To the Editor:We read with great interest the recent article by Shi et al.pub-lished in Hepatobiliary Pancreatic Diseases International[1].Shi’s study was based on radiological features and clinical factors to constr...To the Editor:We read with great interest the recent article by Shi et al.pub-lished in Hepatobiliary Pancreatic Diseases International[1].Shi’s study was based on radiological features and clinical factors to construct a model to predict the effectiveness of first transarterial chemoembolization(TACE)treatment for hepatocellular carcinoma(HCC)in prolonging patient survival.The results showed that area under the receiver operating characteristic curve was 0.964 for the training cohort and 0.949 for the validation cohort.展开更多
In the petroleum industry,the properties of catalysts play a crucial role in the performance of hydroprocessing reactions.Carbon modification can effectively regulate the physicochemical properties of catalysts,but fu...In the petroleum industry,the properties of catalysts play a crucial role in the performance of hydroprocessing reactions.Carbon modification can effectively regulate the physicochemical properties of catalysts,but further in-depth research is necessary.In this study,ethylene glycol was used as the carbon source to investigate the impact of varying carbon amounts on the performance of the Mo-Ni/Al_(2)O_(3)hydrogenation catalyst.The results showed that both the pore structure and surface hydroxyl groups of catalysts can be adjusted after carbon modification.As the carbon content increased,the surface acidity of catalysts gradually decreased,and the interaction between carrier and active metal gradually weakened,leading to more octahedral coordination in form of polynuclear polymolybdic acid.The dispersion and sulfidation degree of Mo species improved,ultimately resulting in more hydrogenation active phases.Consequently,the catalyst exhibited enhanced hydrodesulfurization(HDS)and hydrodenitrification(HDN)activities.展开更多
Data-driven approaches are extensively employed to model complex chemical engineering processes, such as hydrotreating, to address the challenges of mechanism-based methods demanding deep process understanding. Howeve...Data-driven approaches are extensively employed to model complex chemical engineering processes, such as hydrotreating, to address the challenges of mechanism-based methods demanding deep process understanding. However, the development of such models requires specialized expertise in data science, limiting their broader application. Large language models (LLMs), such as GPT-4, have demonstrated potential in supporting and guiding research efforts. This work presents a novel AI-assisted framework where GPT-4, through well-engineered prompts, facilitates the construction and explanation of multi-objective neural networks. These models predict hydrotreating products properties (such as distillation range), including refined diesel and refined gas oil, using feedstock properties, operating conditions, and recycle hydrogen composition. Gradient-weighted class activation mapping was employed to identify key features influencing the output variables. This work illustrates an innovative AI-guided paradigm for chemical engineering applications, and the designed prompts hold promise for adaptation to other complex processes.展开更多
The development of efficient photocatalysts for selective organic transformations under visible light remains a major challenge in sustainable chemistry.In this study,we present a straightforward solvothermal strategy...The development of efficient photocatalysts for selective organic transformations under visible light remains a major challenge in sustainable chemistry.In this study,we present a straightforward solvothermal strategy for fabricating a defect-engineered ZrO_(2)/UiO-66-NH_(2)hybrid material with abundant oxygen vacancies,enabling the visible-light-driven oxidation of benzyl alcohol to benzaldehyde.By optimizing the solvothermal treatment duration,the composite(UiO-66-NH_(2)-2h)achieves a 74.1%conversion of benzyl alcohol with>99%selectivity toward benzaldehyde under mild conditions,substantially out-performing pristine UiO-66-NH_(2).Structural and mechanistic studies reveal that the solvothermal process induces the in situ formation of ultrasmall,uniformly dispersed ZrO_(2)nanoparticles(~2.3 nm)within the MOF matrix,while simultaneously generating abundant oxygen vacancies,as confirmed by XPS,EPR,and HRTEM analyses.The defect-mediated electronic structure of the ZrO_(2)/UiO-66-NH_(2)hybrid enhances visible-light absorption,facilitates charge carrier separation,and pro-motes efficient activation of O_(2)into superoxide radicals(·O_(2)^(−)),the primary reactive species.Transient photocurrent measure-ments and electrochemical impedance spectroscopy further verify the improved charge separation efficiency.The synergistic interplay between oxygen vacancies and the intimate ZrO_(2)/UiO-66-NH_(2)interface provides a unique defect-mediated charge transfer pathway,distinguishing this system from conventional heterojunctions.This study demonstrates a facile,one-step approach to integrate defect engineering with interfacial hybridization in MOF-based photocatalysts,off ering a scalable route for solar-driven organic synthesis.展开更多
The development of flexible supercapacitors(FSCs) capable of operating at high temperatures is crucial for expanding the application areas and operating conditions of supercapacitors. Gel polymer electrolytes and elec...The development of flexible supercapacitors(FSCs) capable of operating at high temperatures is crucial for expanding the application areas and operating conditions of supercapacitors. Gel polymer electrolytes and electrode materials stand as two key components that significantly impact the efficacy of hightemperature-tolerant FSCs(HT-FSCs). They should not only exhibit high electrochemical performance and excellent flexibility, but also withstand intense thermal stress. Considerable efforts have been devoted to enhancing their thermal stability while maintaining high electrochemical and mechanical performance. In this review, the fundamentals of HT-FSCs are outlined. A comprehensive overview of state-of-the-art progress and achievements in HT-FSCs, with a focus on thermally stable gel polymer electrolytes and electrode materials is provided. Finally, challenges and future perspectives regarding HT-FSCs are discussed, alongside strategies for elevating operational temperatures and performance.This review offers both theoretical foundations and practical guidelines for designing and manufacturing HT-FSCs, further promoting their widespread adoption across diverse fields.展开更多
Hot compressive experiments of the laser solid formed(LSFed)TC4 titanium alloy were conducted at a wide temperature range of 650-950℃and strain rate of 0.01-10 s^(-1).The Arrheniustype constitutive models of the LSFe...Hot compressive experiments of the laser solid formed(LSFed)TC4 titanium alloy were conducted at a wide temperature range of 650-950℃and strain rate of 0.01-10 s^(-1).The Arrheniustype constitutive models of the LSFed TC4 alloy were established at the temperature range of 800-950℃and of 650-800℃,respectively.The average relative error between the predicted stresses and experimental values in those two temperature ranges are 10.4%and 8.3%,respectively,indicating that the prediction models constructed in this paper are in a good agreement with experimental data.Processing maps were established by the principle of dynamic materials modeling on the basis of the data achieved from the hot compression experiments.The processing parameters corresponding to the stable and unstable regions of material deformation can be determined from the processing maps.The microstructure evolution of the stable and unstable regions of the samples after tests were observed.Finally,the effect of hot compressive parameters on the microstructure were investigated to research the dynamic recrystallization and the texture of the deformed LSFed TC4 alloy.展开更多
