Chemical synthesis is essential in industries such as petrochemicals, fine chemicals, and pharmaceuticals, driving economic and social development. The increasing demand for new molecules and materials calls for novel...Chemical synthesis is essential in industries such as petrochemicals, fine chemicals, and pharmaceuticals, driving economic and social development. The increasing demand for new molecules and materials calls for novel chemical reactions;however, manual experimental screening is time-consuming. Artificial intelligence (AI) offers a promising solution by leveraging large-scale experimental data to model chemical reactions, although challenges such as the lack of standardization and predictability in chemical synthesis hinder AI applications. Additionally, the multi-scale nature of chemical reactions, along with complex multiphase processes, further complicates the task. Recent advances in microchemical systems, particularly continuous flow methods using microreactors, provide precise control over reaction conditions, enhancing reproducibility and enabling high-throughput experimentation. These systems minimize transport-related inconsistencies and facilitate scalable industrial applications. This review systematically explores recent developments in intelligent synthesis based on microchemical systems, focusing on reaction system design, synthesis robots, closed-loop optimization, and high-throughput experimentation, while identifying key areas for future research.展开更多
Rechargeable lithium-ion batteries(LIBs)afford a profound impact on our modern daily life.However,LIBs are approaching the theoretical energy density,due to the inherent limitations of intercalation chemistry;thus,the...Rechargeable lithium-ion batteries(LIBs)afford a profound impact on our modern daily life.However,LIBs are approaching the theoretical energy density,due to the inherent limitations of intercalation chemistry;thus,they cannot further satisfy the increasing demands of portable electronics,electric vehicles,and grids.Therefore,battery chemistries beyond LIBs are being widely investigated.Next-generation lithium(Li)batteries,which employ Li metal as the anode and intercalation or conversion materials as the cathode,receive the most intensive interest due to their high energy density and excellent potential for commercialization.Moreover,significant progress has been achieved in Li batteries attributed to the increasing fundamental understanding of the materials and reactions,as well as to technological improvement.This review starts by summarizing the electrolytes for next-generation Li batteries.Key challenges and recent progress in lithium-ion,lithium–sulfur,and lithium–oxygen batteries are then reviewed from the perspective of energy and chemical engineering science.Finally,possible directions for further development in Li batteries are presented.Next-generation Li batteries are expected to promote the sustainable development of human civilization.展开更多
This paper discussed an extended model for flexibility analysis of chemical process. Under uncertainty, probability density function is used to describe uncertain parameters instead of hyper-rectangle, and chanceconst...This paper discussed an extended model for flexibility analysis of chemical process. Under uncertainty, probability density function is used to describe uncertain parameters instead of hyper-rectangle, and chanceconstrained programming is a feasible way to deal with the violation of constraints. Because the feasible region of control variables would change along with uncertain parameters, its smallest acceptable size threshold is presented to ensure the controllability condition. By synthesizing the considerations mentioned above, a modified model can describe the flexibility analysis problem more exactly. Then a hybrid algorithm, which integrates stochastic simulation and genetic algorithm, is applied to solve this model and maximize the flexibility region. Both numerical and chemical process examples are presented to demonstrate the effectiveness of the method.展开更多
In the preliminary stage of chemical process design, the choice of chemical reaction route is the key design decision, and the concepts of atom utilization and environmental quotient have become extremely useful tools...In the preliminary stage of chemical process design, the choice of chemical reaction route is the key design decision, and the concepts of atom utilization and environmental quotient have become extremely useful tools. However, the waste quality such as chemical toxicity and other engineering factors have not been taken into account. Therefore, a synthetic route selection index, Iroute, is proposed to determine the suitability of a chemical route in this paper. Iroute considers the effects of 'extended atom economy', material renewability, chemical characteristics and some engineering factors. The extended atom economy concept regards not only the value of the desired product but also the value of byproducts. The methodology by using Iroute to compare different routes is illustrated in case study of cyclohexanone oxime and acrylonitrile manufacture.展开更多
The concept of“carbon neutrality”poses a huge challenge for chemical engineering and brings great opportunities for boosting the development of novel technologies to realize carbon offsetting and reduce carbon emiss...The concept of“carbon neutrality”poses a huge challenge for chemical engineering and brings great opportunities for boosting the development of novel technologies to realize carbon offsetting and reduce carbon emissions.Developing high-efficient,low-cost,energy-efficient and eco-friendly microfluidicbased microchemical engineering is of great significance.Such kind of“green microfluidics”can reduce carbon emissions from the source of raw materials and facilitate controllable and intensified microchemical engineering processes,which represents the new power for the transformation and upgrading of chemical engineering industry.Here,a brief review of green microfluidics for achieving carbon neutral microchemical engineering is presented,with specific discussions about the characteristics and feasibility of applying green microfluidics in realizing carbon neutrality.Development of green microfluidic systems are categorized and reviewed,including the construction of microfluidic devices by bio-based substrate materials and by low carbon fabrication methods,and the use of more biocompatible and nondestructive fluidic systems such as aqueous two-phase systems(ATPSs).Moreover,low carbon applications benefit from green microfluidics are summarized,ranging from separation and purification of biomolecules,high-throughput screening of chemicals and drugs,rapid and cost-effective detections,to synthesis of fine chemicals and novel materials.Finally,challenges and perspectives for further advancing green microfluidics in microchemical engineering for carbon neutrality are proposed and discussed.展开更多
