Developing a cost-effective and environmentally friendly process for the production of valuable chemicals from abundant herbal biomass receives great attentions in recent years.Herein,taking advantage of the“lignin f...Developing a cost-effective and environmentally friendly process for the production of valuable chemicals from abundant herbal biomass receives great attentions in recent years.Herein,taking advantage of the“lignin first”strategy,corn straw is converted to valuable chemicals including lignin monomers,furfural and 5-methoxymethylfurfural via a two steps process.The key of this research lies in the development of a green and low-cost catalytic process utilizing magnetic Raney Ni catalyst and high boiling point ethylene glycol.The utilization of neat ethylene glycol as the sole slovent under atmospheric conditions obviates the need for additional additives,thereby facilitating the entire process to be conducted in glass flasks and rendering it highly convenient for scaling up.In the initial step,depolymerization of corn straw lignin resulted in a monomer yield of 18.1 wt%.Subsequently,in a dimethyl carbonate system,the carbohydrate component underwent complete conversion in a one-pot process,yielding furfural and 5-methoxymethylfurfural as the primary products with an impressive yield of 47.7%.展开更多
Although solar steam generation strategy is efficient in desalinating seawater,it is still challenging to achieve continuous solar-thermal desalination of seawater and catalytic degradation of organic pollutants.Herei...Although solar steam generation strategy is efficient in desalinating seawater,it is still challenging to achieve continuous solar-thermal desalination of seawater and catalytic degradation of organic pollutants.Herein,dynamic regulations of hydrogen bonding networks and solvation structures are realized by designing an asymmetric bilayer membrane consisting of a bacterial cellulose/carbon nanotube/Co_(2)(OH)_(2)CO_(3)nanorod top layer and a bacterial cellulose/Co_(2)(OH)_(2)CO_(3)nanorod(BCH)bottom layer.Crucially,the hydrogen bonding networks inside the membrane can be tuned by the rich surface–OH groups of the bacterial cellulose and Co_(2)(OH)_(2)CO_(3)as well as the ions and radicals in situ generated during the catalysis process.Moreover,both SO_(4)^(2−)and HSO_(5)−can regulate the solvation structure of Na^(+)and be adsorbed more preferentially on the evaporation surface than Cl^(−),thus hindering the de-solvation of the solvated Na^(+)and subsequent nucleation/growth of NaCl.Furthermore,the heat generated by the solar-thermal energy conversion can accelerate the reaction kinetics and enhance the catalytic degradation efficiency.This work provides a flow-bed water purification system with an asymmetric solar-thermal and catalytic membrane for synergistic solar thermal desalination of seawater/brine and catalytic degradation of organic pollutants.展开更多
Atomically precise metal nanoclusters are an emerging type of nanomaterial which has diverse interfacial metal-ligand coordination motifs that can significantly affect their physicochemical properties and functionalit...Atomically precise metal nanoclusters are an emerging type of nanomaterial which has diverse interfacial metal-ligand coordination motifs that can significantly affect their physicochemical properties and functionalities.Among that,Cu nanoclusters have been gaining continuous increasing research attentions,thanks to the low cost,diversified structures,and superior catalytic performance for various reactions.In this review,we first summarize the recent progress regarding the synthetic methods of atomically precise Cu nanoclusters and the coordination modes between Cu and several typical ligands and then discuss the catalytic applications of these Cu nanoclusters with some explicit examples to explain the atomical-level structure-performance relationship.Finally,the current challenges and future research perspectives with some critical thoughts are elaborated.We hope this review can not only provide a whole picture of the current advances regarding the synthesis and catalytic applications of atomically precise Cu nanoclusters,but also points out some future research visions in this rapidly booming field.展开更多
Deformable catalytic material with excellent flexible structure is a new type of catalyst that has been applied in various chemical reactions,especially electrocatalytic hydrogen evolution reaction(HER).In recent year...Deformable catalytic material with excellent flexible structure is a new type of catalyst that has been applied in various chemical reactions,especially electrocatalytic hydrogen evolution reaction(HER).In recent years,deformable catalysts for HER have made great progress and would become a research hotspot.The catalytic activities of deformable catalysts could be adjustable by the strain engineering and surface reconfiguration.The surface curvature of flexible catalytic materials is closely related to the electrocatalytic HER properties.Here,firstly,we systematically summarized self-adaptive catalytic performance of deformable catalysts and various micro–nanostructures evolution in catalytic HER process.Secondly,a series of strategies to design highly active catalysts based on the mechanical flexibility of lowdimensional nanomaterials were summarized.Last but not least,we presented the challenges and prospects of the study of flexible and deformable micro–nanostructures of electrocatalysts,which would further deepen the understanding of catalytic mechanisms of deformable HER catalyst.展开更多
Electrochemical water splitting has long been considered an effective energy conversion technology for trans-ferring intermittent renewable electricity into hydrogen fuel,and the exploration of cost-effective and high...Electrochemical water splitting has long been considered an effective energy conversion technology for trans-ferring intermittent renewable electricity into hydrogen fuel,and the exploration of cost-effective and high-performance electrocatalysts is crucial in making electrolyzed water technology commercially viable.Cobalt phosphide(Co-P)has emerged as a catalyst of high potential owing to its high catalytic activity and durability in water splitting.This paper systematically reviews the latest advances in the development of Co-P-based materials for use in water splitting.The essential effects of P in enhancing the catalytic performance of the hydrogen evolution reaction and oxygen evolution reaction are first outlined.Then,versatile synthesis techniques for Co-P electrocatalysts are summarized,followed by advanced strategies to enhance the electrocatalytic performance of Co-P materials,including heteroatom doping,composite construction,integration with well-conductive sub-strates,and structure control from the viewpoint of experiment.Along with these optimization strategies,the understanding of the inherent mechanism of enhanced catalytic performance is also discussed.Finally,some existing challenges in the development of highly active and stable Co-P-based materials are clarified,and pro-spective directions for prompting the wide commercialization of water electrolysis technology are proposed.展开更多