Light cycle oil(LCO) with high content of poly-aromatics was difficult to upgrade and convert,which had hindered upgrading fuel quality to meet with the standard of automotive diesel for the purpose of sustainable dev...Light cycle oil(LCO) with high content of poly-aromatics was difficult to upgrade and convert,which had hindered upgrading fuel quality to meet with the standard of automotive diesel for the purpose of sustainable development.The hydrocracking behaviors of typical aromatics in LCO of naphthalene and tetralin were investigated over NiMo and CoMo catalysts.Several characterization methods including N2-adsoprtion and desorption,ammonia temperature-programmed desorption(NH3-TPD),Pyridine infrared spectroscopy(Py-IR),CO infrared spectroscopy(CO-IR),Raman and X-ray photoelectron spectroscopy(XPS) were applied to determine the properties of different catalysts.The results showed that CoMo catalyst with high concentration of S-edges could hydrosaturate more naphthalene to tetralin but exhibit lower yield of high-value light aromatics(carbon numbers less than 10) than NiMo catalyst.NiMo catalyst with high concentration of Mo-edges also presented a higher selectivity of converting naphthalene into cyclanes than CoMo catalyst.Subsequently,the naphthalene and LCO hydrocracking performances were also investigated over different catalysts systems.The activity evaluation and kinetic analysis results showed that the naphthalene hydrocracking conversion and the yield of light aromatics for CoMo-AY/NiMo-AY grading catalysts were higher than NiMo-AY/CoMo-AY grading catalysts at same condition.A stepwise reaction principle was proposed to explain the high efficiency of CoMo-AY/NiMoAY grading catalysts.Finally,the LCO hydrocracking evaluation results confirmed that CoMo-AY/NiMoAY catalysts grading system with low carbon deposition and high stability could remain high percentage of active phases,which was more efficient to convert LCO to high-octane gasoline.展开更多
Hydrotreating of vacuum residue by ebullated-bed shows tremendous significance due to more stringent environmental regulations and growing demand for lighter fuels. However, enhancing the catalyst stability still rema...Hydrotreating of vacuum residue by ebullated-bed shows tremendous significance due to more stringent environmental regulations and growing demand for lighter fuels. However, enhancing the catalyst stability still remains as a challenging task. Herein, two Ni–Mo/Al_(2)O_(3) catalysts with distinct morphologies(i.e., spherical and cylindrical) were first designed, and the morphology effect on deactivation was systematically elucidated employing multi-characterizations, such as HRTEM with EDX mapping, electron microprobe analysis, FT-IR, TGA and Raman. It is found that spherical catalyst exhibits superior hydrotreating stability over 1600 h. The carbonaceous deposits on spherical catalyst with less graphite structure are lighter, and the coke weight is also smaller. In addition, the metal deposits uniformly distribute in the spherical catalyst, which is better than the concentrated distribution near the pore mouth for the cylindrical catalyst. Furthermore, the intrinsic reason for the differences was analyzed by the bed expansion experiment. Higher bed expansion rate together with the better mass transfer ability leads to the enhanced performance. This work sheds new light on the design of more efficient industrial hydrotreating catalyst based on morphology effect.展开更多
The coupled CFD-E-model for multiphase micro-mixing was developed,and used to predict the micro-mixing effects on the parallel competing chemical reactions in semi-batch gas–liquid and solid–liquid stirred tanks.Bas...The coupled CFD-E-model for multiphase micro-mixing was developed,and used to predict the micro-mixing effects on the parallel competing chemical reactions in semi-batch gas–liquid and solid–liquid stirred tanks.Based on the multiphase macro-flow field,the key parameters of the micro-mixing E-model were obtained with solving the Reynolds-averaged transport equations of mixture fraction and its variance at low computational costs.Compared with experimental data,the multiphase numerical method shows the satisfactory predicting ability.For the gas–liquid system,the segregated reaction zone is mainly near the feed point,and shrinks to the exit of feed-pipe when the feed position is closer to the impeller.Besides,surface feed requires more time to completely exhaust the added H+solution than that of impeller region feed at the same operating condition.For the solid–liquid system,when the solid suspension cloud is formed at high solid holdups,the flow velocity in the clear liquid layer above the cloud is notably reduced and the reactions proceed slowly in this almost stagnant zone.Therefore,the segregation index in this case is larger than that in the dilute solid–liquid system.展开更多
The rate performance and cycle stability of graphitized needle coke(GNC)as anode are still limited by the sluggish kinetics and volume expansion during the Li ions intercalation and de-intercalation process.Especially...The rate performance and cycle stability of graphitized needle coke(GNC)as anode are still limited by the sluggish kinetics and volume expansion during the Li ions intercalation and de-intercalation process.Especially,the output of energy density for lithium ion batteries(LIBs)is directly affected by the delithiation capacity below 0.5 V.Here,the mildly expanded graphitized needle coke(MEGNC)with the enlarged interlayer spacing from 0.346 to 0.352 nm is obtained by the two-step mild oxidation intercalation modification.The voltage plateau of MEGNC anode below 0.5 V is obviously broadened as compared to the initial GNC anode,contributing to the enhancement of Li storage below the low voltage plateau.Moreover,the coin full cell and pouch full cell configured with MEGNC anode exhibit much enhanced Li storage ability,energy density and better cycling stability than those full cells configured with GNC and commercial graphite anodes,demonstrating the practical application value of MEGNC.The superior anode behaviors of MEGNC including the increased effective capacity at low voltage and superior cyclic stability are mainly benefited from the enlarged interlayer spacing,which not only accelerates the Li ions diffusion rate,but also effectively alleviates the volume expansion and fragmentation during the Li ions intercalation process.In addition,the above result is further confirmed by the density functional theory simulation.This work provides an effective modification strategy for the NC-based graphite to enhance the delithiation capacity at a low voltage plateau,dedicated to improving the energy density and durability of LIBs.展开更多