This review focuses on the application of process engineering in electrochemical energy conversion and storage devices innovation. For polymer electrolyte based devices, it highlights that a strategic simple switch fr...This review focuses on the application of process engineering in electrochemical energy conversion and storage devices innovation. For polymer electrolyte based devices, it highlights that a strategic simple switch from proton exchange membranes(PEMs) to hydroxide exchange membranes(HEMs) may lead to a new-generation of affordable electrochemical energy devices including fuel cells, electrolyzers, and solar hydrogen generators. For lithium-ion batteries, a series of advancements in design and chemistry are required for electric vehicle and energy storage applications. Manufacturing process development and optimization of the LiF eP O_4/C cathode materials and several emerging novel anode materials are also discussed using the authors' work as examples.Design and manufacturing process of lithium-ion battery electrodes are introduced in detail, and modeling and optimization of large-scale lithium-ion batteries are also presented. Electrochemical energy materials and device innovations can be further prompted by better understanding of the fundamental transport phenomena involved in unit operations.展开更多
Heavy-metal-free ternary Cu–In–Se quantum dots(CISe QDs)are promising for solar fuel production because of their low toxicity,tunable band gap,and high light absorption coefficient.Although defects significantly aff...Heavy-metal-free ternary Cu–In–Se quantum dots(CISe QDs)are promising for solar fuel production because of their low toxicity,tunable band gap,and high light absorption coefficient.Although defects significantly affect the photophysical properties of QDs,the influence on photoelectrochemical hydrogen production is not well understood.Herein,we present the defect engineering of CISe QDs for efficient solar-energy conversion.Lewis acid–base reactions between metal halide–oleylamine complexes and oleylammonium selenocarbamate are modulated to achieve CISe QDs with the controlled amount of Cu vacancies without changing their morphology.Among them,CISe QDs with In/Cu=1.55 show the most outstanding photoelectrochemical hydrogen generation with excellent photocurrent density of up to 10.7 mA cm-2(at 0.6 VRHE),attributed to the suitable electronic band structures and enhanced carrier concentrations/lifetimes of the QDs.The proposed method,which can effectively control the defects in heavy-metal-free ternary QDs,offers a deeper understanding of the effects of the defects and provides a practical approach to enhance photoelectrochemical hydrogen generation.展开更多
The zebra mussel is an important aquatic pest that causes great damage to freshwater-dependent industries, due to biofouling. The main goal of the project discussed here is to develop improved solutions to control thi...The zebra mussel is an important aquatic pest that causes great damage to freshwater-dependent industries, due to biofouling. The main goal of the project discussed here is to develop improved solutions to control this species. Three approaches have been explored in an attempt to design innovative application strategies for existing biocides： （i） encapsulation of toxins; （ii） combination of toxins; （iii） investigation of the seasonal variation of the species＇ tolerance to toxins. In this paper, the principles behind these approaches and the major results on each topic are presented. The benefits of adopting a chemical product engineering approach in conducting this project are also discussed.展开更多
Rare-earth elements （REEs） are essential metals for the design and development of sustainable energy applications, Recycling these elements from waste streams enriched in them is crucial for securing an independent ...Rare-earth elements （REEs） are essential metals for the design and development of sustainable energy applications, Recycling these elements from waste streams enriched in them is crucial for securing an independent future supply for sustainable applications, This study compares the mechanisms of mechan- ical activation prior to a hydrometallurgical acid-leaching process and a solvometallurgical mechanochemical leaching process for the recovery of REEs from green lamp phosphor, LaPO4：Ce3＋, Th3＋, After 60 min of processing time, the REE leaching rates showed a significant enhancement of 60% after cycled mechanical activation, and 98% after the combined mechanochemical leaching process, High-resolution transmission electron microscopy （HR-TEM） imaging disclosed the cause for the improved REE leaching rates： The improved leaching and leaching patterns could he attributed to changes in the crystal morphology from monocrystalline to polycrystalline, Reduction of the crystallite size to the nanoscale in a polycrystalline material creates irregular packing of chemical units, resulting in an increase in defect-rich grain boundaries in the crystals, which enhances the leaching process, A solvometallurgical method was developed to combine the mechanical activation and leaching process into a single step, which is beneficial for operational cost, This results in an efficient and simple process that provides an alternative and greener recycling route for lamp phosphor waste,展开更多
With the development of manufacturing technology on the nanoscale, the precision of nano-devices is rapidly increasing with lower cost. Different from macroscale or microscale fluids, many specific phenomena and advan...With the development of manufacturing technology on the nanoscale, the precision of nano-devices is rapidly increasing with lower cost. Different from macroscale or microscale fluids, many specific phenomena and advantages are observed in nanofluidics. Devices and process involving and utilizing these phenomena play an important role in many fields in chemical engineering including separation, chemical analysis and transmission.In this article, we summarize the state-of-the-art progress in theoretical studies and manufacturing technologies on nanofluidics. Then we discuss practical applications of nanofluidics in many chemical engineering fields,especially in separation and encountering problems. Finally, we are looking forward to the future of nanofluidics and believe it will be more important in the separation process and the modern chemical industry.展开更多
Electrochemical methods are environmentally friendly and have unique advantages in the synthesis of organic chemicals.However,their implementation is limited due to the complex transport problems posed by traditional ...Electrochemical methods are environmentally friendly and have unique advantages in the synthesis of organic chemicals.However,their implementation is limited due to the complex transport problems posed by traditional electrochemical reactors.Recently,the application of microreaction technology in electrosynthesis studies has reduced the transport distance of ions and increased the specific surface area of electrodes,leading to efficient,successive,and easily scaled-up electrosynthesis technologies.In this review article,engineering advantages of using microchannels in electrosynthesis are discussed from process enhancement perspective.Flow patterns and mass transfer behaviors in recently reported electrochemical microreactors are analyzed,and prototypes for the reactor scale-up are reviewed.As a relatively new research area,many scientific rules and engineering features of electrosynthesis in microreactors require elucidation.Potential research foci,considered crucial for the development of novel electrosynthesis technology,are therefore proposed.展开更多
