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
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
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
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
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
Hydrophilicity is critical in Nafion membranes during fuel cell operation as insufficient membrane hydration leads to brittle behavior and a drop in proton conductivity.The incorporation of APTS(3-(aminopro pyl)trieth...Hydrophilicity is critical in Nafion membranes during fuel cell operation as insufficient membrane hydration leads to brittle behavior and a drop in proton conductivity.The incorporation of APTS(3-(aminopro pyl)triethoxysilane)into exfoliated graphene oxide(EGO)by covalent functionalization to be used as filler into Nafion membranes allows higher hydrophilicity for these membranes.This is associated with promoting hydroxyl,carbonyl,siloxane,silane,and amine groups within the EGO-APTS matrix.The incorporation of these materials as Fuel Cell MEAs leads to a significant reduction of the ohmic resistance measured at high frequency resistance(HFR)in electrochemical impedance spectroscopy(EIS)experiments and achieves maximum power densities of 1.33 W cm^(-2)at 60℃ at 100%RH(APTS-EGO,0.2 wt%)and1.33 W cm^(-2)at 60℃ at 70%RH(APTS-EGO,0.3 wt%),which represents an improvement of 190%compared to the commercial Nafion 212 when utilizing low humidification conditions(70%).Moreover,the as-synthesized membrane utilizes lower Nafion ionomer mass,which,in conjunction with the excellent cell performance,has the potential to decrease the cost of the membrane from 87 to 80£/W as well as a reduction of fluorinated compounds within the membrane.展开更多
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
Single-atom catalysts(SACs),as the rising stars in the field of catalytic science,are leading catalytic technology into an un-precedented new era.However,the synthe-sis of high-performance SACs with well-de-fined acti...Single-atom catalysts(SACs),as the rising stars in the field of catalytic science,are leading catalytic technology into an un-precedented new era.However,the synthe-sis of high-performance SACs with well-de-fined active sites and high loadings under precise control has become a hotly debated topic in scientific research.Metal-organic frameworks(MOFs),with their exceptional properties such as ultrahigh specific surface areas,precisely controllable structural de-signs,and highly flexible functional cus-tomization capabilities,are regarded as one of the ideal matrices for supporting and sta-bilizing SACs.This review provides an in-sightful overview of the diverse preparation strategies for MOFs-derived SACs.It comprehen-sively analyzes the unique advantages and challenges of each method in achieving efficient synthesis of SACs,emphasizing the crucial role of optimized processes in unlocking the antici-pated performance of SACs.Furthermore,this review delves into a series of advanced charac-terization techniques,including aberration-corrected scanning transmission electron mi-croscopy(AC-STEM),electron energy loss spectroscopy(EELS),X-ray absorption spec-troscopy(XAS),and infrared absorption spectroscopy(IRAS),offering valuable insights into the atomic-scale fine structures and properties of SACs,significantly advancing the under-standing of SAC mechanisms.Moreover,this review focuses on exploring the potential appli-cations of MOFs-derived SACs in electrocatalysis frontier fields.This comprehensive exami-nation lays a solid theoretical foundation and provides a directional guidance for the rational design and controllable synthesis of high-performance MOFs-derived SACs.展开更多
Various novel conjugated polymers(CPs)have been developed for organic photodetectors(OPDs),but their application to practical image sensors such as X-ray,R/G/B,and fingerprint sensors is rare.In this article,we report...Various novel conjugated polymers(CPs)have been developed for organic photodetectors(OPDs),but their application to practical image sensors such as X-ray,R/G/B,and fingerprint sensors is rare.In this article,we report the entire process from the synthesis and molecular engineering of novel CPs to the development of OPDs and fingerprint image sensors.We synthesized six benzo[1,2-d:4,5-d’]bis(oxazole)(BBO)-based CPs by modifying the alkyl side chains of the CPs.Several relationships