The Trans-North China Orogen is a major Neoarchean Paleoproterozoic collisional orogenic belt above the North China Craton, formed due to prolonged and complex processes. Even though many NeoarcheanPaleoproterozoic ma...The Trans-North China Orogen is a major Neoarchean Paleoproterozoic collisional orogenic belt above the North China Craton, formed due to prolonged and complex processes. Even though many NeoarcheanPaleoproterozoic magmatic and metamorphic activities have been reported, due to the Huozhou Complex’s small outcropping range, little attention has been paid to the origin of various igneous rocks of the Huozhou Complex in the center of the Trans-North China Orogen. The Huozhou Complex, located south of the Luè liang, Wutai, and Hengshan complexes, is an important window into the Early Precambrian structure and evolution of the North China Craton. Its magma and metamorphism are crucial to understanding the development of the structural evolution of the Trans-North China Orogen. The Huozhou metamorphic complex area exposes a range of Precambrian metamorphic rocks, among which the most extensively dispersed is felsic biotite plagioclase gneiss. In this study comprehensive geological field survey, micropetrology,chronology, geochemistry, and Hf isotope analysis were carried out for the Qinggangping and Anziping gneiss in the north of the Huozhou Complex. The results show that the magmatic zircon age of the Qinggangping gneiss is2196 ± 14 Ma, and its protolith is I-type granite, formed by partial melting of igneous rocks in the absence of weathering. Its source is mainly the juvenile crust from depleted mantle dating 2431–2719 Ma, with a small amount of mantle-derived material. The Anziping gneiss has a metamorphic zircon age of 1931 ± 13 Ma with an S-type granite protolith belonging to peraluminous granite.The Anziping gneiss is formed by recycling pre-existing crustal components at 2613–2848 Ma. A minor quantity of mantle-derived magma is also introduced to the crust simultaneously. The samples of Qinggangping gneiss and Anziping gneiss show the characteristics of obvious negative Nb, Ti, and P elements in the spider diagram of primitive mantle standardization. This implies that the rocks have the characteristics of magmatic rocks in an island arc or subduction environment, which could have formed in the tectonic environment of the continental margin arc.展开更多
Hydrocracking represents an important process in modern petroleum refining industry,whose performance mainly relies on the identity of catalyst.In this work,we perform a combined thermodynamics and kinetics study on t...Hydrocracking represents an important process in modern petroleum refining industry,whose performance mainly relies on the identity of catalyst.In this work,we perform a combined thermodynamics and kinetics study on the hydrogenation of naphthalene over a commercialized NiMo/HY catalyst.The reaction network is constructed for the respective production of decalin and methylindane via the intermediate product of tetralin,which could further undergo hydrogenation to butylbenzene,ethylbenzene,xylene,toluene,benzene,methylcyclohexane and cyclohexane.The thermodynamics analysis suggests the optimum operating conditions for the production of monoaromatics are 400℃,8.0 MPa,and 4.0 hydrogen/naphthalene ratio.Based on these,the influences of reaction temperature,pressure,hydrogen/-naphthalene ratio,and liquid hourly space velocity(LHSV)are investigated to fit the Langmuir-Hinshelwood model.It is found that the higher temperature and pressure while lower LHSV favors monoaromatics production,which is insensitive to the hydrogen/naphthalene ratio.Furthermore,the high consistence between the experimental and simulated data further validates the as-obtained kinetics model on the prediction of catalytic performance over this kind of catalyst.展开更多
Flotation is an efficient pre-treatment technology for oily water.In this work,the interaction process between the moving oil droplet and the gas bubble was studied by high-speed camera and Bassset-Boussinesq-Oseen(BB...Flotation is an efficient pre-treatment technology for oily water.In this work,the interaction process between the moving oil droplet and the gas bubble was studied by high-speed camera and Bassset-Boussinesq-Oseen(BBO)theoretical model,and the experimental and simulation results of the oil droplet trajectory were compared.Moreover,the micro-particle image velocimetry system was utilized to observe the flow inside and outside of the moving oil droplet.The results show that the BBO model with the mobile bubble’s surface can reflect the velocity change trend of the oil droplet during the interaction process between the moving oil droplet and the gas bubble,but there are some significant differences between the experimental and simulation results.While the oil droplet is moving on the bubble’s surface,the velocity of the area near the contact point of oil droplet–gas bubble is less than that of the other areas inside the oil droplet.Meanwhile,the flow of water above the oil drop is more biased towards the gas bubble.展开更多
Recently,high-entropy ceramics have attracted considerable attentions because of comprehensive physical and chemical properties of high hardness,fracture toughness,and conductivity.However,as a newly emerging class of...Recently,high-entropy ceramics have attracted considerable attentions because of comprehensive physical and chemical properties of high hardness,fracture toughness,and conductivity.However,as a newly emerging class of materials,the synthesis,performance and applications of high-entropy ceramics are subject to further development.Here,we reported a new non-stoichiometric TiC0.4/WC/0.5Mo2C medium-entropy carbide(MEC)with a rock-salt structure.Attributed to the solid solution strengthening and twinning strengthening,the TiCO0.4/WC/0.5Mo2C sintered at 1900℃by spark plasma sintering(SPS)shows superior mechanical behaviors of microhardness(21.7 GPa),which exceeds that expected from the rule of mixture(ROM)of three individual metal carbides(19.1 GPa)and good fracture toughness(5.3 MPa m1/2).Significantly,the bulk synthesized via high-pressure and high-temperature(HPHT)sintering possesses smaller grain size and shows better comprehensive mechanical properties of microhardness(23.7 GPa)and fracture toughness(6.2 MPa m1/2).In addition,the effect of anion vacancies on the thermodynamic stability and synthesizability of TiC0.4/WC/0.5Mo2C was analyzed via quantitatively calculated entropy.Vacancies could significantly enhance the configuratio nal entropy of mixing of the solid phase.The introduction of vacancy defects may expand synthetic path for entropy-stabilized ceramics,especially for multi-component high tempe rature refractory ceramics.展开更多