Electrochemical N_(2) reduction reaction(eNRR) over Cu-based catalysts suffers from an intrinsically low activity of Cu for activation of stable N_(2) molecules and the limited supply of N_(2) to the catalyst due to i...Electrochemical N_(2) reduction reaction(eNRR) over Cu-based catalysts suffers from an intrinsically low activity of Cu for activation of stable N_(2) molecules and the limited supply of N_(2) to the catalyst due to its low solubility in aqueous electrolytes.Herein,we propose phosphorus-activated Cu electrocatalysts to generate electron-deficient Cu sites on the catalyst surface to promote the adsorption of N_(2) molecules.The eNRR system is further modified using a gas diffusion electrode(GDE) coated with polytetrafluoroethylene(PTFE) to form an effective three-phase boundary of liquid water-gas N_(2)-solid catalyst to facilitate easy access of N_(2) to the catalytic sites.As a result,the new catalyst in the flow-type cell records a Faradaic efficiency of 13.15% and an NH_(3) production rate of 7.69 μg h^(-1) cm^(-2) at-0.2 V_(RHE),which represent 3.56 and 59.2 times increases from those obtained with a pristine Cu electrode in a typical electrolytic cell.This work represents a successful demonstration of dual modification strategies;catalyst modification and N_(2) supplying system engineering,and the results would provide a useful platform for further developments of electrocatalysts and reaction systems.展开更多
Increasing importance of heat transfer in chemical engineering science causes that investigation in the field of enhancement techniques is always one of the up-to-date topics for study.In the current comparative analy...Increasing importance of heat transfer in chemical engineering science causes that investigation in the field of enhancement techniques is always one of the up-to-date topics for study.In the current comparative analysis,the thermal enhancement and friction penalty are explored numerically for curved tubes via twisted configuration.To accomplish this,three common geometries namely helical,serpentine,and Archimedes spiral,are considered at different coil-pitches and twist-pitches as well as five Reynolds numbers in the laminar flow regime.The results exhibit noticeable enhancements(up to 60%)in the thermal performance of the twisted cases as compared to the smooth cases.The highest increases are recorded for the serpentine case,followed by the helical and spiral cases.It is found that these enhancements vary via coil-pitch and twist-pitch.Increasing coil-pitch and twist-pitch augments both heat transfer coefficient and pressure drop in all curved-twisted tubes,however,the effects of twist-pitch are more pronounced.To predict Nusselt number and friction factor,new correlations are also proposed.The maximum deviations of the predicted results compared to the simulated data are within±5%.展开更多
Magnesium(Mg)-based bioresorbable stents represent a potentially groundbreaking advancement in cardiovascular therapy;offering tem-porary vessel support and complete biodegradability—addressing limitations of traditi...Magnesium(Mg)-based bioresorbable stents represent a potentially groundbreaking advancement in cardiovascular therapy;offering tem-porary vessel support and complete biodegradability—addressing limitations of traditional stents like in-stent restenosis and long-term com-plications.However,challenges such as rapid corrosion and suboptimal endothelialisation have hindered their clinical adoption.This review highlights the latest breakthroughs in surface modification,alloying,and coating strategies to enhance the mechanical integrity,corrosion resistance,and biocompatibility of Mg-based stents.Key surface engineering techniques,including polymer and bioactive coatings,are ex-amined for their role in promoting endothelial healing and minimising inflammatory responses.Future directions are proposed,focusing on personalised stent designs to optimize efficacy and long-term outcomes,positioning Mg-based stents as a transformative solution in interventional cardiology.展开更多
All-solid-state lithium batteries(ASSLBs)are strongly considered as the next-generation energy storage devices for their high energy density and intrinsic safety.The solid-solid contact between lithium metal and solid...All-solid-state lithium batteries(ASSLBs)are strongly considered as the next-generation energy storage devices for their high energy density and intrinsic safety.The solid-solid contact between lithium metal and solid electrolyte plays a vital role in the performance of working ASSLBs,which is challenging to investigate quantitatively by experimental approach.This work proposed a quantitative model based on the finite element method for electrochemical impedance spectroscopy simulation of different solid-solid contact states in ASSLBs.With the assistance of an equivalent circuit model and distribution of relaxation times,it is discovered that as the number of voids and the sharpness of cracks increase,the contact resistance Rcgrows and ultimately dominates the battery impedance.Through accurate fitting,inverse proportional relations between contact resistance Rcand(1-porosity)as well as crack angle was disclosed.This contribution affords a fresh insight into clarifying solid-solid contact states in ASSLBs.展开更多
Biomass-derived heteroatom self-doped cathode catalysts has attracted considerable interest for electrochemical advanced oxidation processes(EAOPs)due to its high performance and sustainable synthesis.Herein,we illust...Biomass-derived heteroatom self-doped cathode catalysts has attracted considerable interest for electrochemical advanced oxidation processes(EAOPs)due to its high performance and sustainable synthesis.Herein,we illustrated the morphological fates of waste leaf-derived graphitic carbon(WLGC)produced from waste ginkgo leaves via pyrolysis temperature regulation and used as bifunctional cathode catalyst for simultaneous H_(2)O_(2) electrochemical generation and organic pollutant degradation,discovering S/N-self-doping shown to facilitate a synergistic effect on reactive oxygen species(ROS)generation.Under the optimum temperature of 800℃,the WLGC exhibited a H_(2)O_(2) selectivity of 94.2%and tetracycline removal of 99.3%within 60 min.Density functional theory calculations and in-situ Fourier transformed infrared spectroscopy verified that graphitic N was the critical site for H_(2)O_(2) generation.While pyridinic N and thiophene S were the main active sites responsible for OH generation,N vacancies were the active sites to produce ^(1)O_(2) from O_(2).The performance of the novel cathode for tetracycline degradation remains well under a wide pH range(3–11),maintaining excellent stability in 10 cycles.It is also industrially applicable,achieving satisfactory performance treating in real water matrices.This system facilitates both radical and non-radical degradation,offering valuable advances in the preparation of cost-effective and sustainable electrocatalysts and hold strong potentials in metal-free EAOPs for organic pollutant degradation.展开更多
