Titanium exhibits outstanding properties,particularly,high specific strength and resistance to both high and low temperatures,earning it a reputation as the metal of the future.However,because of the highly reactive n...Titanium exhibits outstanding properties,particularly,high specific strength and resistance to both high and low temperatures,earning it a reputation as the metal of the future.However,because of the highly reactive nature of titanium,metallic titanium production involves extensive procedures and high costs.Considering its advantages and limitations,the European Union has classified titanium metal as a critical raw material(CRM)of low category.The Kroll process is predominantly used to produce titanium;however,molten salt electrolysis(MSE)is currently being explored for producing metallic titanium at a low cost.Since 2000,electrolytic titanium production has undergone a wave of technological advancements.However,because of the intermediate and disproportionation reactions in the electrolytic titanium production process,the process efficiency and titanium purity according to industrial standards could not be achieved.Consequently,metallic titanium production has gradually diversified into employing technologies such as thermal reduction,MSE,and titanium alloy preparation.This study provides a comprehensive review of research advances in titanium metal preparation technologies over the past two decades,highlighting the challenges faced by the existing methods and proposing potential solutions.It offers useful insights into the development of low-cost titanium preparation technologies.展开更多
Methane, an abundant one-carbon(C_(1)) resource, is extensively used in the industrial production of vital fuels and value-added chemicals. However, current industrial methane conversion technologies are energy-and ca...Methane, an abundant one-carbon(C_(1)) resource, is extensively used in the industrial production of vital fuels and value-added chemicals. However, current industrial methane conversion technologies are energy-and carbon-intensive, mainly due to the high activation energy required to break the inert C–H bond, low selectivity, and problematic side reactions, including CO_(2)emissions and coke deposition. Electrochemical conversion of methane(ECM) using intermittent renewable energy offers an attractive solution, due to its modular reactor design and operational flexibility across a broad spectrum of temperatures and pressures. This review emphasizes conversion pathways of methane in various reaction systems, highlighting the significance and advantages of ECM in facilitating a sustainable artificial carbon cycle. This work provides a comprehensive overview of conventional methane activation mechanisms and delineates the complete pathways of methane conversion in electrolysis contexts. Based on surface/interface chemistry, this work systematically analyzes proposed reaction pathways and corresponding strategies to enhance ECM efficiency towards various target products, including syngas, hydrocarbons, oxygenates, and advanced carbon materials. The discussion also encompasses opportunities and challenges for the ECM process, including insights into ECM pathways, rational electrocatalyst design, establishment of benchmarking protocols, electrolyte engineering, enhancement of CH4conversion rates, and minimization of CO_(2)emission.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
Spinel-structured LiNi_(0.5)Mn_(1.5)O_(4) cathodes in lithium-ion batteries have gained attention for their high operating voltage,which provides high energy density,and their cost advantages due to the absence of cob...Spinel-structured LiNi_(0.5)Mn_(1.5)O_(4) cathodes in lithium-ion batteries have gained attention for their high operating voltage,which provides high energy density,and their cost advantages due to the absence of cobalt.However,issues such as low cycle and thermal stabilities have been identified,with side reactions occurring at the electrode/electrolyte interface during continuous charge/discharge cycles that degrade electrode performance.Herein,we first optimized LiNi_(0.5)Mn_(1.5)O_(4) using the Pechini sol–gel method to achieve uniform particles and controlled calcination temperatures.We then employed density functional theory and electrochemical testing to identify the optimal conditions.Uniform coating of the electrode surface with the oxide solid electrolyte Li_(6.28)Al_(0.24)La_(3)Zr_(2)O_(12)(LALZO)was confirmed,aiming to improve lithium-ion conductivity and enhance cycle and thermal stability.As a result,the formation of a coating layer on the electrode surface suppressed side reactions with the electrolyte and blocked contact,leading to an increase in ion conductivity.This improvement resulted in an enhanced rate capability and a significant increase in retention over 100 cycles at 0.2 C.Additionally,the interface resistance significantly improved with the coating layer,demonstrating reduced voltage decay due to overvoltage and improved interface stability.Finally,thermal stability was enhanced,with retention improving after 100 cycles at 0.5 C.展开更多
H_2O_(2) is one of the most important chemicals in the world.Recently,the electrochemical synthesis of H_2O_(2)by two-electron oxygen reduction reaction(2e^(-)ORR)has attracted great interest.Carbon-based catalysts sh...H_2O_(2) is one of the most important chemicals in the world.Recently,the electrochemical synthesis of H_2O_(2)by two-electron oxygen reduction reaction(2e^(-)ORR)has attracted great interest.Carbon-based catalysts show great promise for electrocatalytic production of H_2O_(2),due to the ease of regulation of the carbon materials with regard to the pore structure,surface properties,and heteroatom doping.Biomass as the carbon precursor has the advantages of low cost,sustainable supply,and extensive availability.Conversion of biomass to functional carbon-based materials shows the attractive merits,such as low carbon emission in the life cycle and diversity of the obtained carbon materials due to the wide source of biomass feedstocks.In this article,a comprehensive review on the mechanisms and processes of electrochemical synthesis of H_2O_(2) by 2e^(-)ORR over carbon-based catalysts is provided.The potential biomass feedstock used for obtaining the carbon-based catalysts,and the strategies to prepare the catalysts by carbonization and heteroatom doping,as well as optimization of electrodes and design of electrolyzer,are discussed.It is recommended that future work focus on developing efficient methods to prepare the catalysts from low-cost biomass feedstock,understanding the mechanisms of 2e^(-)ORR over the catalysts,optimization of electrode materials loaded with biomass-derived catalysts,as well as development of electrolyzers for larger-scale applications.展开更多