A method is proposed for the prospecting prediction of subsurface mineral deposits based on soil geochemistry data and a deep convolutional neural network model.This method uses three techniques(window offset,scaling,...A method is proposed for the prospecting prediction of subsurface mineral deposits based on soil geochemistry data and a deep convolutional neural network model.This method uses three techniques(window offset,scaling,and rotation)to enhance the number of training data for the model.A window area is used to extract the spatial distribution characteristics of soil geochemistry and measure their correspondence with the occurrence of known subsurface deposits.Prospecting prediction is achieved by matching the characteristics of the window area of an unknown area with the relationships established in the known area.This method can efficiently predict mineral prospective areas where there are few ore deposits used for generating the training dataset,meaning that the deep-learning method can be effectively used for deposit prospecting prediction.Using soil active geochemical measurement data,this method was applied in the Daqiao area,Gansu Province,for which seven favorable gold prospecting target areas were predicted.The Daqiao orogenic gold deposit of latest Jurassic and Early Jurassic age in the southern domain has more than 105 t of gold resources at an average grade of 3-4 g/t.In 2020,the project team drilled and verified the K prediction area,and found 66 m gold mineralized bodies.The new method should be applicable to prospecting prediction using conventional geochemical data in other areas.展开更多
Although geothermal energy has many clear advantages,including its sustainability and environmentally friendly nature,research into potential geothermal resources across the Longgang Block,Northeast China,has been lim...Although geothermal energy has many clear advantages,including its sustainability and environmentally friendly nature,research into potential geothermal resources across the Longgang Block,Northeast China,has been limited.Here we present the first analysis of the potential geothermal resources in this region that employs joint geological and non-seismic geophysical methods to identify target areas that may be economically viable.We acquire and analyze high-precision gravity,magnetic,and magnetotelluric sounding data,which are constrained using the petrophysical parameters of outcropping rocks across the Longgang Block,to conduct a comprehensive evaluation of the region’s deep geological structures and their geothermal resources potential,with a focus on identifying faults,rock masses,and thermal storage structures.We find that Archean granitic gneiss and Mesozoic rock masses in the deeper section of the Longgang Block possess weak gravity anomalies and high resistivities.We also identify thermal storage structures near these deeper geological units based on their extremely low resistivities.The data are used to infer the dip and depth of known or hidden faults,to constrain the spatial distribution of intrusive rock masses,and to determine the spatial distribution of subsurface thermal storage structures.The potential of the target areas for geothermal resources exploitation is divided into three grades based on contact depths between faults and thermal storage structures,and the scale of their thermal storage structures.Our results suggest that a joint non-seismic geophysical approach can be effective in locating and evaluating geothermal resources in complex geological settings.展开更多
Vacuum gas oil(VGO)is the most important feedstock for hydrocracking processes in refineries,but its molecular composition cannot be fully acquired by current analysis techniques owing to its complexity.In order to bu...Vacuum gas oil(VGO)is the most important feedstock for hydrocracking processes in refineries,but its molecular composition cannot be fully acquired by current analysis techniques owing to its complexity.In order to build an accurate and reliable molecular-level kinetic model for reactor design and process optimization,the molecular composition of VGO has to be reconstructed based on limited measurements.In this study,a modified stochastic reconstruction-entropy maximization(SR-REM)algorithm was applied to reconstruct VGOs,with generation of a general molecule library once and for all via the SR method at the first step and adjustment of the molecular abundance of various VGOs via the REM method at the second step.The universality of the molecule library and the effectiveness of the modified SR-REM method were validated by fifteen VGOs(three from the literature)from different geographic regions of the world and with different properties.The simulated properties(density,elemental composition,paraffin-naphthene-aromatics distribution,boiling point distribution,detailed composition of naphthenes and aromatics in terms of ring number as well as composition of S-heterocycles)are in good agreement with the measured counterparts,showing average absolute relative errors of below 10%for each property.展开更多
It is usually difficult to remove dibenzothiophenes from diesel fuels by oxidation with molecular oxygen as an oxidant.In the study,tungsten oxide was supported on magnetic mesoporous silica by calcination to form a m...It is usually difficult to remove dibenzothiophenes from diesel fuels by oxidation with molecular oxygen as an oxidant.In the study,tungsten oxide was supported on magnetic mesoporous silica by calcination to form a magnetically separable catalyst for oxidative desulfurization of diesel fuel.By tuning different calcining temperatures,the catalyst calcined at 500℃showed a high catalytic activity with molecular oxygen as the oxidant.Under optimal reaction conditions,the sulfur removal of DBT reached 99.9%at 120℃after 8 h.Furthermore,the removals of 4-methyldibenzothiophene and 4,6-dimethyldibenzothiophene could also get up to 98.2%and 92.3%under the same conditions.The reaction mechanism was explored by selective quenching experiments and FT-IR spectra.展开更多
基金supported by a grant from the Nursing Re-search Program of the First Affiliated Hospital of Zhejiang Univer-sity School of Medicine(No.2022ZYHL045).
文摘To the Editor:We read with great interest the recent article by Shi et al.pub-lished in Hepatobiliary Pancreatic Diseases International[1].Shi’s study was based on radiological features and clinical factors to construct a model to predict the effectiveness of first transarterial chemoembolization(TACE)treatment for hepatocellular carcinoma(HCC)in prolonging patient survival.The results showed that area under the receiver operating characteristic curve was 0.964 for the training cohort and 0.949 for the validation cohort.
基金supported by grants from the National Natural Science Foundation of China(22122807 and 22378038)Fundamental Research Funds for the Central Universities(DUT23RC(3)044)+1 种基金State Key Laboratory of Heavy Oil Processing,China University of Petroleum(WX20230149)China Postdoctoral Science Foundation(2024M750328).
文摘In the petroleum industry,the properties of catalysts play a crucial role in the performance of hydroprocessing reactions.Carbon modification can effectively regulate the physicochemical properties of catalysts,but further in-depth research is necessary.In this study,ethylene glycol was used as the carbon source to investigate the impact of varying carbon amounts on the performance of the Mo-Ni/Al_(2)O_(3)hydrogenation catalyst.The results showed that both the pore structure and surface hydroxyl groups of catalysts can be adjusted after carbon modification.As the carbon content increased,the surface acidity of catalysts gradually decreased,and the interaction between carrier and active metal gradually weakened,leading to more octahedral coordination in form of polynuclear polymolybdic acid.The dispersion and sulfidation degree of Mo species improved,ultimately resulting in more hydrogenation active phases.Consequently,the catalyst exhibited enhanced hydrodesulfurization(HDS)and hydrodenitrification(HDN)activities.
