancies can efficiently diminish the accumulation of a small number of the intermediary species (phenolate, C6H5-OH) produced during the catalytic oxidation of toluene.
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This study aimed to explore the influence of activated carbon, oily sludge pyrolysis residue, and biochar and their contents on the distribution of three-phase products of oily sludge subjected to microwave pyrolysis. A microwave reaction system, refinery gas analyzer, and chromatography-mass spectrometry were used to carry out the experiment and analyze the results. The results showed that all three additives reduced the yield of solid products and increased the yield of gas products. With an increase in the additive content, the volatile matter and moisture content in the pyrolysis residue greatly reduced. The content of CH4 and H2 in the pyrolysis gas increased with an increase in the additive content. When the amount of activated carbon was 20%, the H2 content reached a maximum (39.7%), and when the amount of biochar was 20%, the CH4 content reached a maximum (44.5%). All three additives increased the content of small molecules in the pyrolysis oil; when 10% activated carbon was added, the oil recovery rate reached up to 78.5%. The results of this study can guide the industrial application of microwave pyrolysis oily sludge.
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Pirólisis , Aguas del Alcantarillado , Calor , Microondas , AceitesRESUMEN
In this paper, a step-by-step classification algorithm based on double-layer SVM model is constructed to predict the secondary structure of proteins. The most important feature of this algorithm is to improve the prediction accuracy of α+ß and α/ß classes through transforming the prediction of two classes of proteins, α+ß and α/ß classes, with low accuracy in the past, into the prediction of all-α and all-ß classes with high accuracy. A widely-used dataset, 25PDB dataset with sequence similarity lower than 40%, is used to evaluate this method. The results show that this method has good performance, and on the basis of ensuring the accuracy of other three structural classes of proteins, the accuracy of α+ß class proteins is improved significantly.
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Análisis de Secuencia de Proteína/métodos , Máquina de Vectores de Soporte , Animales , Humanos , Conformación Proteica en Hélice alfa , Conformación Proteica en Lámina beta , Análisis de Secuencia de Proteína/normasRESUMEN
Interactions between microwaves and certain catalysts can lead to efficient, energy-directed convergence of a relatively dispersed microwave field onto the reactive sites of the catalyst, which produces thermal or discharge effects around the catalyst. These interactions form "high-energy sites" (HeS) that promote energy efficient utilization and enhanced in situ degradation of organic pollutants. This article focuses on the processes occurring between microwaves and absorbing catalysts, and presents a critical review of microwave-absorbing mechanisms. This article also discusses aqueous phase applications of relevant catalysts (iron-based, carbon-based, soft magnetic, rare earth, and other types) and microwaves, special effects caused by the dimensions and structures of catalytic materials, and the optimization and design of relevant reactors for microwave-assisted catalysis of wastewater. The results of this study demonstrate that microwave-assisted catalysis can effectively enhance the degradation rate of organic compounds in an aqueous phase and has potential applications to a variety of engineering fields such as microwave-assisted pyrolysis, pollutant removal, material synthesis, and water treatment.
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Microondas , Contaminantes Químicos del Agua/química , Contaminantes del Agua/química , Purificación del Agua/métodos , Catálisis , Contaminantes del Agua/análisis , Contaminantes Químicos del Agua/análisisRESUMEN
This study demonstrated rapid degradation of malachite green (MG) by a microwave (MW)-induced enhanced catalytic process with CoFe2O4-SiC foam. The catalyst was synthesized from CoFe2O4 particles and SiC foam by the hydrothermal method. X-ray diffraction and scanning electron microscopy techniques were used to confirm that CoFe2O4 particles were settled on the surface of SiC foam. In this experiment, a novel fixed-bed reactor was set up with this catalyst for a continuous flow process in a MW oven. The different parameters that affect the MW-induced degradation rate of MG were explored. The MW irradiation leads to the effective catalytic degradation of MG, achieving 95.01% degradation within 5 min at pH 8.5. At the same time, the good stability and applicability of CoFe2O4-SiC foam for the degradation process were also discussed, as well as the underlying mechanism. In brief, these findings make the CoFe2O4-SiC foam an excellent catalyst that could be used in practical rapid degradation of MG.
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Volatile organic compounds (VOCs) are air pollutants that pose a major concern, and novel treatment technologies must be continuously explored and developed. In this study, microwave-induced metal discharge was applied to investigate the destruction of acetone as a representative model VOC compound. Results revealed that metal discharge intensity largely depended on microwave output power and the number of metal strips. Microwave metal discharge exerted the distinct combined effects of intense heat, strong light, and plasma. In the case of MW without metal discharge, the decrease in acetone at 200â¯ppm was remarkably limited (approximately 5.5% (mol/mol)). By contrast, in the case of microwave-induced metal discharge, a considerably high destruction efficiency of up to 65% (mol/mol) was obtained at low concentrations. This finding highlights the potential of microwave-induced discharge for VOC removal. Initial assessment indicated that energy consumption can be acceptable.