Lithium metal batteries are regarded as prominent contenders to address the pressing needs owing to the high theoretical capacity.Toward the broader implementation,the primary obstacle lies in the intricate multi-elec...Lithium metal batteries are regarded as prominent contenders to address the pressing needs owing to the high theoretical capacity.Toward the broader implementation,the primary obstacle lies in the intricate multi-electron,multi-step redox reaction associated with sluggish conversion kinetics,subsequently giving rise to a cascade of parasitic issues.In order to smooth reaction kinetics,catalysts are widely introduced to accelerate reaction rate via modulating the energy barrier.Over past decades,a large amount of research has been devoted to the catalyst design and catalytic mechanism exploration,and thus the great progress in electrochemical performance has been realized.Therefore,it is necessary to make a comprehensive review toward key progress in catalyst design and future development pathway.In this review,the basic mechanism of lithium metal batteries is provided along with corresponding advantages and existing challenges detailly described.The main catalysts employed to accelerate cathode reaction with emphasis on their catalytic mechanism are summarized as well.Finally,the rational design and innovative direction toward efficient catalysts are suggested for future application in metal-sulfur/gas battery and beyond.This review is expected to drive and benefit future research on rational catalyst design with multi-parameter synergistic impacts on the activity and stability of next-generation metal battery,thus opening new avenue for sustainable solution to climate change,energy and environmental issues,and the potential industrial economy.展开更多
The preparation of bifunctional catalysts for oxygen reduction(ORR)and oxygen evolution(OER)is crucial for Zn-air batteries.Here,we report a La doped CoFe_(2)O_(4) spinel catalyst supported on threedimensional graphen...The preparation of bifunctional catalysts for oxygen reduction(ORR)and oxygen evolution(OER)is crucial for Zn-air batteries.Here,we report a La doped CoFe_(2)O_(4) spinel catalyst supported on threedimensional graphene(3D-G),where La can facilitate electron transfer from Co to Fe,leading to increased electron cloud density in Fe and improved catalytic performance.The redshift of the G peak in the Raman spectra indicates the interaction between theπbond of 3D-G and d orbitals in La_(0.2)CoFe_(1.8)O_(4).La_(0.2)CoFe_(1.8)/3D-G exhibits superior ORR performance(E_(1/2)=0.86 V vs.RHE)and OER performance(E_(j=10)=1.55 V vs.RHE)to CoFe_(2)O_(4)/3D-G(E_(1/2)=0.831 V vs.RHE,E_(j=10)=1.603 V vs.RHE).Furthermore,it demonstrates excellent bifunctional oxygen catalytic performance while maintaining high power density and stability in liquid zinc-air batteries(ZABs)and flexible ZABs(F-ZABs).This work presents a viable strategy for utilizing rare earth element doped spinels to enhance oxygen catalyst and ZABs performance.展开更多
The transformation of aldose to ketose or common sugars into rare saccharides,including rare ketoses and aldoses,is of great value and interest to the food industry and for saccharidic biomass utilization,medicine,and...The transformation of aldose to ketose or common sugars into rare saccharides,including rare ketoses and aldoses,is of great value and interest to the food industry and for saccharidic biomass utilization,medicine,and the synthesis of drugs.Nowadays,high-fructose corn syrup(HFCS)is industrially produced in more than 10 million tons annually using immobilized glucose isomerase.Some low-calorie saccharides such as tagatose and psicose,which are becoming popular sweeteners,have also been produced on a pilot scale in order to replace sucrose and HFCS.However,current catalysts and catalytic processes are still difficult to utilize in biomass conversion and also have strong substrate dependence in producing high-value,rare sugars.Considering the specific reaction properties of saccharides and catalysts,since the pioneering discovery by Fischer,various catalysts and catalytic systems have been discovered or developed in attempts to extend the reaction pathways,improve the reaction efficiency,and to potentially produce commercial products.In this review,we trace the history of sugar isomerization/epimerization reactions and summarize the important breakthroughs for each reaction as well as the difficulties that remain unresolved to date.展开更多
Accurate prediction of the frictional pressure drop is important for the design and operation of subsea oil and gas transporting system considering the length of the pipeline. The applicability of the correlations to ...Accurate prediction of the frictional pressure drop is important for the design and operation of subsea oil and gas transporting system considering the length of the pipeline. The applicability of the correlations to pipeline-riser flow needs evaluation since the flow condition in pipeline-riser is quite different from the original data where they were derived from. In the present study, a comprehensive evaluation of 24prevailing correlation in predicting frictional pressure drop is carried out based on experimentally measured data of air-water and air-oil two-phase flows in pipeline-riser. Experiments are performed in a system having different configuration of pipeline-riser with the inclination of the downcomer varied from-2°to-5°to investigated the effect of the elbow on the frictional pressure drop in the riser. The inlet gas velocity ranges from 0.03 to 6.2 m/s, and liquid velocity varies from 0.02 to 1.3 m/s. A total of885 experimental data points including 782 on air-water flows and 103 on air-oil flows are obtained and used to access the prediction ability of the correlations. Comparison of the predicted results with the measured data indicate that a majority of the investigated correlations under-predict the pressure drop on severe slugging. The result of this study highlights the requirement of new method considering the effect of pipe layout on the frictional pressure drop.展开更多
A novel ultra-stable zeolite, NSZ, rich in secondary pores was developed through the combination of gas-phase andmild hydrothermal methods. This zeolite was successfully tested in an industrial setting for the first t...A novel ultra-stable zeolite, NSZ, rich in secondary pores was developed through the combination of gas-phase andmild hydrothermal methods. This zeolite was successfully tested in an industrial setting for the first time in the world. The porestructure characteristics of the NSZ zeolite prepared for industrial use were analyzed and characterized using BET. The resultsindicate a significant increase in the secondary pore volume of NSZ zeolite compared to the existing ultra-stable zeolite HSZ-5, which is produced through a conventional gas-phase method. The average secondary pore volume to total pore volume ratioin NSZ zeolite was found to be 58.96% higher. The catalytic cracking performance of NSZ zeolite was evaluated. The resultsshowed that the NSC-LTA catalyst, with NSZ as the active component, outperformed the HSC-LTA catalyst with HSZ-5 zeolitein terms of obtaining more high-value products (gasoline and liquefied petroleum gas) during the hydrogenated light cycle oilprocessing. Additionally, the NSC-LTA catalyst showed a significant improvement in coke selectivity.展开更多
Understanding fingering, as a challenge to stable displacement during the immiscible flow, has become a crucial phenomenon for geological carbon sequestration, enhanced oil recovery, and groundwater protection. Typica...Understanding fingering, as a challenge to stable displacement during the immiscible flow, has become a crucial phenomenon for geological carbon sequestration, enhanced oil recovery, and groundwater protection. Typically governed by gravity, viscous and capillary forces, these factors lead invasive fluids to occupy pore space irregularly and incompletely. Previous studies have demonstrated capillary numbers,describing the viscous and capillary forces, to quantificationally induce evolution of invasion patterns.While the evolution mechanisms of invasive patterns have not been deeply elucidated under the constant capillary number and three variable parameters including velocity, viscosity, and interfacial tension.Our research employs two horizontal visualization systems and a two-phase laminar flow simulation to investigate the tendency of invasive pattern transition by various parameters at the pore scale. We showed that increasing invasive viscosity or reducing interfacial tension in a homogeneous pore space significantly enhanced sweep efficiency, under constant capillary number. Additionally, in the fingering crossover pattern, the region near the inlet was prone to capillary fingering with multi-directional invasion, while the viscous fingering with unidirectional invasion was more susceptible occurred in the region near the outlet. Furthermore, increasing invasive viscosity or decreasing invasive velocity and interfacial tension promoted the extension of viscous fingering from the outlet to the inlet, presenting that the subsequent invasive fluid flows toward the outlet. In the case of invasive trunk along a unidirectional path, the invasive flow increased exponentially closer to the outlet, resulting in a significant decrease in the width of the invasive interface. Our work holds promising applications for optimizing invasive patterns in heterogeneous porous media.展开更多