基金supported by the National Key Research and Development Program of China(2023YFA1507601)the National Natural Science Foundation of China(22278127,22378038)+2 种基金the Fundamental Research Funds for the Central Universities(2022ZFJH004)the Shanghai Pilot Program for Basic Research(22T01400100-18)the Natural Science Foundation of Liaoning Province,China(2024-MSBA-15).
文摘Data-driven approaches are extensively employed to model complex chemical engineering processes, such as hydrotreating, to address the challenges of mechanism-based methods demanding deep process understanding. However, the development of such models requires specialized expertise in data science, limiting their broader application. Large language models (LLMs), such as GPT-4, have demonstrated potential in supporting and guiding research efforts. This work presents a novel AI-assisted framework where GPT-4, through well-engineered prompts, facilitates the construction and explanation of multi-objective neural networks. These models predict hydrotreating products properties (such as distillation range), including refined diesel and refined gas oil, using feedstock properties, operating conditions, and recycle hydrogen composition. Gradient-weighted class activation mapping was employed to identify key features influencing the output variables. This work illustrates an innovative AI-guided paradigm for chemical engineering applications, and the designed prompts hold promise for adaptation to other complex processes.
基金the National Natural Sci-ence Foundation of China(Nos.22271038,22378038,22172012)C.P.thanks Dalian Science and Technology Innovation Fund(No.2024JJ12CG033)+1 种基金C.P.and Z.S thank State Key Laboratory of Heavy Oil Processing(Nos.WX20230149,SKLHOP202402005)Y.-Y.L.thanks the Guangxi Key Laboratory of Information Materials,Guilin University of Electronic Technology(No.231019-K).
文摘The development of efficient photocatalysts for selective organic transformations under visible light remains a major challenge in sustainable chemistry.In this study,we present a straightforward solvothermal strategy for fabricating a defect-engineered ZrO_(2)/UiO-66-NH_(2)hybrid material with abundant oxygen vacancies,enabling the visible-light-driven oxidation of benzyl alcohol to benzaldehyde.By optimizing the solvothermal treatment duration,the composite(UiO-66-NH_(2)-2h)achieves a 74.1%conversion of benzyl alcohol with>99%selectivity toward benzaldehyde under mild conditions,substantially out-performing pristine UiO-66-NH_(2).Structural and mechanistic studies reveal that the solvothermal process induces the in situ formation of ultrasmall,uniformly dispersed ZrO_(2)nanoparticles(~2.3 nm)within the MOF matrix,while simultaneously generating abundant oxygen vacancies,as confirmed by XPS,EPR,and HRTEM analyses.The defect-mediated electronic structure of the ZrO_(2)/UiO-66-NH_(2)hybrid enhances visible-light absorption,facilitates charge carrier separation,and pro-motes efficient activation of O_(2)into superoxide radicals(·O_(2)^(−)),the primary reactive species.Transient photocurrent measure-ments and electrochemical impedance spectroscopy further verify the improved charge separation efficiency.The synergistic interplay between oxygen vacancies and the intimate ZrO_(2)/UiO-66-NH_(2)interface provides a unique defect-mediated charge transfer pathway,distinguishing this system from conventional heterojunctions.This study demonstrates a facile,one-step approach to integrate defect engineering with interfacial hybridization in MOF-based photocatalysts,off ering a scalable route for solar-driven organic synthesis.
基金Fundamental Research Funds for the Central Universities of China(Grant No. SWU-KT22030)Scientific and Technological Research Program of Chongqing Municipal Education Commission of China (No.KJQN202300205)financial support from the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under the project of 457444676。
文摘The development of flexible supercapacitors(FSCs) capable of operating at high temperatures is crucial for expanding the application areas and operating conditions of supercapacitors. Gel polymer electrolytes and electrode materials stand as two key components that significantly impact the efficacy of hightemperature-tolerant FSCs(HT-FSCs). They should not only exhibit high electrochemical performance and excellent flexibility, but also withstand intense thermal stress. Considerable efforts have been devoted to enhancing their thermal stability while maintaining high electrochemical and mechanical performance. In this review, the fundamentals of HT-FSCs are outlined. A comprehensive overview of state-of-the-art progress and achievements in HT-FSCs, with a focus on thermally stable gel polymer electrolytes and electrode materials is provided. Finally, challenges and future perspectives regarding HT-FSCs are discussed, alongside strategies for elevating operational temperatures and performance.This review offers both theoretical foundations and practical guidelines for designing and manufacturing HT-FSCs, further promoting their widespread adoption across diverse fields.
基金the National Key Research and Development Program of China(No.2016YFB1100104)the National Natural Science Foundation of China(No.51875470)+1 种基金the State Key Laboratory of Solidification Processing(NPU,China)(2019-QZ-01)the financial support from the fund of SAST(SAST2016043)。
文摘Hot compressive experiments of the laser solid formed(LSFed)TC4 titanium alloy were conducted at a wide temperature range of 650-950℃and strain rate of 0.01-10 s^(-1).The Arrheniustype constitutive models of the LSFed TC4 alloy were established at the temperature range of 800-950℃and of 650-800℃,respectively.The average relative error between the predicted stresses and experimental values in those two temperature ranges are 10.4%and 8.3%,respectively,indicating that the prediction models constructed in this paper are in a good agreement with experimental data.Processing maps were established by the principle of dynamic materials modeling on the basis of the data achieved from the hot compression experiments.The processing parameters corresponding to the stable and unstable regions of material deformation can be determined from the processing maps.The microstructure evolution of the stable and unstable regions of the samples after tests were observed.Finally,the effect of hot compressive parameters on the microstructure were investigated to research the dynamic recrystallization and the texture of the deformed LSFed TC4 alloy.