between the molecular structure and the OPD performance were revealed,and increasing the number of linear octyl side chains on the conjugated backbone was the best way to improve Jph and reduce Jd in the OPDs.The optimized CP demonstrated promising OPD performance with a responsivity(R)of 0.22 A/W,specific detectivity(D^(*))of 1.05×10^(13)Jones at a bias of-1 V,rising/falling response time of 2.9/6.9μs,and cut-off frequency(f_(-3dB))of 134 kHz under collimated 530 nm LED irradiation.Finally,a fingerprint image sensor was fabricated by stacking the POTB1-based OPD layer on the organic thin-film transistors(318 ppi).The image contrast caused by the valleys and ridges in the fingerprints was obtained as a digital signal.展开更多
The increasing demand for sustainable energy solutions necessitates innovative approaches to biomass utilization.This study introduces a comprehensive biorefinery model that valorizes poplar biomass into high-value pr...The increasing demand for sustainable energy solutions necessitates innovative approaches to biomass utilization.This study introduces a comprehensive biorefinery model that valorizes poplar biomass into high-value products,including ethanol,furfural,phenol,and biochar.These products not only serve as promising sources for biofuel and renewable chemicals but also contribute to pollution mitigation.The approach employs a biphasic pretreatment system utilizing p-toluenesulfonic acid,pentanol,and AlCl_(3) under optimized conditions(120℃ for 45 min),achieving remarkable efficiencies of 95.8%xylan removal,90.2%delignification,and 90.7%glucan recovery.The underlying mechanism,elucidated through density functional theory,demonstrates how the disruption of lignin-carbohydrate complexes via electrostatic and hydrogen-bonding interactions enhances product yields.The cellulose-rich substrate yielded 71.3 g/L ethanol,while solubilized xylan converted to 86.7%furfural without additional acid.Furthermore,lignin pyrolysis produced bio-oil containing over 45.2%phenolic compounds,while biochar demonstrated significant adsorptive capacity for perfluorooctanoic acid.Scaling this biorefinery model to process 140 million tons of poplar biomass annually reduces CO_(2)emissions by 75.3 million tons and provides socioeconomic savings of $17.3 billion,supporting sustainable industrial transformation.展开更多
Plant cell wall(CW)-like soft materials,referred to as artificial CWs,are composites of assembled polymers containing micro-/nanoparticles or fibers/fibrils that are designed to mimic the composition,structure,and mec...Plant cell wall(CW)-like soft materials,referred to as artificial CWs,are composites of assembled polymers containing micro-/nanoparticles or fibers/fibrils that are designed to mimic the composition,structure,and mechanics of plant CWs.CW-like materials have recently emerged to test hypotheses pertaining to the intricate structure–property relationships of native plant CWs or to fabricate functional materials.Here,research on plant CWs and CW-like materials is reviewed by distilling key studies on biomimetic composites primarily composed of plant polysaccharides,including cellulose,pectin,and hemicellulose,as well as organic polymers like lignin.Micro-and nanofabrication of plant CW-like composites,characterization techniques,and in silico studies are reviewed,with a brief overview of current and potential applications.Micro-/nanofabrication approaches include bacterial growth and impregnation,layer-by-layer assembly,film casting,3-dimensional templating microcapsules,and particle coating.Various characterization techniques are necessary for the comprehensive mechanical,chemical,morphological,and structural analyses of plant CWs and CW-like materials.CW-like materials demonstrate versatility in real-life applications,including biomass conversion,pulp and paper,food science,construction,catalysis,and reaction engineering.This review seeks to facilitate the rational design and thorough characterization of plant CW-mimetic materials,with the goal of advancing the development of innovative soft materials and elucidating the complex structure–property relationships inherent in native CWs.展开更多