Oil production from hydrocarbon reservoirs is invariably accompanied by water production,which poses significant challenges to both production and injection systems,particularly due to the formation of mineral scales....Oil production from hydrocarbon reservoirs is invariably accompanied by water production,which poses significant challenges to both production and injection systems,particularly due to the formation of mineral scales.While scale formation in production wells has been extensively studied,its impact on water disposal wells which is critical for managing produced water and ensuring environmental compliance,remains underexplored.This research gap is especially important because disposal wells face unique challenges,such as injectivity loss,environmental risks from wastewater release,and the need for sustainable scale management practices.This study addresses these challenges by investigating mineral scale formation in a water disposal well in southern Iran.Unlike previous research focused on production wells,this work emphasizes the unique operational and environmental implications of scale precipitation in disposal wells.For this purpose,field information including well schematic,disposal injection system data and acidizing jobs processes performed in well A is investigated.Analyzing and simulation of the composition of the water disposal sample resulted that maximum amount of scale precipitation in surface pipeline is equal to 92 mg/l owing to CaSO_(4) precipitation.Also,CaSO_(4) and CaCO_(3) are precipitated within near wellbore area.CaSO_(4) is the dominate scale type and maximum amount of this scale is 656 mg/l and CaCO_(3) is minor scale type with 54.42 mg/l in near wellbore condition.Furthermore,based on the injection pressure and injection rate data assessment in the time interval between two consecutive acidizing jobs,the formation of scales and the reduction of injectivity in well A are proved.Also,from operation point of view and according to ASTM-0374 method,scale inhibitor should be injected continuously at a concentration of 40 ppm from the surface to cover the entire injection system.The results show that scale inhibitor is an effective solution in prevention of scale precipitation,with 95.2%efficiency in scale formation inhibition.By focusing on disposal wells,this study provides novel insights into scale management strategies tailored to the unique requirements of water disposal operations.The findingshighlight the effectiveness of chemical inhibitors in preventing scale formation and offer a sustainable alternative to conventional acidizing methods.This research contributes to advancing environmentally responsible practices in oilfield water disposal,addressing a critical gap in the field.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
The Edikan Mine,which consists of Fobinso and Esuajah gold deposits,lies within the Asankrangwa Gold Belt of the Birimian Supergroup in the Kumasi Basin.The metasedimentary rocks in the Basins and the faulted metavolc...The Edikan Mine,which consists of Fobinso and Esuajah gold deposits,lies within the Asankrangwa Gold Belt of the Birimian Supergroup in the Kumasi Basin.The metasedimentary rocks in the Basins and the faulted metavolcanic rocks in the Belts that make up the Birimian Supergroup were intruded by granitoids during the Eburnean Orogeny.This research aims to classify granitoids in the Edikan Mine and ascertain the petrogenetic and geochemical characteristics of some auriferous granitoids in the wider Kumasi Basin,Ghana,to understand the implications for geodynamic settings.A multi-methods approach involving field studies,petrographic studies,and whole-rock geochemical analysis was used to achieve the goal of the study.Petrographic studies revealed a relatively high abundance of plagioclase and a low percentage of K-feldspars(anorthoclase and orthoclase)in the Fobinso samples,suggesting that the samples are granodioritic in nature,while the Esuajah samples showed relatively low plagioclase abundance and a high percentage in K-feldspars,indicating that they are granitic.The granitoids from the study areas are co-magmatic.The granitoids in Esuajah and Fobinso are generally enriched in large ion lithophile elements and light rare earth elements than high field strength elements,middle rare earth elements,and heavy rare earth elements,indicating mixing with crustal sources during the evolution of the granitoids.The granitoids were tectonically formed in a syn-collisional+VAG setting,which implies that they were formed in the subduction zone setting.Fobinso granodiorites showed S-type signatures with evidence of extensive crustal contamination,while the Esuajah granites showed I-type signatures with little or no crustal contamination and are peraluminous.Gold mineralization in the study area is structurally and lithologically controlled with shear zones,faulting,and veining as the principal structures controlling the mineralization.The late-stage vein,V3,in the Edikan Mine is characterized by a low vein angle and is mineralized.展开更多