基金supported by the National Natural Science Foundation of China (Nos. 21878330, 21676298)the National Science and Technology Major Project, the CNPC Key Research Project (2016E-0707)the King Abdullah University of Science and Technology (KAUST) Office of Sponsored Research (OSR) under Award (No. OSR-2019-CPF-4103.2)。
文摘Light cycle oil(LCO) with high content of poly-aromatics was difficult to upgrade and convert,which had hindered upgrading fuel quality to meet with the standard of automotive diesel for the purpose of sustainable development.The hydrocracking behaviors of typical aromatics in LCO of naphthalene and tetralin were investigated over NiMo and CoMo catalysts.Several characterization methods including N2-adsoprtion and desorption,ammonia temperature-programmed desorption(NH3-TPD),Pyridine infrared spectroscopy(Py-IR),CO infrared spectroscopy(CO-IR),Raman and X-ray photoelectron spectroscopy(XPS) were applied to determine the properties of different catalysts.The results showed that CoMo catalyst with high concentration of S-edges could hydrosaturate more naphthalene to tetralin but exhibit lower yield of high-value light aromatics(carbon numbers less than 10) than NiMo catalyst.NiMo catalyst with high concentration of Mo-edges also presented a higher selectivity of converting naphthalene into cyclanes than CoMo catalyst.Subsequently,the naphthalene and LCO hydrocracking performances were also investigated over different catalysts systems.The activity evaluation and kinetic analysis results showed that the naphthalene hydrocracking conversion and the yield of light aromatics for CoMo-AY/NiMo-AY grading catalysts were higher than NiMo-AY/CoMo-AY grading catalysts at same condition.A stepwise reaction principle was proposed to explain the high efficiency of CoMo-AY/NiMoAY grading catalysts.Finally,the LCO hydrocracking evaluation results confirmed that CoMo-AY/NiMoAY catalysts grading system with low carbon deposition and high stability could remain high percentage of active phases,which was more efficient to convert LCO to high-octane gasoline.
基金supported by Natural Science Foundation of China(21978325)the National Key Technologies Research and Development Program of China(2017YFB0306503)+5 种基金Fundamental Research Funds for the Central Universities(18CX02130A,18CX02014A)Open Project of State Key Laboratory of Chemical Engineering(SKL-Ch E-18C04)Doctoral Start-up Foundation of Liaoning Province(2019-BS054)Program for Liaoning Innovative Talents in University(XLYC1807245)China Postdoctoral Science Foundation(2019M661409)High-level Talent Innovation and Business Project of Dalian(2017RQ085)。
文摘Hydrotreating of vacuum residue by ebullated-bed shows tremendous significance due to more stringent environmental regulations and growing demand for lighter fuels. However, enhancing the catalyst stability still remains as a challenging task. Herein, two Ni–Mo/Al_(2)O_(3) catalysts with distinct morphologies(i.e., spherical and cylindrical) were first designed, and the morphology effect on deactivation was systematically elucidated employing multi-characterizations, such as HRTEM with EDX mapping, electron microprobe analysis, FT-IR, TGA and Raman. It is found that spherical catalyst exhibits superior hydrotreating stability over 1600 h. The carbonaceous deposits on spherical catalyst with less graphite structure are lighter, and the coke weight is also smaller. In addition, the metal deposits uniformly distribute in the spherical catalyst, which is better than the concentrated distribution near the pore mouth for the cylindrical catalyst. Furthermore, the intrinsic reason for the differences was analyzed by the bed expansion experiment. Higher bed expansion rate together with the better mass transfer ability leads to the enhanced performance. This work sheds new light on the design of more efficient industrial hydrotreating catalyst based on morphology effect.
基金supported by the National Key Research and Development Program(2016YFB0301702)the National Natural Science Foundation of China(21808221,21776282,21938009)+3 种基金Major Research Plan of NSFC(91934301)the Key Research Program of Frontier Sciences,CAS(QYZDJ-SSW-JSC030)the Key Research Program of Nanjing IPE Institute of Green Manufacturing Industry(No.E0010719)the Youth Innovation Promotion Association CAS。
文摘The coupled CFD-E-model for multiphase micro-mixing was developed,and used to predict the micro-mixing effects on the parallel competing chemical reactions in semi-batch gas–liquid and solid–liquid stirred tanks.Based on the multiphase macro-flow field,the key parameters of the micro-mixing E-model were obtained with solving the Reynolds-averaged transport equations of mixture fraction and its variance at low computational costs.Compared with experimental data,the multiphase numerical method shows the satisfactory predicting ability.For the gas–liquid system,the segregated reaction zone is mainly near the feed point,and shrinks to the exit of feed-pipe when the feed position is closer to the impeller.Besides,surface feed requires more time to completely exhaust the added H+solution than that of impeller region feed at the same operating condition.For the solid–liquid system,when the solid suspension cloud is formed at high solid holdups,the flow velocity in the clear liquid layer above the cloud is notably reduced and the reactions proceed slowly in this almost stagnant zone.Therefore,the segregation index in this case is larger than that in the dilute solid–liquid system.
基金supported by the National Natural Science Foundation of China(21776309,22122807 and 21706283)。
文摘The rate performance and cycle stability of graphitized needle coke(GNC)as anode are still limited by the sluggish kinetics and volume expansion during the Li ions intercalation and de-intercalation process.Especially,the output of energy density for lithium ion batteries(LIBs)is directly affected by the delithiation capacity below 0.5 V.Here,the mildly expanded graphitized needle coke(MEGNC)with the enlarged interlayer spacing from 0.346 to 0.352 nm is obtained by the two-step mild oxidation intercalation modification.The voltage plateau of MEGNC anode below 0.5 V is obviously broadened as compared to the initial GNC anode,contributing to the enhancement of Li storage below the low voltage plateau.Moreover,the coin full cell and pouch full cell configured with MEGNC anode exhibit much enhanced Li storage ability,energy density and better cycling stability than those full cells configured with GNC and commercial graphite anodes,demonstrating the practical application value of MEGNC.The superior anode behaviors of MEGNC including the increased effective capacity at low voltage and superior cyclic stability are mainly benefited from the enlarged interlayer spacing,which not only accelerates the Li ions diffusion rate,but also effectively alleviates the volume expansion and fragmentation during the Li ions intercalation process.In addition,the above result is further confirmed by the density functional theory simulation.This work provides an effective modification strategy for the NC-based graphite to enhance the delithiation capacity at a low voltage plateau,dedicated to improving the energy density and durability of LIBs.