Polymer flooding in fractured wells has been extensively applied in oilfields to enhance oil recovery.In contrast to water,polymer solution exhibits non-Newtonian and nonlinear behavior such as effects of shear thinni...Polymer flooding in fractured wells has been extensively applied in oilfields to enhance oil recovery.In contrast to water,polymer solution exhibits non-Newtonian and nonlinear behavior such as effects of shear thinning and shear thickening,polymer convection,diffusion,adsorption retention,inaccessible pore volume and reduced effective permeability.Meanwhile,the flux density and fracture conductivity along the hydraulic fracture are generally non-uniform due to the effects of pressure distribution,formation damage,and proppant breakage.In this paper,we present an oil-water two-phase flow model that captures these complex non-Newtonian and nonlinear behavior,and non-uniform fracture characteristics in fractured polymer flooding.The hydraulic fracture is firstly divided into two parts:high-conductivity fracture near the wellbore and low-conductivity fracture in the far-wellbore section.A hybrid grid system,including perpendicular bisection(PEBI)and Cartesian grid,is applied to discrete the partial differential flow equations,and the local grid refinement method is applied in the near-wellbore region to accurately calculate the pressure distribution and shear rate of polymer solution.The combination of polymer behavior characterizations and numerical flow simulations are applied,resulting in the calculation for the distribution of water saturation,polymer concentration and reservoir pressure.Compared with the polymer flooding well with uniform fracture conductivity,this non-uniform fracture conductivity model exhibits the larger pressure difference,and the shorter bilinear flow period due to the decrease of fracture flow ability in the far-wellbore section.The field case of the fall-off test demonstrates that the proposed method characterizes fracture characteristics more accurately,and yields fracture half-lengths that better match engineering reality,enabling a quantitative segmented characterization of the near-wellbore section with high fracture conductivity and the far-wellbore section with low fracture conductivity.The novelty of this paper is the analysis of pressure performances caused by the fracture dynamics and polymer rheology,as well as an analysis method that derives formation and fracture parameters based on the pressure and its derivative curves.展开更多
Significant challenges are posed by the limitations of gas sensing mechanisms for trace-level detection of ammonia(NH3).In this study,we propose to exploit single-atom catalytic activation and targeted adsorption prop...Significant challenges are posed by the limitations of gas sensing mechanisms for trace-level detection of ammonia(NH3).In this study,we propose to exploit single-atom catalytic activation and targeted adsorption properties to achieve highly sensitive and selective NH3 gas detection.Specifically,Ni singleatom active sites based on N,C coordination(Ni-N-C)were interfacially confined on the surface of two-dimensional(2D)MXene nanosheets(Ni-N-C/Ti_(3)C_(2)Tx),and a fully flexible gas sensor(MNPE-Ni-N-C/Ti_(3)C_(2)Tx)was integrated.The sensor demonstrates a remarkable response value to 5 ppm NH3(27.3%),excellent selectivity for NH3,and a low theoretical detection limit of 12.1 ppb.Simulation analysis by density functional calculation reveals that the Ni single-atom center with N,C coordination exhibits specific targeted adsorption properties for NH3.Additionally,its catalytic activation effect effectively reduces the Gibbs free energy of the sensing elemental reaction,while its electronic structure promotes the spill-over effect of reactive oxygen species at the gas-solid interface.The sensor has a dual-channel sensing mechanism of both chemical and electronic sensitization,which facilitates efficient electron transfer to the 2D MXene conductive network,resulting in the formation of the NH3 gas molecule sensing signal.Furthermore,the passivation of MXene edge defects by a conjugated hydrogen bond network enhances the long-term stability of MXene-based electrodes under high humidity conditions.This work achieves highly sensitive room-temperature NH3 gas detection based on the catalytic mechanism of Ni single-atom active center with N,C coordination,which provides a novel gas sensing mechanism for room-temperature trace gas detection research.展开更多
Catalytic cracking oil slurry is a by-product of catalytic cracking projects,and the efficient conversion and sustainable utilization of this material are issues of continuous concern in the petroleum refining industr...Catalytic cracking oil slurry is a by-product of catalytic cracking projects,and the efficient conversion and sustainable utilization of this material are issues of continuous concern in the petroleum refining industry.In this study,oxygen-enriched activated carbon is prepared using a one-step KOH activation method with catalytic cracking oil slurry as the raw material.The as-prepared oil slurry-based activated carbon exhibits a high specific surface area of 2102 m^(2)/g,welldefined micropores with an average diameter of 2 nm,and a rich oxygen doping content of 32.97%.The electrochemical performance of the nitrogen-doped porous carbon is tested in a three-electrode system using a 6 mol/L KOH solution as the electrolyte.It achieves a specific capacitance of up to 230 F/g at a current density of 1 A/g.Moreover,the capacitance retention rate exceeds 89%after 10000 charge and discharge cycles,demonstrating excellent cycle stability.This method not only improves the utilization efficiency of industrial fuel waste but also reduces the production cost of supercapacitor electrode materials,thereby providing a simple and effective strategy for the resource utilization of catalytic cracking oil slurries.展开更多
Based on the displacement discontinuity method and the discrete fracture unified pipe network model,a sequential iterative numerical method was used to build a fracturing-production integrated numerical model of shale...Based on the displacement discontinuity method and the discrete fracture unified pipe network model,a sequential iterative numerical method was used to build a fracturing-production integrated numerical model of shale gas well considering the two-phase flow of gas and water.The model accounts for the influence of natural fractures and matrix properties on the fracturing process and directly applies post-fracturing formation pressure and water saturation distribution to subsequent well shut-in and production simulation,allowing for a more accurate fracturing-production integrated simulation.The results show that the reservoir physical properties have great impacts on fracture propagation,and the reasonable prediction of formation pressure and reservoir fluid distribution after the fracturing is critical to accurately predict the gas and fluid production of the shale gas wells.Compared with the conventional method,the proposed model can more accurately simulate the water and gas production by considering the impact of fracturing on both matrix pressure and water saturation.The established model is applied to the integrated fracturing-production simulation of practical horizontal shale gas wells.The simulation results are in good agreement with the practical production data,thus verifying the accuracy of the model.展开更多