Electrocatalysis has emerged as a sustainable approach for the selective oxidation of fatty alcohols to fatty acids,circumventing the environmental concerns associated with conventional routes.However,the low aqueous ...Electrocatalysis has emerged as a sustainable approach for the selective oxidation of fatty alcohols to fatty acids,circumventing the environmental concerns associated with conventional routes.However,the low aqueous solubility of hydrophobic fatty alcohols presents a major challenge.While nickel hydroxide(Ni(OH)_(2))serves as a cost-effective catalyst for alcohol oxidation,its hydrophilic nature limits substrate accessibility and mass transport,causing sluggish kinetics and competing oxygen evolution.Herein,we propose a hydrophobic interface engineering strategy via co-electrodeposition of Ni(OH)_(2)with polytetrafluoroethylene(PTFE),fabricating the composite electrode(ED-Ni(OH)_(2)-PTFE).The optimized electrode achieves 95%Faradaic efficiency for octanoic acid at 1.5 V vs.RHE,with a production rate 2–3 times higher than pristine Ni(OH)_(2).Mechanistic studies combining in situ Raman spectroscopy,fluorescence imaging,and coarse-grained molecular dynamics simulations reveal that PTFE selectively enriches octanol at the electrode-electrolyte interface by modulating interfacial hydrophobicity.A continuous-flow microreactor integrating anodic octanol oxidation with cathodic hydrogen evolution reduces cell voltage by~100 m V,achieving simultaneous fatty acid and hydrogen production.This work highlights the critical role of hydrophobic interfacial microenvironment design in organic electrosynthesis,offering a promising strategy for upgrading fatty alcohols under mild conditions.展开更多
Cardiac tissue engineering aims to efficiently replace or repair injured heart tissue using scaffolds,relevant cells,or their combination.While the combination of scaffolds and relevant cells holds the potential to ra...Cardiac tissue engineering aims to efficiently replace or repair injured heart tissue using scaffolds,relevant cells,or their combination.While the combination of scaffolds and relevant cells holds the potential to rapidly remuscularize the heart,thereby avoiding the slow process of cell recruitment,the proper ex vivo cellularization of a scaffold poses a substantial challenge.First,proper diffusion of nutrients and oxygen should be provided to the cell-seeded scaffold.Second,to generate a functional tissue construct,cells can benefit from physiological-like conditions.To meet these challenges,we developed a modular bioreactor for the dynamic cellularization of full-thickness cardiac scaffolds under synchronized mechanical and electrical stimuli.In this unique bioreactor system,we designed a cyclic mechanical load that mimics the left ventricle volume inflation,thus achieving a steady stimulus,as well as an electrical stimulus with an action potential profile to mirror the cells’microenvironment and electrical stimuli in the heart.These mechanical and electrical stimuli were synchronized according to cardiac physiology and regulated by constant feedback.When applied to a seeded thick porcine cardiac extracellular matrix(pcECM)scaffold,these stimuli improved the proliferation of mesenchymal stem/stromal cells(MSCs)and induced the formation of a dense tissue-like structure near the scaffold’s surface.Most importantly,after 35 d of cultivation,the MSCs presented the early cardiac progenitor markers Connexin-43 andα-actinin,which were absent in the control cells.Overall,this research developed a new bioreactor system for cellularizing cardiac scaffolds under cardiac-like conditions,aiming to restore a sustainable dynamic living tissue that can bear the essential cardiac excitation–contraction coupling.展开更多
Lignocellulosic biomass is one of the viable solutions to alleviate the global warming. However, the limited utilization of biomass majorly focused on cellulose and hemicellulose restricts the economic and environment...Lignocellulosic biomass is one of the viable solutions to alleviate the global warming. However, the limited utilization of biomass majorly focused on cellulose and hemicellulose restricts the economic and environmental feasibilities. To cope with this issue, we proposed an integrated process of co-producing 1,6-hexanediol(1,6-HDO) with tetrahydrofuran and adipic acid from biomass, referred to as Strategy A. To compare the impacts of lignin upgrading and feedstock, Strategy B, which co-produces tetrahydrofuran alone, and Strategy C, which is the traditional route to produce 1,6-HDO from fossil fuels, were used. Heat networks are also designed to reduce operating costs and indirect carbon emissions due to energy consumption, saving 87% and 83% of the heat and cooling requirements, respectively, in Strategy A. The market competitiveness of Strategy A was evaluated by determining the minimum selling price through techno-economic analysis, and sustainability was thoroughly investigated by quantifying the environmental impacts through both midpoint and endpoint life-cycle assessments(LCAs).Strategy A was found to be the most favorable both economically(USRDSCHARDOLLAR3,402/ton) and environmentally(-26.9 kg CO_(2)eq.). This indicates that lignin valorization is not only economically but also environmentally preferred. Finally, changes in economic and environmental feasibilities depending on economic, process, and environmental parameters were investigated using sensitivity and uncertainty analyses. The results of these analyses provide valuable insight into bio-based chemical production.展开更多
In pursuit of meeting the demands for the next generation of high energy density and flexible electronic products,there is a growing interest in flexible energy storage devices.Silicon(Si)stands out as a promising ele...In pursuit of meeting the demands for the next generation of high energy density and flexible electronic products,there is a growing interest in flexible energy storage devices.Silicon(Si)stands out as a promising electrode material due to its high theoretical specific capacity(~3579 mA h g^(-1)),low lithiation potential(~0.40 V),and abundance in nature.We have successfully developed freestanding and flexible CNT/Si/low-melting-point metal(LM)electrodes,which obviate the need for conductive additives,adhesives,and thereby increase the energy density of the device.As an anode material for lithium-ion batteries(LIBs),the CNT/Si/LM electrode demonstrates remarkable cycling stability and rate performance,achieving a reversible capacity of 1871.8 mA h g^(-1)after 100 cycles at a current density of 0.2 A g^(-1).In-situ XRD and in-situ thickness analysis are employed to elucidate the underlying mechanisms during the lithiation/delithiation.Density functional theory(DFT)calculations further substantiate the mechanism by which LM enhances the electrochemical performance of Si,focusing on the aspects of stress mitigation and reduction of the diffusion energy barrier.This research introduces a novel approach to flexible electrode design by integrating CNT films,LM,and Si,thereby charting a path forward for the development of next-generation flexible LIBs.展开更多
基金supported by the National Natural Science Foundation of China(22378227)Shijiazhuang Science and Technology Bureau(231790163A).