Terpenoids,one of the most diverse and structurally varied natural products in nature,are widely distributed in plants,microbes,and other organisms.Their structural diversity confers significant importance in medicine...Terpenoids,one of the most diverse and structurally varied natural products in nature,are widely distributed in plants,microbes,and other organisms.Their structural diversity confers significant importance in medicine,food,flavorings,and energy.However,traditional methods of plant extraction and chemical synthesis have limitations in industrial applications.Consequently,microbial cell factories have emerged as an important platform for terpenoid production.Terpene synthases(TPSs)are crucial in determining the structural and functional diversity of terpenoids.This review discussed the origin and classificationof TPSs,outlines commonly used TPS mining methods,and summarizes advances in TPS engineering.In addition,it also explores the influenceof machine learning on enzyme mining,the existing challenges and the future opportunities alongside cutting-edge technologies.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
This study investigates the electrochemical behavior of molybdenum disulfide(MoS_(2))as an anode in Li-ion batteries,focusing on the extra capacity phenomenon.Employing advanced characterization methods such as in sit...This study investigates the electrochemical behavior of molybdenum disulfide(MoS_(2))as an anode in Li-ion batteries,focusing on the extra capacity phenomenon.Employing advanced characterization methods such as in situ and ex situ X-ray diffraction,Raman spectroscopy,X-ray photoelectron spectroscopy,and transmission electron microscopy,the research unravels the complex structural and chemical evolution of MoS_(2) throughout its cycling.A key discovery is the identification of a unique Li intercalation mechanism in MoS_(2),leading to the formation of reversible Li_(2)MoS_(2) phases that contribute to the extra capacity of the MoS_(2) electrode.Density function theory calculations suggest the potential for overlithiation in MoS_(2),predicting Li5MoS_(2) as the most energetically favorable phase within the lithiation–delithiation process.Additionally,the formation of a Li-rich phase on the surface of Li_(4)MoS_(2) is considered energetically advantageous.After the first discharge,the battery system engages in two main reactions.One involves operation as a Li-sulfur battery within the carbonate electrolyte,and the other is the reversible intercalation and deintercalation of Li in Li_(2)MoS_(2).The latter reaction contributes to the extra capacity of the battery.The incorporation of reduced graphene oxide as a conductive additive in MoS_(2) electrodes notably improves their rate capability and cycling stability.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
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
Lithium-oxygen(Li-O2)batteries are perceived as a promising breakthrough in sustainable electrochemical energy storage,utilizing ambient air as an energy source,eliminating the need for costly cathode materials,and of...Lithium-oxygen(Li-O2)batteries are perceived as a promising breakthrough in sustainable electrochemical energy storage,utilizing ambient air as an energy source,eliminating the need for costly cathode materials,and offering the highest theoretical energy density(~3.5 k Wh kg^(-1))among discussed candidates.Contributing to the poor cycle life of currently reported Li-O_(2)cells is singlet oxygen(1O_(2))formation,inducing parasitic reactions,degrading key components,and severely deteriorating cell performance.Here,we harness the chirality-induced spin selectivity effect of chiral cobalt oxide nanosheets(Co_(3)O_(4)NSs)as cathode materials to suppress 1O_(2)in Li-O_(2)batteries for the first time.Operando photoluminescence spectroscopy reveals a 3.7-fold and 3.23-fold reduction in 1O_(2)during discharge and charge,respectively,compared to conventional carbon paperbased cells,consistent with differential electrochemical mass spectrometry results,which indicate a near-theoretical charge-to-O_(2)ratio(2.04 e-/O_(2)).Density functional theory calculations demonstrate that chirality induces a peak shift near the Fermi level,enhancing Co 3d-O 2p hybridization,stabilizing reaction intermediates,and lowering activation barriers for Li_(2)O_(2)formation and decomposition.These findings establish a new strategy for improving the stability and energy efficiency of sustainable Li-O_(2)batteries,abridging the current gap to commercialization.展开更多
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.