The transition metal complexes of triaminoguanidine(TAG-M,where M=Cobalt(Co)or Iron(Fe))have been prepared.The catalytic effect of these complexes on the thermolysis of energetic composite based on nitrocellulose and ...The transition metal complexes of triaminoguanidine(TAG-M,where M=Cobalt(Co)or Iron(Fe))have been prepared.The catalytic effect of these complexes on the thermolysis of energetic composite based on nitrocellulose and diethylene glycol dinitrate,has been investigated.Extensive characterization of the resulting energetic composites was carried out using scanning electron microscopy(SEM),X-ray diffraction(XRD),Fourier transform infrared spectroscopy(FTIR),and differential scanning calorimetry(DSC).Isoconversional kinetic analysis was performed to determine the Arrhenius parameters associated with the thermolysis of the elaborated energetic formulations.It is found that TAG-M complexes have strong catalytic effect on the thermo-kinetic decomposition of NC/DEGDN by decreasing the apparent activation energy and significantly increased the total heat release.The models that govern the decomposition processes are also studied,and it is revealed that different reaction processes are accomplished by introduction metal complexes of triaminoguanidine.Overall,this study serves as a valuable reference for future research focused on the investigation of catalytic combustion features of solid propellants.展开更多
In recent years,porous organic catalysts have been developed and become research hotspots in photo/electrocatalysis due to their inherent pores,high specific surface area,chemical and thermal stability,and diverse fun...In recent years,porous organic catalysts have been developed and become research hotspots in photo/electrocatalysis due to their inherent pores,high specific surface area,chemical and thermal stability,and diverse functional building blocks.Phenazine-linked organic catalysts,exhibited excellent conjugation,electrical conductivity,chemical,and thermal stability,could bring in N atoms with specific numbers and positions to regulate electron levels,anchor metals,and absorb near-infrared light,which expands solar energy utilization.These advantages of the phenazine-linked catalysts attracted our group and numerous researchers to conduct experimental and computational work on photo/electrocatalytic applications and mechanisms.This review summarizes the recent significant research progress,synthesis methods,photo/electrocatalytic performance,and applications of relative phenazine-linked catalysts.Furthermore,the photo/electrocatalytic mechanism was systematized and summarized by combining experiments and density functional theory calculations simultaneously.展开更多
Electrocatalytic CO_(2) reduction reaction (eCO_(2)RR) presents a promising approach for harnessing renewable energy and converting greenhouse gas (CO_(2)) into high value-added CO products.N-doped single atom (SA) an...Electrocatalytic CO_(2) reduction reaction (eCO_(2)RR) presents a promising approach for harnessing renewable energy and converting greenhouse gas (CO_(2)) into high value-added CO products.N-doped single atom (SA) and atomic-level metal nanocluster (MN) tandem catalysts with rich defects for eCO_(2)RR are reported,which achieved a maximum CO Faraday efficiency (FE_(CO)) of 97.7%(-0.7 V vs.RHE) in the H-type cell and maintained over 95% FE_(CO)at potentials from -0.18 to -0.73 V vs.RHE in the flow cell.Furthermore,the catalyst in the flow cell demonstrated a remarkably low onset potential of-0.14 V vs.RHE and the current density was approximately three times that of the H-type cell.Interestingly,XPS analysis indicates that carbon substrates containing defects have more pyridine-N content.DFT calculations and in-situ attenuated total reflection Fourier transform infrared support this finding by showing that the Ni-(N-C_(2))_(3) active sites with defect favors preferentially convert CO_(2)-to-CO.展开更多
Since chemical processes are highly non-linear and multiscale,it is vital to deeply mine the multiscale coupling relationships embedded in the massive process data for the prediction and anomaly tracing of crucial pro...Since chemical processes are highly non-linear and multiscale,it is vital to deeply mine the multiscale coupling relationships embedded in the massive process data for the prediction and anomaly tracing of crucial process parameters and production indicators.While the integrated method of adaptive signal decomposition combined with time series models could effectively predict process variables,it does have limitations in capturing the high-frequency detail of the operation state when applied to complex chemical processes.In light of this,a novel Multiscale Multi-radius Multi-step Convolutional Neural Network(Msrt Net)is proposed for mining spatiotemporal multiscale information.First,the industrial data from the Fluid Catalytic Cracking(FCC)process decomposition using Complete Ensemble Empirical Mode Decomposition with Adaptive Noise(CEEMDAN)extract the multi-energy scale information of the feature subset.Then,convolution kernels with varying stride and padding structures are established to decouple the long-period operation process information encapsulated within the multi-energy scale data.Finally,a reconciliation network is trained to reconstruct the multiscale prediction results and obtain the final output.Msrt Net is initially assessed for its capability to untangle the spatiotemporal multiscale relationships among variables in the Tennessee Eastman Process(TEP).Subsequently,the performance of Msrt Net is evaluated in predicting product yield for a 2.80×10^(6) t/a FCC unit,taking diesel and gasoline yield as examples.In conclusion,Msrt Net can decouple and effectively extract spatiotemporal multiscale information from chemical process data and achieve a approximately reduction of 30%in prediction error compared to other time-series models.Furthermore,its robustness and transferability underscore its promising potential for broader applications.展开更多
Fe-Al catalysts with hollow nano-spherical structures were synthesized following the hard template method using self-made carbon spheres as templates.The catalytic performance of these catalysts in the production of c...Fe-Al catalysts with hollow nano-spherical structures were synthesized following the hard template method using self-made carbon spheres as templates.The catalytic performance of these catalysts in the production of carbon nanotubes(CNTs)was evaluated through ethane catalytic cracking on a fixed bed reactor.Furthermore,the influence of these hollow nanospheres on the yield and quality of CNTs was investigated.The results showed that compared to the irregular-shaped catalyst synthesized by coprecipitation and the catalyst with micro-spherical structures prepared by the impregnation method,the Fe-Al hollow nano-spherical catalysts exhibited significantly enhanced specific surface area and pore volume,reaching 236 m^(2)/g and 0.77 cm^(3)/g,respectively.At a reaction temperature of 700℃ and an ethane feed rate of 90 mL/min,the CNTs yield of Fe-Al hollow nano-spherical catalyst reached as high as 48.6 gCNT/gcat,which was 1.8 and 4.6 times higher than the yield of irregular-shaped(27.7 gCNT/gcat)and micro-spherical(10.5 gCNT/gcat)catalysts,respectively.This was mainly attributed to the hollow cavity structure of Fe-Al catalyst providing sufficient space for the CNTs growth.As a result,the blockage of catalyst internal pores was prevented by the formed CNTs,which isolated ethane molecules from the active sites and lead to catalyst deactivation.Furthermore,the CNTs synthesized by Fe-Al hollow nano-spherical catalyst exhibited a uniform diameter distribution and a higher degree of graphitization.展开更多
基金supported by the Fundamental Research Funds for the Central Universities(QNTD202302)National Natural Science Foundation of China(22378024)the Foreign expert program(G2022109001L).