文摘Chemical synthesis is essential in industries such as petrochemicals, fine chemicals, and pharmaceuticals, driving economic and social development. The increasing demand for new molecules and materials calls for novel chemical reactions;however, manual experimental screening is time-consuming. Artificial intelligence (AI) offers a promising solution by leveraging large-scale experimental data to model chemical reactions, although challenges such as the lack of standardization and predictability in chemical synthesis hinder AI applications. Additionally, the multi-scale nature of chemical reactions, along with complex multiphase processes, further complicates the task. Recent advances in microchemical systems, particularly continuous flow methods using microreactors, provide precise control over reaction conditions, enhancing reproducibility and enabling high-throughput experimentation. These systems minimize transport-related inconsistencies and facilitate scalable industrial applications. This review systematically explores recent developments in intelligent synthesis based on microchemical systems, focusing on reaction system design, synthesis robots, closed-loop optimization, and high-throughput experimentation, while identifying key areas for future research.
基金the National Key Research and Development Program(2016YFA0202500 and 2016YFA0200102)the National Natural Science Foundation of China(21676160,21776019,and 21825501)the Tsinghua University Initiative Scientific Research Program.
文摘Rechargeable lithium-ion batteries(LIBs)afford a profound impact on our modern daily life.However,LIBs are approaching the theoretical energy density,due to the inherent limitations of intercalation chemistry;thus,they cannot further satisfy the increasing demands of portable electronics,electric vehicles,and grids.Therefore,battery chemistries beyond LIBs are being widely investigated.Next-generation lithium(Li)batteries,which employ Li metal as the anode and intercalation or conversion materials as the cathode,receive the most intensive interest due to their high energy density and excellent potential for commercialization.Moreover,significant progress has been achieved in Li batteries attributed to the increasing fundamental understanding of the materials and reactions,as well as to technological improvement.This review starts by summarizing the electrolytes for next-generation Li batteries.Key challenges and recent progress in lithium-ion,lithium–sulfur,and lithium–oxygen batteries are then reviewed from the perspective of energy and chemical engineering science.Finally,possible directions for further development in Li batteries are presented.Next-generation Li batteries are expected to promote the sustainable development of human civilization.
文摘This paper discussed an extended model for flexibility analysis of chemical process. Under uncertainty, probability density function is used to describe uncertain parameters instead of hyper-rectangle, and chanceconstrained programming is a feasible way to deal with the violation of constraints. Because the feasible region of control variables would change along with uncertain parameters, its smallest acceptable size threshold is presented to ensure the controllability condition. By synthesizing the considerations mentioned above, a modified model can describe the flexibility analysis problem more exactly. Then a hybrid algorithm, which integrates stochastic simulation and genetic algorithm, is applied to solve this model and maximize the flexibility region. Both numerical and chemical process examples are presented to demonstrate the effectiveness of the method.
文摘In the preliminary stage of chemical process design, the choice of chemical reaction route is the key design decision, and the concepts of atom utilization and environmental quotient have become extremely useful tools. However, the waste quality such as chemical toxicity and other engineering factors have not been taken into account. Therefore, a synthetic route selection index, Iroute, is proposed to determine the suitability of a chemical route in this paper. Iroute considers the effects of 'extended atom economy', material renewability, chemical characteristics and some engineering factors. The extended atom economy concept regards not only the value of the desired product but also the value of byproducts. The methodology by using Iroute to compare different routes is illustrated in case study of cyclohexanone oxime and acrylonitrile manufacture.
基金the supports of the National Science Foundation of China (22008130, 22025801)the China Postdoctoral Science Foundation (2020M682124)+1 种基金the Qingdao Postdoctoral Researchers Applied Research Project Foundation (RZ2000001426)the Scientific Research Foundation for Youth Scholars from Qingdao University (DC1900014265) for this work
文摘The concept of“carbon neutrality”poses a huge challenge for chemical engineering and brings great opportunities for boosting the development of novel technologies to realize carbon offsetting and reduce carbon emissions.Developing high-efficient,low-cost,energy-efficient and eco-friendly microfluidicbased microchemical engineering is of great significance.Such kind of“green microfluidics”can reduce carbon emissions from the source of raw materials and facilitate controllable and intensified microchemical engineering processes,which represents the new power for the transformation and upgrading of chemical engineering industry.Here,a brief review of green microfluidics for achieving carbon neutral microchemical engineering is presented,with specific discussions about the characteristics and feasibility of applying green microfluidics in realizing carbon neutrality.Development of green microfluidic systems are categorized and reviewed,including the construction of microfluidic devices by bio-based substrate materials and by low carbon fabrication methods,and the use of more biocompatible and nondestructive fluidic systems such as aqueous two-phase systems(ATPSs).Moreover,low carbon applications benefit from green microfluidics are summarized,ranging from separation and purification of biomolecules,high-throughput screening of chemicals and drugs,rapid and cost-effective detections,to synthesis of fine chemicals and novel materials.Finally,challenges and perspectives for further advancing green microfluidics in microchemical engineering for carbon neutrality are proposed and discussed.
基金Supported by the National Basic Research Program of China(2014CB239703)the National Natural Science Foundation of China(21336003)the Science and Technology Commission of Shanghai Municipality(14DZ2250800)
文摘This review focuses on the application of process engineering in electrochemical energy conversion and storage devices innovation. For polymer electrolyte based devices, it highlights that a strategic simple switch from proton exchange membranes(PEMs) to hydroxide exchange membranes(HEMs) may lead to a new-generation of affordable electrochemical energy devices including fuel cells, electrolyzers, and solar hydrogen generators. For lithium-ion batteries, a series of advancements in design and chemistry are required for electric vehicle and energy storage applications. Manufacturing process development and optimization of the LiF eP O_4/C cathode materials and several emerging novel anode materials are also discussed using the authors' work as examples.Design and manufacturing process of lithium-ion battery electrodes are introduced in detail, and modeling and optimization of large-scale lithium-ion batteries are also presented. Electrochemical energy materials and device innovations can be further prompted by better understanding of the fundamental transport phenomena involved in unit operations.
基金the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(grant nos.2021R1C1C1007844,2021M3I3A1085039,2020R1F1A1061505,and 2020R1C1C1012014).