基金supported by the open fund from the Key Laboratory of Deep-Earth Dynamics of Ministry of Natural Resources,Institute of Geology,Chinese Academy of Geological Sciences (Number J1901-16)the project of graduate education and teaching reform in Shanxi Province (Award Number 2021YJJG147)+3 种基金the teaching reform project ‘‘Geographic Modeling,Simulation and Visualization’’ established by Shanxi Normal University (Number 2019JGXM-39)‘‘The Research Start-up Fund of Shanxi Normal University for Dr. Peng Chong in 2016’’(Number0505/02070438)‘‘The Research Start-up Fund of Shanxi Normal University for Dr. Liu Haiyan in 2017’’(Number 0505/02070458)‘‘The Research Fund for Outstanding Doctor in 2017’’(Number0503/02010168)。
文摘The Trans-North China Orogen is a major Neoarchean Paleoproterozoic collisional orogenic belt above the North China Craton, formed due to prolonged and complex processes. Even though many NeoarcheanPaleoproterozoic magmatic and metamorphic activities have been reported, due to the Huozhou Complex’s small outcropping range, little attention has been paid to the origin of various igneous rocks of the Huozhou Complex in the center of the Trans-North China Orogen. The Huozhou Complex, located south of the Luè liang, Wutai, and Hengshan complexes, is an important window into the Early Precambrian structure and evolution of the North China Craton. Its magma and metamorphism are crucial to understanding the development of the structural evolution of the Trans-North China Orogen. The Huozhou metamorphic complex area exposes a range of Precambrian metamorphic rocks, among which the most extensively dispersed is felsic biotite plagioclase gneiss. In this study comprehensive geological field survey, micropetrology,chronology, geochemistry, and Hf isotope analysis were carried out for the Qinggangping and Anziping gneiss in the north of the Huozhou Complex. The results show that the magmatic zircon age of the Qinggangping gneiss is2196 ± 14 Ma, and its protolith is I-type granite, formed by partial melting of igneous rocks in the absence of weathering. Its source is mainly the juvenile crust from depleted mantle dating 2431–2719 Ma, with a small amount of mantle-derived material. The Anziping gneiss has a metamorphic zircon age of 1931 ± 13 Ma with an S-type granite protolith belonging to peraluminous granite.The Anziping gneiss is formed by recycling pre-existing crustal components at 2613–2848 Ma. A minor quantity of mantle-derived magma is also introduced to the crust simultaneously. The samples of Qinggangping gneiss and Anziping gneiss show the characteristics of obvious negative Nb, Ti, and P elements in the spider diagram of primitive mantle standardization. This implies that the rocks have the characteristics of magmatic rocks in an island arc or subduction environment, which could have formed in the tectonic environment of the continental margin arc.
基金the National Natural Science Foundation of China(91934301)The China Postdoctoral Science Foundation(2019M661409 and 2020T130190)+3 种基金Doctoral Start-up Foundation of Liaoning Province(2019-BS-054)Liaoning Revitalization Talents Program(XLYC1807245)The Open Project of State Key Laboratory of Chemical Engineering(SKL-ChE-18C04)Dalian High-Level Talent Innovation Program(2017RQ085).
文摘Hydrocracking represents an important process in modern petroleum refining industry,whose performance mainly relies on the identity of catalyst.In this work,we perform a combined thermodynamics and kinetics study on the hydrogenation of naphthalene over a commercialized NiMo/HY catalyst.The reaction network is constructed for the respective production of decalin and methylindane via the intermediate product of tetralin,which could further undergo hydrogenation to butylbenzene,ethylbenzene,xylene,toluene,benzene,methylcyclohexane and cyclohexane.The thermodynamics analysis suggests the optimum operating conditions for the production of monoaromatics are 400℃,8.0 MPa,and 4.0 hydrogen/naphthalene ratio.Based on these,the influences of reaction temperature,pressure,hydrogen/-naphthalene ratio,and liquid hourly space velocity(LHSV)are investigated to fit the Langmuir-Hinshelwood model.It is found that the higher temperature and pressure while lower LHSV favors monoaromatics production,which is insensitive to the hydrogen/naphthalene ratio.Furthermore,the high consistence between the experimental and simulated data further validates the as-obtained kinetics model on the prediction of catalytic performance over this kind of catalyst.
基金supported by the National Natural Science Foundation of China(51578239)the Education and Scientific Research Projects of Shanghai(17DZ1202802)。
文摘Flotation is an efficient pre-treatment technology for oily water.In this work,the interaction process between the moving oil droplet and the gas bubble was studied by high-speed camera and Bassset-Boussinesq-Oseen(BBO)theoretical model,and the experimental and simulation results of the oil droplet trajectory were compared.Moreover,the micro-particle image velocimetry system was utilized to observe the flow inside and outside of the moving oil droplet.The results show that the BBO model with the mobile bubble’s surface can reflect the velocity change trend of the oil droplet during the interaction process between the moving oil droplet and the gas bubble,but there are some significant differences between the experimental and simulation results.While the oil droplet is moving on the bubble’s surface,the velocity of the area near the contact point of oil droplet–gas bubble is less than that of the other areas inside the oil droplet.Meanwhile,the flow of water above the oil drop is more biased towards the gas bubble.
基金financially supported by the Natural Science Foundation of Hebei Province of China(Nos.E2016203425 and E2017203223)the Key Projects of Scientific and Technological Research in Hebei Province(No.ZD2017074)。
文摘Recently,high-entropy ceramics have attracted considerable attentions because of comprehensive physical and chemical properties of high hardness,fracture toughness,and conductivity.However,as a newly emerging class of materials,the synthesis,performance and applications of high-entropy ceramics are subject to further development.Here,we reported a new non-stoichiometric TiC0.4/WC/0.5Mo2C medium-entropy carbide(MEC)with a rock-salt structure.Attributed to the solid solution strengthening and twinning strengthening,the TiCO0.4/WC/0.5Mo2C sintered at 1900℃by spark plasma sintering(SPS)shows superior mechanical behaviors of microhardness(21.7 GPa),which exceeds that expected from the rule of mixture(ROM)of three individual metal carbides(19.1 GPa)and good fracture toughness(5.3 MPa m1/2).Significantly,the bulk synthesized via high-pressure and high-temperature(HPHT)sintering possesses smaller grain size and shows better comprehensive mechanical properties of microhardness(23.7 GPa)and fracture toughness(6.2 MPa m1/2).In addition,the effect of anion vacancies on the thermodynamic stability and synthesizability of TiC0.4/WC/0.5Mo2C was analyzed via quantitatively calculated entropy.Vacancies could significantly enhance the configuratio nal entropy of mixing of the solid phase.The introduction of vacancy defects may expand synthetic path for entropy-stabilized ceramics,especially for multi-component high tempe rature refractory ceramics.