The harsh corrosive environment and sluggish oxygen evolution reaction(OER)kinetics at the anode of proton exchange membrane water electrolysis(PEMWE)cells warrant the use of excess Ir,thereby hindering large-scale in...The harsh corrosive environment and sluggish oxygen evolution reaction(OER)kinetics at the anode of proton exchange membrane water electrolysis(PEMWE)cells warrant the use of excess Ir,thereby hindering large-scale industrialization.To mitigate these issues,the present study aimed at fabricating a robust low-Ir-loading electrode via one-pot synthesis for efficient PEMWE.The pre-electrode was first prepared by alloying through the co-electrodeposition of Ir and Co,followed by the fabrication of Ir–Co oxide(Co-incorporated Ir oxide)electrodes via electrochemical dealloying.Two distinct dealloying techniques resulted in a modified valence state of Ir,and the effects of Co incorporation on the activity and stability of the OER catalysts were clarified using density functional theory(DFT)calculations,which offered theoretical insights into the reaction mechanism.While direct experimental validation of the oxygen evolution mechanism remains challenging under the current conditions,DFT-based theoretical modeling provided valuable perspectives on how Co incorporation could influence key steps in oxygen evolution catalysis.The Ir–Co oxide electrode with a selectively modulated valence state showed impressive performance with an overpotential of 258 mV at 10 mA cm^(−2),a low Tafel slope of 29.4 mV dec^(−1),and stability for 100 h at 100 mA cm^(−2)in the OER,in addition to a low overpotential of 16 mV at−10 mA cm^(−2)and high stability for 24 h in the hydrogen evolution reaction.The PEMWE cell equipped with the bifunctional Ir–Co oxide electrode as the anode and cathode exhibited outstanding performance(11.4 A cm^(−2)at 2.3 Vcell)despite having a low noble-metal content of 0.4 mgNM cm^(−2).展开更多
ZnO-based catalysts have been widely used in hydrogenation reactions,but less attention has been paid to the electrocatalytic hydrogenation process on ZnO electrodes.In this work,the preparation of hydrogen species an...ZnO-based catalysts have been widely used in hydrogenation reactions,but less attention has been paid to the electrocatalytic hydrogenation process on ZnO electrodes.In this work,the preparation of hydrogen species and the associ-ated reduction properties under electrochemi-cal processes in aqueous solutions have been in-vestigated on ZnO and Au/ZnO electrodes.The measurements of cyclic voltammetry(CV),X-ray diffraction,and electron paramagnetic resonance(EPR)confirm the formation of hydro-gen species on the interstitial sites(Hi)or on the oxygen vacancy sites(H_(O)).The hydrogena-tion reaction of p-nitrophenol(pNP)at 40μmol/L occurs on both ZnO and Au/ZnO elec-trodes,and the hydrogenation reduction performance of Au/ZnO electrode is better than that of ZnO electrode.CVs show H_(O)species is much more reactive with pNP than Hi species.Compared with the ZnO electrode,the presence of Au on ZnO promotes the formation of H_(O)species and improves the electro-reduction performance to pNP.These results help us to un-derstand the reaction processes related to the electrochemical hydrogenation on ZnO and Au/ZnO surfaces and shed new light on the design of new catalytic hydrogenation systems.展开更多
Drinking water contamination by heavy metals,particularly chromium and arsenic oxyanions,is a severe challenge threatening humanity’s sustainable development.Electrochemically mediated water purification is gaining a...Drinking water contamination by heavy metals,particularly chromium and arsenic oxyanions,is a severe challenge threatening humanity’s sustainable development.Electrochemically mediated water purification is gaining attention due to its high uptake,rapid kinetics,modularity,and facile regeneration.Here,we designed a composite electrode by combining a redox-active/Faradaic polymer,poly(norbornene-diphenothiazine)(PNP_(2)),with carbon nanotubes(CNTs)–PNP_(2)-CNT.The PNP_(2)-CNT demonstrated exceptional pseudocapacitance behavior,resulting in significantly accelerated adsorption rates for dichromate(Cr(Ⅵ);0.008 gmg^(-1) min^(-1))and arsenite(As(Ⅲ);0.03 gmg^(-1) min^(-1)),surpassing reported materials by a margin of 3–200 times,while demonstrating a high adsorption capacity,666.3 and 612.4 mg g^(-1),respectively.Furthermore,it effectively converted As(Ⅲ)to the less toxic arsenate(As(Ⅴ))during adsorption and Cr(Ⅵ)to the less toxic chromium(Cr(Ⅲ))during desorption.This PNP_(2)-CNT system also showed significantly lower energy consumption,only 0.17%of the CNT control system.This study demonstrated for the first time the use of PNP_(2) redox-active polymers in the separation and conversion process,meeting the six criteria of high uptake,rapid kinetics,selectivity,stability,recyclability,and energy efficiency.This achievement expands the scope of advanced materials that address environmental concerns and make an impact by generating energy-and cost-effective water purification.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
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
A computer-assisted chemical investigation of an intriguing photoreaction of norditerpenoids(3-7)has been first reported,leading to not only their biomimetic conversion,but also the generation of several new products ...A computer-assisted chemical investigation of an intriguing photoreaction of norditerpenoids(3-7)has been first reported,leading to not only their biomimetic conversion,but also the generation of several new products with uncommon 4,14-dioxabicyclo[10.2.1]pentadecane scaffold(8,9,12-14).In bioassay,compounds 10 and 15 exhibited significant stimulation of GLP-1 secretion.This study has given an insight for the application of computational methods on the late-stage skeleton transformation of complex natural products towards new bioactive compounds.展开更多
Among various architectures of polymers,end-group-free rings have attracted growing interests due to their distinct physicochemical performances over the linear counterparts which are exemplified by reduced hydrodynam...Among various architectures of polymers,end-group-free rings have attracted growing interests due to their distinct physicochemical performances over the linear counterparts which are exemplified by reduced hydrodynamic size and slower degradation.It is key to develop facile methods to large-scale synthesis of polymer rings with tunable compositions and microstructures.Recent progresses in large-scale synthesis of polymer rings against single-chain dynamic nanoparticles,and the example applications in synchronous enhancing toughness and strength of polymer nanocomposites are summarized.Once there is the breakthrough in rational design and effective large-scale synthesis of polymer rings and their functional derivatives,a family of cyclic functional hybrids would be available,thus providing a new paradigm in developing polymer science and engineering.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