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financially supported by the UK Research Council EPRSC EP/W03395X/1the Program grant SynHiSel EP/V047078/1the Hydrogen and Fuel Cells Hub(H_(2)FC SUPERGEN)EP/P024807/1。
文摘Hydrophilicity is critical in Nafion membranes during fuel cell operation as insufficient membrane hydration leads to brittle behavior and a drop in proton conductivity.The incorporation of APTS(3-(aminopro pyl)triethoxysilane)into exfoliated graphene oxide(EGO)by covalent functionalization to be used as filler into Nafion membranes allows higher hydrophilicity for these membranes.This is associated with promoting hydroxyl,carbonyl,siloxane,silane,and amine groups within the EGO-APTS matrix.The incorporation of these materials as Fuel Cell MEAs leads to a significant reduction of the ohmic resistance measured at high frequency resistance(HFR)in electrochemical impedance spectroscopy(EIS)experiments and achieves maximum power densities of 1.33 W cm^(-2)at 60℃ at 100%RH(APTS-EGO,0.2 wt%)and1.33 W cm^(-2)at 60℃ at 70%RH(APTS-EGO,0.3 wt%),which represents an improvement of 190%compared to the commercial Nafion 212 when utilizing low humidification conditions(70%).Moreover,the as-synthesized membrane utilizes lower Nafion ionomer mass,which,in conjunction with the excellent cell performance,has the potential to decrease the cost of the membrane from 87 to 80£/W as well as a reduction of fluorinated compounds within the membrane.
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supported by Henan Province Key Research and Development and Promotion of Science and Technology Project(No.25A150001)the National Natural Science Foundation of China(Nos.22409171,22125303,92361302,and 92061203).
文摘Single-atom catalysts(SACs),as the rising stars in the field of catalytic science,are leading catalytic technology into an un-precedented new era.However,the synthe-sis of high-performance SACs with well-de-fined active sites and high loadings under precise control has become a hotly debated topic in scientific research.Metal-organic frameworks(MOFs),with their exceptional properties such as ultrahigh specific surface areas,precisely controllable structural de-signs,and highly flexible functional cus-tomization capabilities,are regarded as one of the ideal matrices for supporting and sta-bilizing SACs.This review provides an in-sightful overview of the diverse preparation strategies for MOFs-derived SACs.It comprehen-sively analyzes the unique advantages and challenges of each method in achieving efficient synthesis of SACs,emphasizing the crucial role of optimized processes in unlocking the antici-pated performance of SACs.Furthermore,this review delves into a series of advanced charac-terization techniques,including aberration-corrected scanning transmission electron mi-croscopy(AC-STEM),electron energy loss spectroscopy(EELS),X-ray absorption spec-troscopy(XAS),and infrared absorption spectroscopy(IRAS),offering valuable insights into the atomic-scale fine structures and properties of SACs,significantly advancing the under-standing of SAC mechanisms.Moreover,this review focuses on exploring the potential appli-cations of MOFs-derived SACs in electrocatalysis frontier fields.This comprehensive exami-nation lays a solid theoretical foundation and provides a directional guidance for the rational design and controllable synthesis of high-performance MOFs-derived SACs.
基金funded by the National Research Foundation(NRF)of Korea(2020M3H4A3081816,RS-2023-00304936,and RS-2024-00398065).
文摘Various novel conjugated polymers(CPs)have been developed for organic photodetectors(OPDs),but their application to practical image sensors such as X-ray,R/G/B,and fingerprint sensors is rare.In this article,we report the entire process from the synthesis and molecular engineering of novel CPs to the development of OPDs and fingerprint image sensors.We synthesized six benzo[1,2-d:4,5-d’]bis(oxazole)(BBO)-based CPs by modifying the alkyl side chains of the CPs.Several relationships between the molecular structure and the OPD performance were revealed,and increasing the number of linear octyl side chains on the conjugated backbone was the best way to improve Jph and reduce Jd in the OPDs.The optimized CP demonstrated promising OPD performance with a responsivity(R)of 0.22 A/W,specific detectivity(D^(*))of 1.05×10^(13)Jones at a bias of-1 V,rising/falling response time of 2.9/6.9μs,and cut-off frequency(f_(-3dB))of 134 kHz under collimated 530 nm LED irradiation.Finally,a fingerprint image sensor was fabricated by stacking the POTB1-based OPD layer on the organic thin-film transistors(318 ppi).The image contrast caused by the valleys and ridges in the fingerprints was obtained as a digital signal.