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In this work, the properties of the CH4-CO2 reforming reaction over the Fe/SiC catalyst during the whole process were studied under microwave irradiation and the reaction process was analyzed by mass spectrometry and Fourier transfer infrared spectrometry in real time. The effects of microwave power on the gas composition, conversion of reactants, and selectivity of products in the reaction were investigated. It was found that the microwave dry reforming reaction can be divided into a rapid reaction stage, slow reaction stage, and reaction equilibrium stage. The conversion of reactants and selectivity of products in the slow reaction stage were both higher than 95% under 90â¯W/g. In the long-term (~50â¯h) stability test, a combination of SEM, XRD, BET, and TG analyses found that the catalyst activity did not reduce significantly and the amount of carbon deposits (which was mainly Cγ) was negligible (~0.78â¯wt%). The results indicate that the cheap Fe-based catalyst has good catalytic activity and stability under microwave irradiation and hence has a promising application.
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The pyrolytic characteristics of tyre powder treated under different microwave powers (300, 500, and 700 W) were studied via microwave thermogravimetric analysis. The product yields at different power levels were studied, along with comparative analysis of microwave pyrolysis and conventional pyrolysis. The feedstock underwent preheating, intense pyrolysis, and final pyrolysis in sequence. The main and secondary weight loss peaks observed during the intense pyrolysis stage were attributed to the decomposition of natural rubbers and synthetic rubbers, respectively. The total mass loss rates, bulk temperatures, and maximum temperatures were distinctively higher at higher powers. However, the maximum mass loss rate (0.005 s-1), the highest yields of liquid product (53%), and the minimum yields of residual solid samples (43.83%) were obtained at 500 W. Compared with conventional pyrolysis, microwave pyrolysis exhibited significantly different behaviour with faster reaction rates, which can decrease the decomposition temperatures of both natural and synthetic rubber by approximately 110 °C-140 °C.
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Calor , Microondas , Eliminación de Residuos , Goma , Termogravimetría/métodos , Residuos , Diseño de Equipo , Polvos , Termogravimetría/instrumentación , Residuos/análisisRESUMEN
Surface soil samples were collected every 36 km2 from Linyi City to study the residues, composition and origin, influencing factors, spatial distribution and environment quality characteristics of soil DDTs. Measurements were taken for DDTs, OrgC, N, etc. for all samples. The results indicated that the detectable rate of DDTs was 71. 75%, and the mean content of DDTs was 0. 035 µg.g-1. p,p'-DDT and p,p'-DDE were the predominant contaminant compounds, with mean concentrations of 0.033 µg.g-1 and 0.010 µg.g-1, and accounted for 60. 99% and 34. 62% of the detectable samples, respectively. The degradation rate of DDTs suggested that 58% surface soils were recently inputted, these newly inputted locations were especially distributed in the middle to south of the study area, meanwhile, p,p'-DDD/p,p'-DDE revealed that the degradation of DDTs was mainly under oxidizing condition, and o,p'-DDT/p,p'-DDT illustrated that 71. 37% DDTs in soils of the study area were concerned with technical DDTs sources. Besides, the correlation, analysis showed that the external factors affecting the distribution of DDTs included OrgC, N, C and pH etc. and the higher the p, p'-DDT proportion of DDTs, the greater the effect. The distribution of DDTs had an obvious point source characteristic, and significant concentration centers were located nearby the cities and counties, typically, the DDTs concentrations of middle to southern area were much higher. However, DDTs environmental quality assessment suggested that the pollution level was relatively low, and the soil was mainly classified into grade I or II, which accounted for 78. 95% and 21. 05% of the whole study area, respectively.
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Hidrocarburos Clorados/análisis , Residuos de Plaguicidas/análisis , Contaminantes del Suelo/análisis , Suelo/química , China , Ciudades , DDT/análisis , Diclorodifenil Dicloroetileno/análisis , Monitoreo del AmbienteRESUMEN
The structural class has become one of the most important features for characterizing the overall folding type of a protein and played important roles in many aspects of protein research. At present, it is still a challenging problem to accurately predict protein structural class for low-similarity sequences. In this study, an 18-dimensional integrated feature vector is proposed by fusing the information about content and position of the predicted secondary structure elements. The consistently high accuracies of jackknife and 10-fold cross-validation tests on different low-similarity benchmark datasets show that the proposed method is reliable and stable. Comparison of our results with other methods demonstrates that our method is an effective computational tool for protein structural class prediction, especially for low-similarity sequences.