文摘Heavy-metal-free ternary Cu–In–Se quantum dots(CISe QDs)are promising for solar fuel production because of their low toxicity,tunable band gap,and high light absorption coefficient.Although defects significantly affect the photophysical properties of QDs,the influence on photoelectrochemical hydrogen production is not well understood.Herein,we present the defect engineering of CISe QDs for efficient solar-energy conversion.Lewis acid–base reactions between metal halide–oleylamine complexes and oleylammonium selenocarbamate are modulated to achieve CISe QDs with the controlled amount of Cu vacancies without changing their morphology.Among them,CISe QDs with In/Cu=1.55 show the most outstanding photoelectrochemical hydrogen generation with excellent photocurrent density of up to 10.7 mA cm-2(at 0.6 VRHE),attributed to the suitable electronic band structures and enhanced carrier concentrations/lifetimes of the QDs.The proposed method,which can effectively control the defects in heavy-metal-free ternary QDs,offers a deeper understanding of the effects of the defects and provides a practical approach to enhance photoelectrochemical hydrogen generation.
基金the Portuguese Foundation for Science and Technology (scholarship SFRH/BD/18731/2004 and Research Project Grant POCI/EQU/59305/2004).
文摘The zebra mussel is an important aquatic pest that causes great damage to freshwater-dependent industries, due to biofouling. The main goal of the project discussed here is to develop improved solutions to control this species. Three approaches have been explored in an attempt to design innovative application strategies for existing biocides： （i） encapsulation of toxins; （ii） combination of toxins; （iii） investigation of the seasonal variation of the species＇ tolerance to toxins. In this paper, the principles behind these approaches and the major results on each topic are presented. The benefits of adopting a chemical product engineering approach in conducting this project are also discussed.
基金supported by KU Leuven (GOA/13/008 and IOFKP RARE3)FWO-Flanders for a SB PhD fellowship (1S23518N)the European Research Council (ERC) under the European Union’s Horizon 2020 Research and Innovation Programme: Grant Agreement 694078-Solvometallurgy for critical metals (SOLCRIMET)
文摘Rare-earth elements （REEs） are essential metals for the design and development of sustainable energy applications, Recycling these elements from waste streams enriched in them is crucial for securing an independent future supply for sustainable applications, This study compares the mechanisms of mechan- ical activation prior to a hydrometallurgical acid-leaching process and a solvometallurgical mechanochemical leaching process for the recovery of REEs from green lamp phosphor, LaPO4：Ce3＋, Th3＋, After 60 min of processing time, the REE leaching rates showed a significant enhancement of 60% after cycled mechanical activation, and 98% after the combined mechanochemical leaching process, High-resolution transmission electron microscopy （HR-TEM） imaging disclosed the cause for the improved REE leaching rates： The improved leaching and leaching patterns could he attributed to changes in the crystal morphology from monocrystalline to polycrystalline, Reduction of the crystallite size to the nanoscale in a polycrystalline material creates irregular packing of chemical units, resulting in an increase in defect-rich grain boundaries in the crystals, which enhances the leaching process, A solvometallurgical method was developed to combine the mechanical activation and leaching process into a single step, which is beneficial for operational cost, This results in an efficient and simple process that provides an alternative and greener recycling route for lamp phosphor waste,
基金Supported by the National Natural Science Foundation of China(No.21476125)Tsinghua University Foundation,(No.2013108930)performed at the “Exploration 100” platform supported by Tsinghua National Laboratory for Information Science and Technology
文摘With the development of manufacturing technology on the nanoscale, the precision of nano-devices is rapidly increasing with lower cost. Different from macroscale or microscale fluids, many specific phenomena and advantages are observed in nanofluidics. Devices and process involving and utilizing these phenomena play an important role in many fields in chemical engineering including separation, chemical analysis and transmission.In this article, we summarize the state-of-the-art progress in theoretical studies and manufacturing technologies on nanofluidics. Then we discuss practical applications of nanofluidics in many chemical engineering fields,especially in separation and encountering problems. Finally, we are looking forward to the future of nanofluidics and believe it will be more important in the separation process and the modern chemical industry.
基金We would like to acknowledge the supports from the National Natural Science Foundation of China(21776150)and the State Key Laboratory of Chemical Engineering(SKL-ChE-20Z01).
文摘Electrochemical methods are environmentally friendly and have unique advantages in the synthesis of organic chemicals.However,their implementation is limited due to the complex transport problems posed by traditional electrochemical reactors.Recently,the application of microreaction technology in electrosynthesis studies has reduced the transport distance of ions and increased the specific surface area of electrodes,leading to efficient,successive,and easily scaled-up electrosynthesis technologies.In this review article,engineering advantages of using microchannels in electrosynthesis are discussed from process enhancement perspective.Flow patterns and mass transfer behaviors in recently reported electrochemical microreactors are analyzed,and prototypes for the reactor scale-up are reviewed.As a relatively new research area,many scientific rules and engineering features of electrosynthesis in microreactors require elucidation.Potential research foci,considered crucial for the development of novel electrosynthesis technology,are therefore proposed.
基金supported by the Climate Change Response Project (NRF-2019M1A2A2065612)the Brainlink Project (NRF2022H1D3A3A01081140)+3 种基金the NRF-2021R1A4A3027878 and the No. RS-2023-00212273 funded by the Ministry of Science and ICT of Korea via National Research Foundationresearch funds from Hanhwa Solutions Chemicals (1.220029.01)UNIST (1.190013.01)supported by the Institute for Basic Science (IBS-R019-D1)。
文摘Electrochemical N_(2) reduction reaction(eNRR) over Cu-based catalysts suffers from an intrinsically low activity of Cu for activation of stable N_(2) molecules and the limited supply of N_(2) to the catalyst due to its low solubility in aqueous electrolytes.Herein,we propose phosphorus-activated Cu electrocatalysts to generate electron-deficient Cu sites on the catalyst surface to promote the adsorption of N_(2) molecules.The eNRR system is further modified using a gas diffusion electrode(GDE) coated with polytetrafluoroethylene(PTFE) to form an effective three-phase boundary of liquid water-gas N_(2)-solid catalyst to facilitate easy access of N_(2) to the catalytic sites.As a result,the new catalyst in the flow-type cell records a Faradaic efficiency of 13.15% and an NH_(3) production rate of 7.69 μg h^(-1) cm^(-2) at-0.2 V_(RHE),which represent 3.56 and 59.2 times increases from those obtained with a pristine Cu electrode in a typical electrolytic cell.This work represents a successful demonstration of dual modification strategies;catalyst modification and N_(2) supplying system engineering,and the results would provide a useful platform for further developments of electrocatalysts and reaction systems.