基金funded by the National Natural Science Foundation of China(22278189,22478154)the Fundamental Research Funds for the Central Universities(Jiangnan University,JUSRP202501024)the Priority Academic Program Development of Jiangsu Higher Education Institutions,the 111 Project(No.111-2-06)。
文摘The increasing demand for sustainable energy solutions necessitates innovative approaches to biomass utilization.This study introduces a comprehensive biorefinery model that valorizes poplar biomass into high-value products,including ethanol,furfural,phenol,and biochar.These products not only serve as promising sources for biofuel and renewable chemicals but also contribute to pollution mitigation.The approach employs a biphasic pretreatment system utilizing p-toluenesulfonic acid,pentanol,and AlCl_(3) under optimized conditions(120℃ for 45 min),achieving remarkable efficiencies of 95.8%xylan removal,90.2%delignification,and 90.7%glucan recovery.The underlying mechanism,elucidated through density functional theory,demonstrates how the disruption of lignin-carbohydrate complexes via electrostatic and hydrogen-bonding interactions enhances product yields.The cellulose-rich substrate yielded 71.3 g/L ethanol,while solubilized xylan converted to 86.7%furfural without additional acid.Furthermore,lignin pyrolysis produced bio-oil containing over 45.2%phenolic compounds,while biochar demonstrated significant adsorptive capacity for perfluorooctanoic acid.Scaling this biorefinery model to process 140 million tons of poplar biomass annually reduces CO_(2)emissions by 75.3 million tons and provides socioeconomic savings of $17.3 billion,supporting sustainable industrial transformation.
基金supported as part of The Center for LignoCellulose Structure and Formation,an Energy Frontier Research Center funded by the U.S.Department of Energy,Office of Science,Basic Energy Sciences under Award#DE-SC0001090support from the Huck Institutes of the Life Sciences at Penn State University through the Patricia and Stephen Benkovic Research Initiativesupported by the Center for Engineering Mechano Biology(CEMB),an NSF Science and Technology Center,under grant agreement CMMI:15-48571。
文摘Plant cell wall(CW)-like soft materials,referred to as artificial CWs,are composites of assembled polymers containing micro-/nanoparticles or fibers/fibrils that are designed to mimic the composition,structure,and mechanics of plant CWs.CW-like materials have recently emerged to test hypotheses pertaining to the intricate structure–property relationships of native plant CWs or to fabricate functional materials.Here,research on plant CWs and CW-like materials is reviewed by distilling key studies on biomimetic composites primarily composed of plant polysaccharides,including cellulose,pectin,and hemicellulose,as well as organic polymers like lignin.Micro-and nanofabrication of plant CW-like composites,characterization techniques,and in silico studies are reviewed,with a brief overview of current and potential applications.Micro-/nanofabrication approaches include bacterial growth and impregnation,layer-by-layer assembly,film casting,3-dimensional templating microcapsules,and particle coating.Various characterization techniques are necessary for the comprehensive mechanical,chemical,morphological,and structural analyses of plant CWs and CW-like materials.CW-like materials demonstrate versatility in real-life applications,including biomass conversion,pulp and paper,food science,construction,catalysis,and reaction engineering.This review seeks to facilitate the rational design and thorough characterization of plant CW-mimetic materials,with the goal of advancing the development of innovative soft materials and elucidating the complex structure–property relationships inherent in native CWs.
基金supported by the National Key Research and Development Program of China(2020YFA0908300)the Natural Science Foundation of China(22138006,22278240).