Juniperus oxycedrus(J.oxycedrus)is a traditional culinary spice and medicinal herb with a longstanding history of ethnopharmacological applications across diverse cultures.While prior research has explored the biologi...Juniperus oxycedrus(J.oxycedrus)is a traditional culinary spice and medicinal herb with a longstanding history of ethnopharmacological applications across diverse cultures.While prior research has explored the biological activities and phytochemical constituents of extracts derived from its leaves and seed cones,the present study systematically investigates their mineral and phenolic profiles alongside their multifunctional bioactive potential.Inductively coupled plasma-atomic emission spectroscopy(ICP-AES)analysis revealed a substantial abundance of essential macro-and microelements.Reversed-phase high-performance liquid chromatography(RP-HPLC)further identified high concentrations of phenolic acids(e.g.,p-coumaric acid)and flavonoids(e.g.,rutin and quercetin).The extracts exhibited potent radical scavenging activity against 2,2-diphenyl-1-picrylhydrazyl(DPPH),robust antioxidant capacity against hydrogen peroxide,and significant inhibition of xanthine oxidase(XO)activity.Notably,both extracts demonstrated marked antibacterial efficacy.In silico molecular docking studies suggested that the antimicrobial activity may stem from the phenolic constituents,which exhibited favorable binding affinities to the active site of bacterial target proteins.These findings underscore J.oxycedrus as a promising reservoir of bioactive natural compounds,warranting further exploration for therapeutic and nutraceutical applications.展开更多
The transport properties of liquid mixtures confined within porous media can change significantly from those observed for bulk mixtures due to changes in the liquid structuring within the pore space.Here,pulsed field ...The transport properties of liquid mixtures confined within porous media can change significantly from those observed for bulk mixtures due to changes in the liquid structuring within the pore space.Here,pulsed field gradient NMR was used to measure the diffusion coefficient of ethanol in ethanol-water liquid mixtures confined within silicas with pore diameters of 6 nm and 3 nm as a function of composition.For liquids imbibed within the 6 nm pores,the composition dependence of the ethanol diffusion coefficient closely followed that of the bulk liquid mixture and the absolute diffusion coefficients were reduced by a tortuosity factor of 3,with a minor contribution due to liquid-surface interactions.For liquids imbibed within the 3 nm pores,the diffusion coefficient of ethanol decreased as the composition of ethanol within the pore space increased,and for single-component ethanol imbibition the effective tortuosity was 63.Fast field cycling NMR experiments showed that the diffusion behaviour was not controlled by an increase in ethanol adsorption strength.A geometric analysis of the pore space was consistent with a highly confined system in which most molecules interacted with the pore walls.Under such confinement,the liquid structuring within the bulk pore space did not reflect that of the bulk liquid mixtures,and the observed decrease in diffusion coefficient as ethanol composition increased was consistent with an increase in confinement due to the larger size of the ethanol molecule.展开更多
The osteochondral(OC)interface exhibits a mineral gradient,varying in thickness by several hundred micrometers across different species.Disruptions in this interface damage OC tissues,leading to osteoarthritis.The nat...The osteochondral(OC)interface exhibits a mineral gradient,varying in thickness by several hundred micrometers across different species.Disruptions in this interface damage OC tissues,leading to osteoarthritis.The natural architecture and composition of native OC interfaces can be replicated using biomaterial scaffolds via regenerative engineering approaches.A novel one-step bioextrusion process was employed to fabricate a unitary synthetic graft(USG),which mimics the native OC interface’s mineral concentration gradient.This novel USG is composed of an agarose-based cartilage layer and a bone layer,consisting of agarose enriched with 20%(200 g/L)hydroxyapatite.The USG features a gradient interface with mineral concentrations transitioning from 0%to 20%(mass fraction),mimicking the transition between the cartilage and bone.Thermogravimetric analysis revealed that the gradient transition lengths of the graft and native OC tissue harvested from bovine knees were similar((647±21)vs.(633±124)μm).The linear viscoelastic properties of the grafts,which were evaluated using strain sweep and frequency sweep tests with oscillatory shear,indicated a dominant storage modulus over loss modulus similar to that of native OC tissues.The compressive and stress relaxation behaviors of the USGs demonstrated that the graft maintained structural integrity under mechanical stress.Viability assays performed after bioextrusion showed that chondrocytes and human fetal osteoblast cells successfully integrated and survived within their designated regions of the graft.The novel USGs exhibit properties similar to native OC tissue and are promising candidates for regenerating OC defects and restoring knee joint functionality.展开更多
Space exploration and manufacturing are of critical importance for scientific advancement,technological innovation,national security,and the acquisition of extraterrestrial resources.In view of this,chemical and biolo...Space exploration and manufacturing are of critical importance for scientific advancement,technological innovation,national security,and the acquisition of extraterrestrial resources.In view of this,chemical and biological nano-/micro-/meso-scale manufacturing provide complementary approaches to overcome key space exploration challenges by enabling the in-situ production of essential life-support materials,propellants,and other resources.This review examines the origin and historical evolution of space manufacturing and the latest advances across different environments—from orbital space stations and the lunar surface to Mars and asteroids.It is structured to present the current state of research,outline key manufacturing strategies and technologies,assess the technical and environmental challenges,and discuss emerging trends and future directions.Besides,the potential applications of emerging technologies such as synthetic biology and artificial intelligence in overcoming the limitations of microgravity,limited resources,and extreme conditions are discussed.Ultimately,this integrative review could serve to guide future development,from advancing space science and disruptive manufacturing to enabling interdisciplinary and application-level innovations.展开更多