文摘Increasing importance of heat transfer in chemical engineering science causes that investigation in the field of enhancement techniques is always one of the up-to-date topics for study.In the current comparative analysis,the thermal enhancement and friction penalty are explored numerically for curved tubes via twisted configuration.To accomplish this,three common geometries namely helical,serpentine,and Archimedes spiral,are considered at different coil-pitches and twist-pitches as well as five Reynolds numbers in the laminar flow regime.The results exhibit noticeable enhancements(up to 60%)in the thermal performance of the twisted cases as compared to the smooth cases.The highest increases are recorded for the serpentine case,followed by the helical and spiral cases.It is found that these enhancements vary via coil-pitch and twist-pitch.Increasing coil-pitch and twist-pitch augments both heat transfer coefficient and pressure drop in all curved-twisted tubes,however,the effects of twist-pitch are more pronounced.To predict Nusselt number and friction factor,new correlations are also proposed.The maximum deviations of the predicted results compared to the simulated data are within±5%.
文摘Magnesium(Mg)-based bioresorbable stents represent a potentially groundbreaking advancement in cardiovascular therapy;offering tem-porary vessel support and complete biodegradability—addressing limitations of traditional stents like in-stent restenosis and long-term com-plications.However,challenges such as rapid corrosion and suboptimal endothelialisation have hindered their clinical adoption.This review highlights the latest breakthroughs in surface modification,alloying,and coating strategies to enhance the mechanical integrity,corrosion resistance,and biocompatibility of Mg-based stents.Key surface engineering techniques,including polymer and bioactive coatings,are ex-amined for their role in promoting endothelial healing and minimising inflammatory responses.Future directions are proposed,focusing on personalised stent designs to optimize efficacy and long-term outcomes,positioning Mg-based stents as a transformative solution in interventional cardiology.
基金supported by the Beijing Natural Science Foundation(Z200011,L233004)the National Key Research and Development Program(2021YFB2500300)+3 种基金the National Natural Science Foundation of China(52394170,52394171,22109011,22393900,and 22108151)the Tsinghua-Jiangyin Innovation Special Fund(TJISF)(2022JYTH0101)the S&T Program of Hebei(22344402D)the Tsinghua University Initiative Scientific Research Program.
文摘All-solid-state lithium batteries(ASSLBs)are strongly considered as the next-generation energy storage devices for their high energy density and intrinsic safety.The solid-solid contact between lithium metal and solid electrolyte plays a vital role in the performance of working ASSLBs,which is challenging to investigate quantitatively by experimental approach.This work proposed a quantitative model based on the finite element method for electrochemical impedance spectroscopy simulation of different solid-solid contact states in ASSLBs.With the assistance of an equivalent circuit model and distribution of relaxation times,it is discovered that as the number of voids and the sharpness of cracks increase,the contact resistance Rcgrows and ultimately dominates the battery impedance.Through accurate fitting,inverse proportional relations between contact resistance Rcand(1-porosity)as well as crack angle was disclosed.This contribution affords a fresh insight into clarifying solid-solid contact states in ASSLBs.
基金financially supported by National Key R&D Program International Cooperation Project(2023YFE0108100)Natural Science Foundation of China(No.52170085)+2 种基金Key Project of Natural Science Foundation of Tianjin(No.21JCZDJC00320)Tianjin Post-graduate Students Research and Innovation Project(2021YJSB013)Fundamental Research Funds for the Central Universities,Nankai University.
文摘Biomass-derived heteroatom self-doped cathode catalysts has attracted considerable interest for electrochemical advanced oxidation processes(EAOPs)due to its high performance and sustainable synthesis.Herein,we illustrated the morphological fates of waste leaf-derived graphitic carbon(WLGC)produced from waste ginkgo leaves via pyrolysis temperature regulation and used as bifunctional cathode catalyst for simultaneous H_(2)O_(2) electrochemical generation and organic pollutant degradation,discovering S/N-self-doping shown to facilitate a synergistic effect on reactive oxygen species(ROS)generation.Under the optimum temperature of 800℃,the WLGC exhibited a H_(2)O_(2) selectivity of 94.2%and tetracycline removal of 99.3%within 60 min.Density functional theory calculations and in-situ Fourier transformed infrared spectroscopy verified that graphitic N was the critical site for H_(2)O_(2) generation.While pyridinic N and thiophene S were the main active sites responsible for OH generation,N vacancies were the active sites to produce ^(1)O_(2) from O_(2).The performance of the novel cathode for tetracycline degradation remains well under a wide pH range(3–11),maintaining excellent stability in 10 cycles.It is also industrially applicable,achieving satisfactory performance treating in real water matrices.This system facilitates both radical and non-radical degradation,offering valuable advances in the preparation of cost-effective and sustainable electrocatalysts and hold strong potentials in metal-free EAOPs for organic pollutant degradation.