文摘Developing a cost-effective and environmentally friendly process for the production of valuable chemicals from abundant herbal biomass receives great attentions in recent years.Herein,taking advantage of the“lignin first”strategy,corn straw is converted to valuable chemicals including lignin monomers,furfural and 5-methoxymethylfurfural via a two steps process.The key of this research lies in the development of a green and low-cost catalytic process utilizing magnetic Raney Ni catalyst and high boiling point ethylene glycol.The utilization of neat ethylene glycol as the sole slovent under atmospheric conditions obviates the need for additional additives,thereby facilitating the entire process to be conducted in glass flasks and rendering it highly convenient for scaling up.In the initial step,depolymerization of corn straw lignin resulted in a monomer yield of 18.1 wt%.Subsequently,in a dimethyl carbonate system,the carbohydrate component underwent complete conversion in a one-pot process,yielding furfural and 5-methoxymethylfurfural as the primary products with an impressive yield of 47.7%.
基金Financial support from the National Natural Science Foundation of China(51972016)the Fundamental Research Funds for the Central Universities(JD2417)is gratefully acknowledged.
文摘Although solar steam generation strategy is efficient in desalinating seawater,it is still challenging to achieve continuous solar-thermal desalination of seawater and catalytic degradation of organic pollutants.Herein,dynamic regulations of hydrogen bonding networks and solvation structures are realized by designing an asymmetric bilayer membrane consisting of a bacterial cellulose/carbon nanotube/Co_(2)(OH)_(2)CO_(3)nanorod top layer and a bacterial cellulose/Co_(2)(OH)_(2)CO_(3)nanorod(BCH)bottom layer.Crucially,the hydrogen bonding networks inside the membrane can be tuned by the rich surface–OH groups of the bacterial cellulose and Co_(2)(OH)_(2)CO_(3)as well as the ions and radicals in situ generated during the catalysis process.Moreover,both SO_(4)^(2−)and HSO_(5)−can regulate the solvation structure of Na^(+)and be adsorbed more preferentially on the evaporation surface than Cl^(−),thus hindering the de-solvation of the solvated Na^(+)and subsequent nucleation/growth of NaCl.Furthermore,the heat generated by the solar-thermal energy conversion can accelerate the reaction kinetics and enhance the catalytic degradation efficiency.This work provides a flow-bed water purification system with an asymmetric solar-thermal and catalytic membrane for synergistic solar thermal desalination of seawater/brine and catalytic degradation of organic pollutants.
基金supported by the open funds of Key Laboratory of Functional Inorganic Material Chemistry (Heilongjiang University), Ministry of Education, Chinathe funding from Guangdong Natural Science Funds (No. 2023A0505050107)。
文摘Atomically precise metal nanoclusters are an emerging type of nanomaterial which has diverse interfacial metal-ligand coordination motifs that can significantly affect their physicochemical properties and functionalities.Among that,Cu nanoclusters have been gaining continuous increasing research attentions,thanks to the low cost,diversified structures,and superior catalytic performance for various reactions.In this review,we first summarize the recent progress regarding the synthetic methods of atomically precise Cu nanoclusters and the coordination modes between Cu and several typical ligands and then discuss the catalytic applications of these Cu nanoclusters with some explicit examples to explain the atomical-level structure-performance relationship.Finally,the current challenges and future research perspectives with some critical thoughts are elaborated.We hope this review can not only provide a whole picture of the current advances regarding the synthesis and catalytic applications of atomically precise Cu nanoclusters,but also points out some future research visions in this rapidly booming field.
基金This work was financially supported by the National Natural Science Foundation of China(Nos.51902101 and 21875203)the Natural Science Foundation of Hunan Province(Nos.2021JJ40044 and 2023JJ50287)Natural Science Foundation of Jiangsu Province(No.BK20201381).
文摘Deformable catalytic material with excellent flexible structure is a new type of catalyst that has been applied in various chemical reactions,especially electrocatalytic hydrogen evolution reaction(HER).In recent years,deformable catalysts for HER have made great progress and would become a research hotspot.The catalytic activities of deformable catalysts could be adjustable by the strain engineering and surface reconfiguration.The surface curvature of flexible catalytic materials is closely related to the electrocatalytic HER properties.Here,firstly,we systematically summarized self-adaptive catalytic performance of deformable catalysts and various micro–nanostructures evolution in catalytic HER process.Secondly,a series of strategies to design highly active catalysts based on the mechanical flexibility of lowdimensional nanomaterials were summarized.Last but not least,we presented the challenges and prospects of the study of flexible and deformable micro–nanostructures of electrocatalysts,which would further deepen the understanding of catalytic mechanisms of deformable HER catalyst.
基金the National Natural Science Foundation of China(21962008)Yunnan Province Excellent Youth Fund Project(202001AW070005)+1 种基金Candidate Talents Training Fund of Yunnan Province(2017PY269SQ,2018HB007)Yunnan Ten Thousand Talents Plan Young&Elite Talents Project(YNWR-QNBJ-2018-346).
文摘Electrochemical water splitting has long been considered an effective energy conversion technology for trans-ferring intermittent renewable electricity into hydrogen fuel,and the exploration of cost-effective and high-performance electrocatalysts is crucial in making electrolyzed water technology commercially viable.Cobalt phosphide(Co-P)has emerged as a catalyst of high potential owing to its high catalytic activity and durability in water splitting.This paper systematically reviews the latest advances in the development of Co-P-based materials for use in water splitting.The essential effects of P in enhancing the catalytic performance of the hydrogen evolution reaction and oxygen evolution reaction are first outlined.Then,versatile synthesis techniques for Co-P electrocatalysts are summarized,followed by advanced strategies to enhance the electrocatalytic performance of Co-P materials,including heteroatom doping,composite construction,integration with well-conductive sub-strates,and structure control from the viewpoint of experiment.Along with these optimization strategies,the understanding of the inherent mechanism of enhanced catalytic performance is also discussed.Finally,some existing challenges in the development of highly active and stable Co-P-based materials are clarified,and pro-spective directions for prompting the wide commercialization of water electrolysis technology are proposed.