基金financial support from the Yunnan Province Key Industries Science and Technology Special Project for Colleges and UniversitiesChina(No.FWCY-QYCT2024006)+6 种基金National Natural Science Foundation of China(Nos.52104351 and 52364051)Science and Technology Major Project of Yunnan Province,China(No.202202AG050007)the Yunnan Fundamental Research ProjectsChina(No.202401AT070314)the Key Technology Research and Development Program of Shandong Province,China(No.2023CXGC010903)Central Guidance Local Scientific and Technological Development Funds,China(No.202407AB110022)Yunnan Province Xingdian Talent Support Plan Project,China。
文摘Titanium exhibits outstanding properties,particularly,high specific strength and resistance to both high and low temperatures,earning it a reputation as the metal of the future.However,because of the highly reactive nature of titanium,metallic titanium production involves extensive procedures and high costs.Considering its advantages and limitations,the European Union has classified titanium metal as a critical raw material(CRM)of low category.The Kroll process is predominantly used to produce titanium;however,molten salt electrolysis(MSE)is currently being explored for producing metallic titanium at a low cost.Since 2000,electrolytic titanium production has undergone a wave of technological advancements.However,because of the intermediate and disproportionation reactions in the electrolytic titanium production process,the process efficiency and titanium purity according to industrial standards could not be achieved.Consequently,metallic titanium production has gradually diversified into employing technologies such as thermal reduction,MSE,and titanium alloy preparation.This study provides a comprehensive review of research advances in titanium metal preparation technologies over the past two decades,highlighting the challenges faced by the existing methods and proposing potential solutions.It offers useful insights into the development of low-cost titanium preparation technologies.
基金National Key R&D Program of China (2023YFA1508001 and 2023YFA1508002)National Natural Science Foundation of China (22272120 and U2202251)+1 种基金Hainan Province Science and Technology Special Fund(ZDYF2023SHFZ120)Research Foundation of Marine Science and Technology Collaborative Innovation Center of Hainan University (XTCX2022HYB01)。
文摘Methane, an abundant one-carbon(C_(1)) resource, is extensively used in the industrial production of vital fuels and value-added chemicals. However, current industrial methane conversion technologies are energy-and carbon-intensive, mainly due to the high activation energy required to break the inert C–H bond, low selectivity, and problematic side reactions, including CO_(2)emissions and coke deposition. Electrochemical conversion of methane(ECM) using intermittent renewable energy offers an attractive solution, due to its modular reactor design and operational flexibility across a broad spectrum of temperatures and pressures. This review emphasizes conversion pathways of methane in various reaction systems, highlighting the significance and advantages of ECM in facilitating a sustainable artificial carbon cycle. This work provides a comprehensive overview of conventional methane activation mechanisms and delineates the complete pathways of methane conversion in electrolysis contexts. Based on surface/interface chemistry, this work systematically analyzes proposed reaction pathways and corresponding strategies to enhance ECM efficiency towards various target products, including syngas, hydrocarbons, oxygenates, and advanced carbon materials. The discussion also encompasses opportunities and challenges for the ECM process, including insights into ECM pathways, rational electrocatalyst design, establishment of benchmarking protocols, electrolyte engineering, enhancement of CH4conversion rates, and minimization of CO_(2)emission.
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supported by the National Research Foundation of Korea(NRF)(No.2020R1A2C2010510,2020R1A6A1A03044977).
文摘Spinel-structured LiNi_(0.5)Mn_(1.5)O_(4) cathodes in lithium-ion batteries have gained attention for their high operating voltage,which provides high energy density,and their cost advantages due to the absence of cobalt.However,issues such as low cycle and thermal stabilities have been identified,with side reactions occurring at the electrode/electrolyte interface during continuous charge/discharge cycles that degrade electrode performance.Herein,we first optimized LiNi_(0.5)Mn_(1.5)O_(4) using the Pechini sol–gel method to achieve uniform particles and controlled calcination temperatures.We then employed density functional theory and electrochemical testing to identify the optimal conditions.Uniform coating of the electrode surface with the oxide solid electrolyte Li_(6.28)Al_(0.24)La_(3)Zr_(2)O_(12)(LALZO)was confirmed,aiming to improve lithium-ion conductivity and enhance cycle and thermal stability.As a result,the formation of a coating layer on the electrode surface suppressed side reactions with the electrolyte and blocked contact,leading to an increase in ion conductivity.This improvement resulted in an enhanced rate capability and a significant increase in retention over 100 cycles at 0.2 C.Additionally,the interface resistance significantly improved with the coating layer,demonstrating reduced voltage decay due to overvoltage and improved interface stability.Finally,thermal stability was enhanced,with retention improving after 100 cycles at 0.5 C.