基金funded by a pilot project entitled“Deep Geological Survey of Benxi-Linjiang Area”(1212011220247)of the 3D Geological Mapping and Deep Geological Survey of China Geological Survey。
文摘A method is proposed for the prospecting prediction of subsurface mineral deposits based on soil geochemistry data and a deep convolutional neural network model.This method uses three techniques(window offset,scaling,and rotation)to enhance the number of training data for the model.A window area is used to extract the spatial distribution characteristics of soil geochemistry and measure their correspondence with the occurrence of known subsurface deposits.Prospecting prediction is achieved by matching the characteristics of the window area of an unknown area with the relationships established in the known area.This method can efficiently predict mineral prospective areas where there are few ore deposits used for generating the training dataset,meaning that the deep-learning method can be effectively used for deposit prospecting prediction.Using soil active geochemical measurement data,this method was applied in the Daqiao area,Gansu Province,for which seven favorable gold prospecting target areas were predicted.The Daqiao orogenic gold deposit of latest Jurassic and Early Jurassic age in the southern domain has more than 105 t of gold resources at an average grade of 3-4 g/t.In 2020,the project team drilled and verified the K prediction area,and found 66 m gold mineralized bodies.The new method should be applicable to prospecting prediction using conventional geochemical data in other areas.
基金jointly supported by the open fund from the Key Laboratory of Deep-Earth Dynamics of Ministry of Natural Resources, Institute of Geology, Chinese Academy of Geological Sciences (Award Number J1901-16)the project of graduate education and teaching reform in Shanxi Province (Award Number 2021YJJG147)+4 种基金the teaching reform project “Geographic Modeling, Simulation and Visualization” established by Shanxi Normal University (Award Number 2019JGXM-39)the “Deep Geological Survey in Benxi-Linjiang Area”, a pilot project set up by the China Geological Survey, China (grant number 1212011220247)“The Research Start-up Fund of Shanxi Normal University for Dr. Peng Chong in 2016” (Award Number 0505/ 02070438)“The Research Start-up Fund of Shanxi Normal University for Dr. Liu Haiyan in 2017” (Award Number 0505/02070458)“The Research Fund for Outstanding Doctor in 2017” (Award Number 0503/02010168), established by the Education Department of Shanxi Province for Dr. Liu Haiyan
文摘Although geothermal energy has many clear advantages,including its sustainability and environmentally friendly nature,research into potential geothermal resources across the Longgang Block,Northeast China,has been limited.Here we present the first analysis of the potential geothermal resources in this region that employs joint geological and non-seismic geophysical methods to identify target areas that may be economically viable.We acquire and analyze high-precision gravity,magnetic,and magnetotelluric sounding data,which are constrained using the petrophysical parameters of outcropping rocks across the Longgang Block,to conduct a comprehensive evaluation of the region’s deep geological structures and their geothermal resources potential,with a focus on identifying faults,rock masses,and thermal storage structures.We find that Archean granitic gneiss and Mesozoic rock masses in the deeper section of the Longgang Block possess weak gravity anomalies and high resistivities.We also identify thermal storage structures near these deeper geological units based on their extremely low resistivities.The data are used to infer the dip and depth of known or hidden faults,to constrain the spatial distribution of intrusive rock masses,and to determine the spatial distribution of subsurface thermal storage structures.The potential of the target areas for geothermal resources exploitation is divided into three grades based on contact depths between faults and thermal storage structures,and the scale of their thermal storage structures.Our results suggest that a joint non-seismic geophysical approach can be effective in locating and evaluating geothermal resources in complex geological settings.
基金supported by the National Natural Science Foundation of China(21978093)。
文摘Vacuum gas oil(VGO)is the most important feedstock for hydrocracking processes in refineries,but its molecular composition cannot be fully acquired by current analysis techniques owing to its complexity.In order to build an accurate and reliable molecular-level kinetic model for reactor design and process optimization,the molecular composition of VGO has to be reconstructed based on limited measurements.In this study,a modified stochastic reconstruction-entropy maximization(SR-REM)algorithm was applied to reconstruct VGOs,with generation of a general molecule library once and for all via the SR method at the first step and adjustment of the molecular abundance of various VGOs via the REM method at the second step.The universality of the molecule library and the effectiveness of the modified SR-REM method were validated by fifteen VGOs(three from the literature)from different geographic regions of the world and with different properties.The simulated properties(density,elemental composition,paraffin-naphthene-aromatics distribution,boiling point distribution,detailed composition of naphthenes and aromatics in terms of ring number as well as composition of S-heterocycles)are in good agreement with the measured counterparts,showing average absolute relative errors of below 10%for each property.
基金financially supported by the National Natural Science Foundation of China(Nos.21978119,21576122,and 21766007)a Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutionsthe support of the Jiangsu Government Scholarship for oversea studies。
文摘It is usually difficult to remove dibenzothiophenes from diesel fuels by oxidation with molecular oxygen as an oxidant.In the study,tungsten oxide was supported on magnetic mesoporous silica by calcination to form a magnetically separable catalyst for oxidative desulfurization of diesel fuel.By tuning different calcining temperatures,the catalyst calcined at 500℃showed a high catalytic activity with molecular oxygen as the oxidant.Under optimal reaction conditions,the sulfur removal of DBT reached 99.9%at 120℃after 8 h.Furthermore,the removals of 4-methyldibenzothiophene and 4,6-dimethyldibenzothiophene could also get up to 98.2%and 92.3%under the same conditions.The reaction mechanism was explored by selective quenching experiments and FT-IR spectra.