基金supported by the National Natural Science Foundation of China(52272194)Liaoning Revitalization Talents Program(XLYC2007155)。
文摘Lithium metal batteries are regarded as prominent contenders to address the pressing needs owing to the high theoretical capacity.Toward the broader implementation,the primary obstacle lies in the intricate multi-electron,multi-step redox reaction associated with sluggish conversion kinetics,subsequently giving rise to a cascade of parasitic issues.In order to smooth reaction kinetics,catalysts are widely introduced to accelerate reaction rate via modulating the energy barrier.Over past decades,a large amount of research has been devoted to the catalyst design and catalytic mechanism exploration,and thus the great progress in electrochemical performance has been realized.Therefore,it is necessary to make a comprehensive review toward key progress in catalyst design and future development pathway.In this review,the basic mechanism of lithium metal batteries is provided along with corresponding advantages and existing challenges detailly described.The main catalysts employed to accelerate cathode reaction with emphasis on their catalytic mechanism are summarized as well.Finally,the rational design and innovative direction toward efficient catalysts are suggested for future application in metal-sulfur/gas battery and beyond.This review is expected to drive and benefit future research on rational catalyst design with multi-parameter synergistic impacts on the activity and stability of next-generation metal battery,thus opening new avenue for sustainable solution to climate change,energy and environmental issues,and the potential industrial economy.
基金financially supported by the National Natural Science Foundation of China(22172093 and 21776167)the Natural Science Foundation of Shandong Province,China(ZR2023MB061).
文摘The preparation of bifunctional catalysts for oxygen reduction(ORR)and oxygen evolution(OER)is crucial for Zn-air batteries.Here,we report a La doped CoFe_(2)O_(4) spinel catalyst supported on threedimensional graphene(3D-G),where La can facilitate electron transfer from Co to Fe,leading to increased electron cloud density in Fe and improved catalytic performance.The redshift of the G peak in the Raman spectra indicates the interaction between theπbond of 3D-G and d orbitals in La_(0.2)CoFe_(1.8)O_(4).La_(0.2)CoFe_(1.8)/3D-G exhibits superior ORR performance(E_(1/2)=0.86 V vs.RHE)and OER performance(E_(j=10)=1.55 V vs.RHE)to CoFe_(2)O_(4)/3D-G(E_(1/2)=0.831 V vs.RHE,E_(j=10)=1.603 V vs.RHE).Furthermore,it demonstrates excellent bifunctional oxygen catalytic performance while maintaining high power density and stability in liquid zinc-air batteries(ZABs)and flexible ZABs(F-ZABs).This work presents a viable strategy for utilizing rare earth element doped spinels to enhance oxygen catalyst and ZABs performance.
基金Financial support by Dual Initiative Project of Jiangsu Province and Changzhou University is gratefully acknowledgedSample analysis supported by Analysis and Testing Center,NERC Biomass of Changzhou University was also greatly acknowledged.
文摘The transformation of aldose to ketose or common sugars into rare saccharides,including rare ketoses and aldoses,is of great value and interest to the food industry and for saccharidic biomass utilization,medicine,and the synthesis of drugs.Nowadays,high-fructose corn syrup(HFCS)is industrially produced in more than 10 million tons annually using immobilized glucose isomerase.Some low-calorie saccharides such as tagatose and psicose,which are becoming popular sweeteners,have also been produced on a pilot scale in order to replace sucrose and HFCS.However,current catalysts and catalytic processes are still difficult to utilize in biomass conversion and also have strong substrate dependence in producing high-value,rare sugars.Considering the specific reaction properties of saccharides and catalysts,since the pioneering discovery by Fischer,various catalysts and catalytic systems have been discovered or developed in attempts to extend the reaction pathways,improve the reaction efficiency,and to potentially produce commercial products.In this review,we trace the history of sugar isomerization/epimerization reactions and summarize the important breakthroughs for each reaction as well as the difficulties that remain unresolved to date.
基金the support of the Opening Fund of State Key Laboratory of Multiphase Flow in Power Engineering(SKLMF-KF-2102)。
文摘Accurate prediction of the frictional pressure drop is important for the design and operation of subsea oil and gas transporting system considering the length of the pipeline. The applicability of the correlations to pipeline-riser flow needs evaluation since the flow condition in pipeline-riser is quite different from the original data where they were derived from. In the present study, a comprehensive evaluation of 24prevailing correlation in predicting frictional pressure drop is carried out based on experimentally measured data of air-water and air-oil two-phase flows in pipeline-riser. Experiments are performed in a system having different configuration of pipeline-riser with the inclination of the downcomer varied from-2°to-5°to investigated the effect of the elbow on the frictional pressure drop in the riser. The inlet gas velocity ranges from 0.03 to 6.2 m/s, and liquid velocity varies from 0.02 to 1.3 m/s. A total of885 experimental data points including 782 on air-water flows and 103 on air-oil flows are obtained and used to access the prediction ability of the correlations. Comparison of the predicted results with the measured data indicate that a majority of the investigated correlations under-predict the pressure drop on severe slugging. The result of this study highlights the requirement of new method considering the effect of pipe layout on the frictional pressure drop.
基金the National Key R&D Program of China(2022YFA1504404)the SINOPEC Research Program(121036-5).
文摘A novel ultra-stable zeolite, NSZ, rich in secondary pores was developed through the combination of gas-phase andmild hydrothermal methods. This zeolite was successfully tested in an industrial setting for the first time in the world. The porestructure characteristics of the NSZ zeolite prepared for industrial use were analyzed and characterized using BET. The resultsindicate a significant increase in the secondary pore volume of NSZ zeolite compared to the existing ultra-stable zeolite HSZ-5, which is produced through a conventional gas-phase method. The average secondary pore volume to total pore volume ratioin NSZ zeolite was found to be 58.96% higher. The catalytic cracking performance of NSZ zeolite was evaluated. The resultsshowed that the NSC-LTA catalyst, with NSZ as the active component, outperformed the HSC-LTA catalyst with HSZ-5 zeolitein terms of obtaining more high-value products (gasoline and liquefied petroleum gas) during the hydrogenated light cycle oilprocessing. Additionally, the NSC-LTA catalyst showed a significant improvement in coke selectivity.
基金supported by the National Natural Science Foundation of China Joint Fund Project (Grant/Award Number: U20B6003)National Natural Science Foundation of China (Grant/Award Number: 52304054)。
文摘Understanding fingering, as a challenge to stable displacement during the immiscible flow, has become a crucial phenomenon for geological carbon sequestration, enhanced oil recovery, and groundwater protection. Typically governed by gravity, viscous and capillary forces, these factors lead invasive fluids to occupy pore space irregularly and incompletely. Previous studies have demonstrated capillary numbers,describing the viscous and capillary forces, to quantificationally induce evolution of invasion patterns.While the evolution mechanisms of invasive patterns have not been deeply elucidated under the constant capillary number and three variable parameters including velocity, viscosity, and interfacial tension.Our research employs two horizontal visualization systems and a two-phase laminar flow simulation to investigate the tendency of invasive pattern transition by various parameters at the pore scale. We showed that increasing invasive viscosity or reducing interfacial tension in a homogeneous pore space significantly enhanced sweep efficiency, under constant capillary number. Additionally, in the fingering crossover pattern, the region near the inlet was prone to capillary fingering with multi-directional invasion, while the viscous fingering with unidirectional invasion was more susceptible occurred in the region near the outlet. Furthermore, increasing invasive viscosity or decreasing invasive velocity and interfacial tension promoted the extension of viscous fingering from the outlet to the inlet, presenting that the subsequent invasive fluid flows toward the outlet. In the case of invasive trunk along a unidirectional path, the invasive flow increased exponentially closer to the outlet, resulting in a significant decrease in the width of the invasive interface. Our work holds promising applications for optimizing invasive patterns in heterogeneous porous media.