基金supported by the National Natural Science Foundation of China(Nos.22478222,22178197,and U23A6005)the Dr.Jentai Yang Sustainable Environmental Protection and Eco-humanistic Education Fund(No.20253000027)which isadministered by the Overseas Chinese Environmental Engineers and Scientists Association。
文摘H_2O_(2) is one of the most important chemicals in the world.Recently,the electrochemical synthesis of H_2O_(2)by two-electron oxygen reduction reaction(2e^(-)ORR)has attracted great interest.Carbon-based catalysts show great promise for electrocatalytic production of H_2O_(2),due to the ease of regulation of the carbon materials with regard to the pore structure,surface properties,and heteroatom doping.Biomass as the carbon precursor has the advantages of low cost,sustainable supply,and extensive availability.Conversion of biomass to functional carbon-based materials shows the attractive merits,such as low carbon emission in the life cycle and diversity of the obtained carbon materials due to the wide source of biomass feedstocks.In this article,a comprehensive review on the mechanisms and processes of electrochemical synthesis of H_2O_(2) by 2e^(-)ORR over carbon-based catalysts is provided.The potential biomass feedstock used for obtaining the carbon-based catalysts,and the strategies to prepare the catalysts by carbonization and heteroatom doping,as well as optimization of electrodes and design of electrolyzer,are discussed.It is recommended that future work focus on developing efficient methods to prepare the catalysts from low-cost biomass feedstock,understanding the mechanisms of 2e^(-)ORR over the catalysts,optimization of electrode materials loaded with biomass-derived catalysts,as well as development of electrolyzers for larger-scale applications.
文摘Oil production from hydrocarbon reservoirs is invariably accompanied by water production,which poses significant challenges to both production and injection systems,particularly due to the formation of mineral scales.While scale formation in production wells has been extensively studied,its impact on water disposal wells which is critical for managing produced water and ensuring environmental compliance,remains underexplored.This research gap is especially important because disposal wells face unique challenges,such as injectivity loss,environmental risks from wastewater release,and the need for sustainable scale management practices.This study addresses these challenges by investigating mineral scale formation in a water disposal well in southern Iran.Unlike previous research focused on production wells,this work emphasizes the unique operational and environmental implications of scale precipitation in disposal wells.For this purpose,field information including well schematic,disposal injection system data and acidizing jobs processes performed in well A is investigated.Analyzing and simulation of the composition of the water disposal sample resulted that maximum amount of scale precipitation in surface pipeline is equal to 92 mg/l owing to CaSO_(4) precipitation.Also,CaSO_(4) and CaCO_(3) are precipitated within near wellbore area.CaSO_(4) is the dominate scale type and maximum amount of this scale is 656 mg/l and CaCO_(3) is minor scale type with 54.42 mg/l in near wellbore condition.Furthermore,based on the injection pressure and injection rate data assessment in the time interval between two consecutive acidizing jobs,the formation of scales and the reduction of injectivity in well A are proved.Also,from operation point of view and according to ASTM-0374 method,scale inhibitor should be injected continuously at a concentration of 40 ppm from the surface to cover the entire injection system.The results show that scale inhibitor is an effective solution in prevention of scale precipitation,with 95.2%efficiency in scale formation inhibition.By focusing on disposal wells,this study provides novel insights into scale management strategies tailored to the unique requirements of water disposal operations.The findingshighlight the effectiveness of chemical inhibitors in preventing scale formation and offer a sustainable alternative to conventional acidizing methods.This research contributes to advancing environmentally responsible practices in oilfield water disposal,addressing a critical gap in the field.
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.