基金Financial supports from the National Natural Science Foundation(No.21991104 and No.22,278,235)。
文摘Electrocatalysis has emerged as a sustainable approach for the selective oxidation of fatty alcohols to fatty acids,circumventing the environmental concerns associated with conventional routes.However,the low aqueous solubility of hydrophobic fatty alcohols presents a major challenge.While nickel hydroxide(Ni(OH)_(2))serves as a cost-effective catalyst for alcohol oxidation,its hydrophilic nature limits substrate accessibility and mass transport,causing sluggish kinetics and competing oxygen evolution.Herein,we propose a hydrophobic interface engineering strategy via co-electrodeposition of Ni(OH)_(2)with polytetrafluoroethylene(PTFE),fabricating the composite electrode(ED-Ni(OH)_(2)-PTFE).The optimized electrode achieves 95%Faradaic efficiency for octanoic acid at 1.5 V vs.RHE,with a production rate 2–3 times higher than pristine Ni(OH)_(2).Mechanistic studies combining in situ Raman spectroscopy,fluorescence imaging,and coarse-grained molecular dynamics simulations reveal that PTFE selectively enriches octanol at the electrode-electrolyte interface by modulating interfacial hydrophobicity.A continuous-flow microreactor integrating anodic octanol oxidation with cathodic hydrogen evolution reduces cell voltage by~100 m V,achieving simultaneous fatty acid and hydrogen production.This work highlights the critical role of hydrophobic interfacial microenvironment design in organic electrosynthesis,offering a promising strategy for upgrading fatty alcohols under mild conditions.
基金funded by the Israeli Ministry of Innovation,Science and Technology(Grant No.3-11873)the Israel Science Foundation(Grant No.1563/10)+1 种基金the Randy L.and Melvin R.Berlin Family Research Center for Regenerative Medicinethe Gurwin Family Foundation.
文摘Cardiac tissue engineering aims to efficiently replace or repair injured heart tissue using scaffolds,relevant cells,or their combination.While the combination of scaffolds and relevant cells holds the potential to rapidly remuscularize the heart,thereby avoiding the slow process of cell recruitment,the proper ex vivo cellularization of a scaffold poses a substantial challenge.First,proper diffusion of nutrients and oxygen should be provided to the cell-seeded scaffold.Second,to generate a functional tissue construct,cells can benefit from physiological-like conditions.To meet these challenges,we developed a modular bioreactor for the dynamic cellularization of full-thickness cardiac scaffolds under synchronized mechanical and electrical stimuli.In this unique bioreactor system,we designed a cyclic mechanical load that mimics the left ventricle volume inflation,thus achieving a steady stimulus,as well as an electrical stimulus with an action potential profile to mirror the cells’microenvironment and electrical stimuli in the heart.These mechanical and electrical stimuli were synchronized according to cardiac physiology and regulated by constant feedback.When applied to a seeded thick porcine cardiac extracellular matrix(pcECM)scaffold,these stimuli improved the proliferation of mesenchymal stem/stromal cells(MSCs)and induced the formation of a dense tissue-like structure near the scaffold’s surface.Most importantly,after 35 d of cultivation,the MSCs presented the early cardiac progenitor markers Connexin-43 andα-actinin,which were absent in the control cells.Overall,this research developed a new bioreactor system for cellularizing cardiac scaffolds under cardiac-like conditions,aiming to restore a sustainable dynamic living tissue that can bear the essential cardiac excitation–contraction coupling.
基金Material Parts Technology Development Program (20017461, Development and Performance Improvement of Air Operated Valve for 105 MPa Hydrogen Charging Station) funded by the Ministry of Trade,Industry and Energy(MOTIE, Republic of Korea)Korea Evaluation Institute of Industrial Technology (KEIT, Republic of Korea)+1 种基金financial support from the Korea Institute of Energy Technology Evaluation and Planning (KETEP)Ministry of Trade,Industry&Energy (MOTIE) of the Republic of Korea(RS-2024-00419764)。
文摘Lignocellulosic biomass is one of the viable solutions to alleviate the global warming. However, the limited utilization of biomass majorly focused on cellulose and hemicellulose restricts the economic and environmental feasibilities. To cope with this issue, we proposed an integrated process of co-producing 1,6-hexanediol(1,6-HDO) with tetrahydrofuran and adipic acid from biomass, referred to as Strategy A. To compare the impacts of lignin upgrading and feedstock, Strategy B, which co-produces tetrahydrofuran alone, and Strategy C, which is the traditional route to produce 1,6-HDO from fossil fuels, were used. Heat networks are also designed to reduce operating costs and indirect carbon emissions due to energy consumption, saving 87% and 83% of the heat and cooling requirements, respectively, in Strategy A. The market competitiveness of Strategy A was evaluated by determining the minimum selling price through techno-economic analysis, and sustainability was thoroughly investigated by quantifying the environmental impacts through both midpoint and endpoint life-cycle assessments(LCAs).Strategy A was found to be the most favorable both economically(USRDSCHARDOLLAR3,402/ton) and environmentally(-26.9 kg CO_(2)eq.). This indicates that lignin valorization is not only economically but also environmentally preferred. Finally, changes in economic and environmental feasibilities depending on economic, process, and environmental parameters were investigated using sensitivity and uncertainty analyses. The results of these analyses provide valuable insight into bio-based chemical production.
基金the National Natural Science Foundation of China(22279070).
文摘In pursuit of meeting the demands for the next generation of high energy density and flexible electronic products,there is a growing interest in flexible energy storage devices.Silicon(Si)stands out as a promising electrode material due to its high theoretical specific capacity(~3579 mA h g^(-1)),low lithiation potential(~0.40 V),and abundance in nature.We have successfully developed freestanding and flexible CNT/Si/low-melting-point metal(LM)electrodes,which obviate the need for conductive additives,adhesives,and thereby increase the energy density of the device.As an anode material for lithium-ion batteries(LIBs),the CNT/Si/LM electrode demonstrates remarkable cycling stability and rate performance,achieving a reversible capacity of 1871.8 mA h g^(-1)after 100 cycles at a current density of 0.2 A g^(-1).In-situ XRD and in-situ thickness analysis are employed to elucidate the underlying mechanisms during the lithiation/delithiation.Density functional theory(DFT)calculations further substantiate the mechanism by which LM enhances the electrochemical performance of Si,focusing on the aspects of stress mitigation and reduction of the diffusion energy barrier.This research introduces a novel approach to flexible electrode design by integrating CNT films,LM,and Si,thereby charting a path forward for the development of next-generation flexible LIBs.