基金This work is supported by the National Natural Science Foundation of China(No.52104049)the Young Elite Scientist Sponsorship Program by Beijing Association for Science and Technology(No.BYESS2023262)Science Foundation of China University of Petroleum,Beijing(No.2462022BJRC004).
文摘Polymer flooding in fractured wells has been extensively applied in oilfields to enhance oil recovery.In contrast to water,polymer solution exhibits non-Newtonian and nonlinear behavior such as effects of shear thinning and shear thickening,polymer convection,diffusion,adsorption retention,inaccessible pore volume and reduced effective permeability.Meanwhile,the flux density and fracture conductivity along the hydraulic fracture are generally non-uniform due to the effects of pressure distribution,formation damage,and proppant breakage.In this paper,we present an oil-water two-phase flow model that captures these complex non-Newtonian and nonlinear behavior,and non-uniform fracture characteristics in fractured polymer flooding.The hydraulic fracture is firstly divided into two parts:high-conductivity fracture near the wellbore and low-conductivity fracture in the far-wellbore section.A hybrid grid system,including perpendicular bisection(PEBI)and Cartesian grid,is applied to discrete the partial differential flow equations,and the local grid refinement method is applied in the near-wellbore region to accurately calculate the pressure distribution and shear rate of polymer solution.The combination of polymer behavior characterizations and numerical flow simulations are applied,resulting in the calculation for the distribution of water saturation,polymer concentration and reservoir pressure.Compared with the polymer flooding well with uniform fracture conductivity,this non-uniform fracture conductivity model exhibits the larger pressure difference,and the shorter bilinear flow period due to the decrease of fracture flow ability in the far-wellbore section.The field case of the fall-off test demonstrates that the proposed method characterizes fracture characteristics more accurately,and yields fracture half-lengths that better match engineering reality,enabling a quantitative segmented characterization of the near-wellbore section with high fracture conductivity and the far-wellbore section with low fracture conductivity.The novelty of this paper is the analysis of pressure performances caused by the fracture dynamics and polymer rheology,as well as an analysis method that derives formation and fracture parameters based on the pressure and its derivative curves.
基金supported by the National Key Research and Development Program of China(2022YFB3205500)the National Natural Science Foundation of China(62371299,62301314 and 62101329)+2 种基金the China Postdoctoral Science Foundation(2023M732198)the Natural Science Foundation of Shanghai(23ZR1430100)supported by the Center for High-Performance Computing at Shanghai Jiao Tong University.
文摘Significant challenges are posed by the limitations of gas sensing mechanisms for trace-level detection of ammonia(NH3).In this study,we propose to exploit single-atom catalytic activation and targeted adsorption properties to achieve highly sensitive and selective NH3 gas detection.Specifically,Ni singleatom active sites based on N,C coordination(Ni-N-C)were interfacially confined on the surface of two-dimensional(2D)MXene nanosheets(Ni-N-C/Ti_(3)C_(2)Tx),and a fully flexible gas sensor(MNPE-Ni-N-C/Ti_(3)C_(2)Tx)was integrated.The sensor demonstrates a remarkable response value to 5 ppm NH3(27.3%),excellent selectivity for NH3,and a low theoretical detection limit of 12.1 ppb.Simulation analysis by density functional calculation reveals that the Ni single-atom center with N,C coordination exhibits specific targeted adsorption properties for NH3.Additionally,its catalytic activation effect effectively reduces the Gibbs free energy of the sensing elemental reaction,while its electronic structure promotes the spill-over effect of reactive oxygen species at the gas-solid interface.The sensor has a dual-channel sensing mechanism of both chemical and electronic sensitization,which facilitates efficient electron transfer to the 2D MXene conductive network,resulting in the formation of the NH3 gas molecule sensing signal.Furthermore,the passivation of MXene edge defects by a conjugated hydrogen bond network enhances the long-term stability of MXene-based electrodes under high humidity conditions.This work achieves highly sensitive room-temperature NH3 gas detection based on the catalytic mechanism of Ni single-atom active center with N,C coordination,which provides a novel gas sensing mechanism for room-temperature trace gas detection research.
基金the National Natural Science Foundation of China(52206262)Small and Medium-sized Sci-tech Enterprises Innovation Capability Improvement Project of Shandong Province,China(2022TSGC2248,2023TSGC0579)+1 种基金Talent Research Project of Qilu University of Technology(Shandong Academy of Sciences)(2023RCKY170)Natural Science Foundation of Shandong Province,China(ZR2020ME191).
文摘Catalytic cracking oil slurry is a by-product of catalytic cracking projects,and the efficient conversion and sustainable utilization of this material are issues of continuous concern in the petroleum refining industry.In this study,oxygen-enriched activated carbon is prepared using a one-step KOH activation method with catalytic cracking oil slurry as the raw material.The as-prepared oil slurry-based activated carbon exhibits a high specific surface area of 2102 m^(2)/g,welldefined micropores with an average diameter of 2 nm,and a rich oxygen doping content of 32.97%.The electrochemical performance of the nitrogen-doped porous carbon is tested in a three-electrode system using a 6 mol/L KOH solution as the electrolyte.It achieves a specific capacitance of up to 230 F/g at a current density of 1 A/g.Moreover,the capacitance retention rate exceeds 89%after 10000 charge and discharge cycles,demonstrating excellent cycle stability.This method not only improves the utilization efficiency of industrial fuel waste but also reduces the production cost of supercapacitor electrode materials,thereby providing a simple and effective strategy for the resource utilization of catalytic cracking oil slurries.
基金Supported by the National Natural Science Foundation of China(52374043)Key Program of the National Natural Science Foundation of China(52234003).