文摘The Edikan Mine,which consists of Fobinso and Esuajah gold deposits,lies within the Asankrangwa Gold Belt of the Birimian Supergroup in the Kumasi Basin.The metasedimentary rocks in the Basins and the faulted metavolcanic rocks in the Belts that make up the Birimian Supergroup were intruded by granitoids during the Eburnean Orogeny.This research aims to classify granitoids in the Edikan Mine and ascertain the petrogenetic and geochemical characteristics of some auriferous granitoids in the wider Kumasi Basin,Ghana,to understand the implications for geodynamic settings.A multi-methods approach involving field studies,petrographic studies,and whole-rock geochemical analysis was used to achieve the goal of the study.Petrographic studies revealed a relatively high abundance of plagioclase and a low percentage of K-feldspars(anorthoclase and orthoclase)in the Fobinso samples,suggesting that the samples are granodioritic in nature,while the Esuajah samples showed relatively low plagioclase abundance and a high percentage in K-feldspars,indicating that they are granitic.The granitoids from the study areas are co-magmatic.The granitoids in Esuajah and Fobinso are generally enriched in large ion lithophile elements and light rare earth elements than high field strength elements,middle rare earth elements,and heavy rare earth elements,indicating mixing with crustal sources during the evolution of the granitoids.The granitoids were tectonically formed in a syn-collisional+VAG setting,which implies that they were formed in the subduction zone setting.Fobinso granodiorites showed S-type signatures with evidence of extensive crustal contamination,while the Esuajah granites showed I-type signatures with little or no crustal contamination and are peraluminous.Gold mineralization in the study area is structurally and lithologically controlled with shear zones,faulting,and veining as the principal structures controlling the mineralization.The late-stage vein,V3,in the Edikan Mine is characterized by a low vein angle and is mineralized.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(RS-2024-00340074,RS-2024-00409901,2022M3I3A1081901,and RS-2024-00413272)。
文摘The harsh corrosive environment and sluggish oxygen evolution reaction(OER)kinetics at the anode of proton exchange membrane water electrolysis(PEMWE)cells warrant the use of excess Ir,thereby hindering large-scale industrialization.To mitigate these issues,the present study aimed at fabricating a robust low-Ir-loading electrode via one-pot synthesis for efficient PEMWE.The pre-electrode was first prepared by alloying through the co-electrodeposition of Ir and Co,followed by the fabrication of Ir–Co oxide(Co-incorporated Ir oxide)electrodes via electrochemical dealloying.Two distinct dealloying techniques resulted in a modified valence state of Ir,and the effects of Co incorporation on the activity and stability of the OER catalysts were clarified using density functional theory(DFT)calculations,which offered theoretical insights into the reaction mechanism.While direct experimental validation of the oxygen evolution mechanism remains challenging under the current conditions,DFT-based theoretical modeling provided valuable perspectives on how Co incorporation could influence key steps in oxygen evolution catalysis.The Ir–Co oxide electrode with a selectively modulated valence state showed impressive performance with an overpotential of 258 mV at 10 mA cm^(−2),a low Tafel slope of 29.4 mV dec^(−1),and stability for 100 h at 100 mA cm^(−2)in the OER,in addition to a low overpotential of 16 mV at−10 mA cm^(−2)and high stability for 24 h in the hydrogen evolution reaction.The PEMWE cell equipped with the bifunctional Ir–Co oxide electrode as the anode and cathode exhibited outstanding performance(11.4 A cm^(−2)at 2.3 Vcell)despite having a low noble-metal content of 0.4 mgNM cm^(−2).
基金supported by the National Key Re-search and Development Program of China(No.2021YFA1500403)the National Natural Science Foundation of China(No.21773047 and No.U1832180)partially carried out at the USTC Center for Micro and Nanoscale Research and Fabrication.
文摘ZnO-based catalysts have been widely used in hydrogenation reactions,but less attention has been paid to the electrocatalytic hydrogenation process on ZnO electrodes.In this work,the preparation of hydrogen species and the associ-ated reduction properties under electrochemi-cal processes in aqueous solutions have been in-vestigated on ZnO and Au/ZnO electrodes.The measurements of cyclic voltammetry(CV),X-ray diffraction,and electron paramagnetic resonance(EPR)confirm the formation of hydro-gen species on the interstitial sites(Hi)or on the oxygen vacancy sites(H_(O)).The hydrogena-tion reaction of p-nitrophenol(pNP)at 40μmol/L occurs on both ZnO and Au/ZnO elec-trodes,and the hydrogenation reduction performance of Au/ZnO electrode is better than that of ZnO electrode.CVs show H_(O)species is much more reactive with pNP than Hi species.Compared with the ZnO electrode,the presence of Au on ZnO promotes the formation of H_(O)species and improves the electro-reduction performance to pNP.These results help us to un-derstand the reaction processes related to the electrochemical hydrogenation on ZnO and Au/ZnO surfaces and shed new light on the design of new catalytic hydrogenation systems.
基金supported by the Research Grants Council of the Hong Kong SAR Government(Early Career Scheme,#26309420,and General Research Fund,#16306921 and#16306022)the Department of Chemical and Biomolecular Engineering,HKUST(startup funding)+1 种基金sponsored by the Shanghai Jiao Tong University High-End Computing Center.Y.W.would like to thank the support from the National Natural Science Foundation of China(No.52102183,No.52281240409)the Natural Science Foundation of Shanghai(No.22ZR1433400).
文摘Drinking water contamination by heavy metals,particularly chromium and arsenic oxyanions,is a severe challenge threatening humanity’s sustainable development.Electrochemically mediated water purification is gaining attention due to its high uptake,rapid kinetics,modularity,and facile regeneration.Here,we designed a composite electrode by combining a redox-active/Faradaic polymer,poly(norbornene-diphenothiazine)(PNP_(2)),with carbon nanotubes(CNTs)–PNP_(2)-CNT.The PNP_(2)-CNT demonstrated exceptional pseudocapacitance behavior,resulting in significantly accelerated adsorption rates for dichromate(Cr(Ⅵ);0.008 gmg^(-1) min^(-1))and arsenite(As(Ⅲ);0.03 gmg^(-1) min^(-1)),surpassing reported materials by a margin of 3–200 times,while demonstrating a high adsorption capacity,666.3 and 612.4 mg g^(-1),respectively.Furthermore,it effectively converted As(Ⅲ)to the less toxic arsenate(As(Ⅴ))during adsorption and Cr(Ⅵ)to the less toxic chromium(Cr(Ⅲ))during desorption.This PNP_(2)-CNT system also showed significantly lower energy consumption,only 0.17%of the CNT control system.This study demonstrated for the first time the use of PNP_(2) redox-active polymers in the separation and conversion process,meeting the six criteria of high uptake,rapid kinetics,selectivity,stability,recyclability,and energy efficiency.This achievement expands the scope of advanced materials that address environmental concerns and make an impact by generating energy-and cost-effective water purification.