文摘Terpenoids,one of the most diverse and structurally varied natural products in nature,are widely distributed in plants,microbes,and other organisms.Their structural diversity confers significant importance in medicine,food,flavorings,and energy.However,traditional methods of plant extraction and chemical synthesis have limitations in industrial applications.Consequently,microbial cell factories have emerged as an important platform for terpenoid production.Terpene synthases(TPSs)are crucial in determining the structural and functional diversity of terpenoids.This review discussed the origin and classificationof TPSs,outlines commonly used TPS mining methods,and summarizes advances in TPS engineering.In addition,it also explores the influenceof machine learning on enzyme mining,the existing challenges and the future opportunities alongside cutting-edge technologies.
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the financial support from the Science, Technology, and Innovation Funding Authority (STIFA, STDF previously) through project number 42691 entitled “Microstructure-Based, Multi-Physics Simulation and Optimization to Improve Battery Performance”supported by the U.S. DOE (Department of Energy), Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357supported by the U.S. DOE Vehicle Technologies office, under contract number DE-AC02-06CH11357
文摘This study investigates the electrochemical behavior of molybdenum disulfide(MoS_(2))as an anode in Li-ion batteries,focusing on the extra capacity phenomenon.Employing advanced characterization methods such as in situ and ex situ X-ray diffraction,Raman spectroscopy,X-ray photoelectron spectroscopy,and transmission electron microscopy,the research unravels the complex structural and chemical evolution of MoS_(2) throughout its cycling.A key discovery is the identification of a unique Li intercalation mechanism in MoS_(2),leading to the formation of reversible Li_(2)MoS_(2) phases that contribute to the extra capacity of the MoS_(2) electrode.Density function theory calculations suggest the potential for overlithiation in MoS_(2),predicting Li5MoS_(2) as the most energetically favorable phase within the lithiation–delithiation process.Additionally,the formation of a Li-rich phase on the surface of Li_(4)MoS_(2) is considered energetically advantageous.After the first discharge,the battery system engages in two main reactions.One involves operation as a Li-sulfur battery within the carbonate electrolyte,and the other is the reversible intercalation and deintercalation of Li in Li_(2)MoS_(2).The latter reaction contributes to the extra capacity of the battery.The incorporation of reduced graphene oxide as a conductive additive in MoS_(2) electrodes notably improves their rate capability and cycling stability.
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.
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%.
基金supported by Basic Science Research Program(Priority Research Institute)through the NRF of Korea funded by the Ministry of Education(2021R1A6A1A10039823)by the Korea Basic Science Institute(National Research Facilities and Equipment Center)grant funded by the Ministry of Education(2020R1A6C101B194)。
文摘Lithium-oxygen(Li-O2)batteries are perceived as a promising breakthrough in sustainable electrochemical energy storage,utilizing ambient air as an energy source,eliminating the need for costly cathode materials,and offering the highest theoretical energy density(~3.5 k Wh kg^(-1))among discussed candidates.Contributing to the poor cycle life of currently reported Li-O_(2)cells is singlet oxygen(1O_(2))formation,inducing parasitic reactions,degrading key components,and severely deteriorating cell performance.Here,we harness the chirality-induced spin selectivity effect of chiral cobalt oxide nanosheets(Co_(3)O_(4)NSs)as cathode materials to suppress 1O_(2)in Li-O_(2)batteries for the first time.Operando photoluminescence spectroscopy reveals a 3.7-fold and 3.23-fold reduction in 1O_(2)during discharge and charge,respectively,compared to conventional carbon paperbased cells,consistent with differential electrochemical mass spectrometry results,which indicate a near-theoretical charge-to-O_(2)ratio(2.04 e-/O_(2)).Density functional theory calculations demonstrate that chirality induces a peak shift near the Fermi level,enhancing Co 3d-O 2p hybridization,stabilizing reaction intermediates,and lowering activation barriers for Li_(2)O_(2)formation and decomposition.These findings establish a new strategy for improving the stability and energy efficiency of sustainable Li-O_(2)batteries,abridging the current gap to commercialization.