文摘Based on the displacement discontinuity method and the discrete fracture unified pipe network model,a sequential iterative numerical method was used to build a fracturing-production integrated numerical model of shale gas well considering the two-phase flow of gas and water.The model accounts for the influence of natural fractures and matrix properties on the fracturing process and directly applies post-fracturing formation pressure and water saturation distribution to subsequent well shut-in and production simulation,allowing for a more accurate fracturing-production integrated simulation.The results show that the reservoir physical properties have great impacts on fracture propagation,and the reasonable prediction of formation pressure and reservoir fluid distribution after the fracturing is critical to accurately predict the gas and fluid production of the shale gas wells.Compared with the conventional method,the proposed model can more accurately simulate the water and gas production by considering the impact of fracturing on both matrix pressure and water saturation.The established model is applied to the integrated fracturing-production simulation of practical horizontal shale gas wells.The simulation results are in good agreement with the practical production data,thus verifying the accuracy of the model.
文摘The transition metal complexes of triaminoguanidine(TAG-M,where M=Cobalt(Co)or Iron(Fe))have been prepared.The catalytic effect of these complexes on the thermolysis of energetic composite based on nitrocellulose and diethylene glycol dinitrate,has been investigated.Extensive characterization of the resulting energetic composites was carried out using scanning electron microscopy(SEM),X-ray diffraction(XRD),Fourier transform infrared spectroscopy(FTIR),and differential scanning calorimetry(DSC).Isoconversional kinetic analysis was performed to determine the Arrhenius parameters associated with the thermolysis of the elaborated energetic formulations.It is found that TAG-M complexes have strong catalytic effect on the thermo-kinetic decomposition of NC/DEGDN by decreasing the apparent activation energy and significantly increased the total heat release.The models that govern the decomposition processes are also studied,and it is revealed that different reaction processes are accomplished by introduction metal complexes of triaminoguanidine.Overall,this study serves as a valuable reference for future research focused on the investigation of catalytic combustion features of solid propellants.
基金supported by the Natural Science Foundation of China(52273288 and U2102211)the Natural Science Foundation of Heilongjiang Province of China(LH2021B014)the Fundamental Research Foundation for Universities of Heilongjiang Province(2021-KYYWF-0004).
文摘In recent years,porous organic catalysts have been developed and become research hotspots in photo/electrocatalysis due to their inherent pores,high specific surface area,chemical and thermal stability,and diverse functional building blocks.Phenazine-linked organic catalysts,exhibited excellent conjugation,electrical conductivity,chemical,and thermal stability,could bring in N atoms with specific numbers and positions to regulate electron levels,anchor metals,and absorb near-infrared light,which expands solar energy utilization.These advantages of the phenazine-linked catalysts attracted our group and numerous researchers to conduct experimental and computational work on photo/electrocatalytic applications and mechanisms.This review summarizes the recent significant research progress,synthesis methods,photo/electrocatalytic performance,and applications of relative phenazine-linked catalysts.Furthermore,the photo/electrocatalytic mechanism was systematized and summarized by combining experiments and density functional theory calculations simultaneously.
基金supported by the Tianjin Science and Technology support key projects (20JCYBJC01420)。
文摘Electrocatalytic CO_(2) reduction reaction (eCO_(2)RR) presents a promising approach for harnessing renewable energy and converting greenhouse gas (CO_(2)) into high value-added CO products.N-doped single atom (SA) and atomic-level metal nanocluster (MN) tandem catalysts with rich defects for eCO_(2)RR are reported,which achieved a maximum CO Faraday efficiency (FE_(CO)) of 97.7%(-0.7 V vs.RHE) in the H-type cell and maintained over 95% FE_(CO)at potentials from -0.18 to -0.73 V vs.RHE in the flow cell.Furthermore,the catalyst in the flow cell demonstrated a remarkably low onset potential of-0.14 V vs.RHE and the current density was approximately three times that of the H-type cell.Interestingly,XPS analysis indicates that carbon substrates containing defects have more pyridine-N content.DFT calculations and in-situ attenuated total reflection Fourier transform infrared support this finding by showing that the Ni-(N-C_(2))_(3) active sites with defect favors preferentially convert CO_(2)-to-CO.
文摘Since chemical processes are highly non-linear and multiscale,it is vital to deeply mine the multiscale coupling relationships embedded in the massive process data for the prediction and anomaly tracing of crucial process parameters and production indicators.While the integrated method of adaptive signal decomposition combined with time series models could effectively predict process variables,it does have limitations in capturing the high-frequency detail of the operation state when applied to complex chemical processes.In light of this,a novel Multiscale Multi-radius Multi-step Convolutional Neural Network(Msrt Net)is proposed for mining spatiotemporal multiscale information.First,the industrial data from the Fluid Catalytic Cracking(FCC)process decomposition using Complete Ensemble Empirical Mode Decomposition with Adaptive Noise(CEEMDAN)extract the multi-energy scale information of the feature subset.Then,convolution kernels with varying stride and padding structures are established to decouple the long-period operation process information encapsulated within the multi-energy scale data.Finally,a reconciliation network is trained to reconstruct the multiscale prediction results and obtain the final output.Msrt Net is initially assessed for its capability to untangle the spatiotemporal multiscale relationships among variables in the Tennessee Eastman Process(TEP).Subsequently,the performance of Msrt Net is evaluated in predicting product yield for a 2.80×10^(6) t/a FCC unit,taking diesel and gasoline yield as examples.In conclusion,Msrt Net can decouple and effectively extract spatiotemporal multiscale information from chemical process data and achieve a approximately reduction of 30%in prediction error compared to other time-series models.Furthermore,its robustness and transferability underscore its promising potential for broader applications.
文摘Fe-Al catalysts with hollow nano-spherical structures were synthesized following the hard template method using self-made carbon spheres as templates.The catalytic performance of these catalysts in the production of carbon nanotubes(CNTs)was evaluated through ethane catalytic cracking on a fixed bed reactor.Furthermore,the influence of these hollow nanospheres on the yield and quality of CNTs was investigated.The results showed that compared to the irregular-shaped catalyst synthesized by coprecipitation and the catalyst with micro-spherical structures prepared by the impregnation method,the Fe-Al hollow nano-spherical catalysts exhibited significantly enhanced specific surface area and pore volume,reaching 236 m^(2)/g and 0.77 cm^(3)/g,respectively.At a reaction temperature of 700℃ and an ethane feed rate of 90 mL/min,the CNTs yield of Fe-Al hollow nano-spherical catalyst reached as high as 48.6 gCNT/gcat,which was 1.8 and 4.6 times higher than the yield of irregular-shaped(27.7 gCNT/gcat)and micro-spherical(10.5 gCNT/gcat)catalysts,respectively.This was mainly attributed to the hollow cavity structure of Fe-Al catalyst providing sufficient space for the CNTs growth.As a result,the blockage of catalyst internal pores was prevented by the formed CNTs,which isolated ethane molecules from the active sites and lead to catalyst deactivation.Furthermore,the CNTs synthesized by Fe-Al hollow nano-spherical catalyst exhibited a uniform diameter distribution and a higher degree of graphitization.