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 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the National Key Research and Development Program of China(Nos.2021YFF0502400,2022YFC2804100)the Natural Science Foundation of China(Nos.82022069,81991521,42076099,22171153,81903682)+2 种基金Shandong Laboratory Program(No.SYS202205)Ningbo Natural Science Foundation Programme(No.2022J171)the CAS Youth Interdisciplinary Team,and Taishan Scholars Program(Nos.tstp0648,tsqn202312302).
文摘A computer-assisted chemical investigation of an intriguing photoreaction of norditerpenoids(3-7)has been first reported,leading to not only their biomimetic conversion,but also the generation of several new products with uncommon 4,14-dioxabicyclo[10.2.1]pentadecane scaffold(8,9,12-14).In bioassay,compounds 10 and 15 exhibited significant stimulation of GLP-1 secretion.This study has given an insight for the application of computational methods on the late-stage skeleton transformation of complex natural products towards new bioactive compounds.
基金Supported by the National Natural Science Foundation of China(Nos.52293472,22473096 and 22471164)。
文摘Among various architectures of polymers,end-group-free rings have attracted growing interests due to their distinct physicochemical performances over the linear counterparts which are exemplified by reduced hydrodynamic size and slower degradation.It is key to develop facile methods to large-scale synthesis of polymer rings with tunable compositions and microstructures.Recent progresses in large-scale synthesis of polymer rings against single-chain dynamic nanoparticles,and the example applications in synchronous enhancing toughness and strength of polymer nanocomposites are summarized.Once there is the breakthrough in rational design and effective large-scale synthesis of polymer rings and their functional derivatives,a family of cyclic functional hybrids would be available,thus providing a new paradigm in developing polymer science and engineering.
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.
文摘Juniperus oxycedrus(J.oxycedrus)is a traditional culinary spice and medicinal herb with a longstanding history of ethnopharmacological applications across diverse cultures.While prior research has explored the biological activities and phytochemical constituents of extracts derived from its leaves and seed cones,the present study systematically investigates their mineral and phenolic profiles alongside their multifunctional bioactive potential.Inductively coupled plasma-atomic emission spectroscopy(ICP-AES)analysis revealed a substantial abundance of essential macro-and microelements.Reversed-phase high-performance liquid chromatography(RP-HPLC)further identified high concentrations of phenolic acids(e.g.,p-coumaric acid)and flavonoids(e.g.,rutin and quercetin).The extracts exhibited potent radical scavenging activity against 2,2-diphenyl-1-picrylhydrazyl(DPPH),robust antioxidant capacity against hydrogen peroxide,and significant inhibition of xanthine oxidase(XO)activity.Notably,both extracts demonstrated marked antibacterial efficacy.In silico molecular docking studies suggested that the antimicrobial activity may stem from the phenolic constituents,which exhibited favorable binding affinities to the active site of bacterial target proteins.These findings underscore J.oxycedrus as a promising reservoir of bioactive natural compounds,warranting further exploration for therapeutic and nutraceutical applications.
文摘The transport properties of liquid mixtures confined within porous media can change significantly from those observed for bulk mixtures due to changes in the liquid structuring within the pore space.Here,pulsed field gradient NMR was used to measure the diffusion coefficient of ethanol in ethanol-water liquid mixtures confined within silicas with pore diameters of 6 nm and 3 nm as a function of composition.For liquids imbibed within the 6 nm pores,the composition dependence of the ethanol diffusion coefficient closely followed that of the bulk liquid mixture and the absolute diffusion coefficients were reduced by a tortuosity factor of 3,with a minor contribution due to liquid-surface interactions.For liquids imbibed within the 3 nm pores,the diffusion coefficient of ethanol decreased as the composition of ethanol within the pore space increased,and for single-component ethanol imbibition the effective tortuosity was 63.Fast field cycling NMR experiments showed that the diffusion behaviour was not controlled by an increase in ethanol adsorption strength.A geometric analysis of the pore space was consistent with a highly confined system in which most molecules interacted with the pore walls.Under such confinement,the liquid structuring within the bulk pore space did not reflect that of the bulk liquid mixtures,and the observed decrease in diffusion coefficient as ethanol composition increased was consistent with an increase in confinement due to the larger size of the ethanol molecule.
基金supported by the School of Engineering and Digital Sciences of Nazarbayev University,Astana,Kazakhstan(to CE)。
文摘The osteochondral(OC)interface exhibits a mineral gradient,varying in thickness by several hundred micrometers across different species.Disruptions in this interface damage OC tissues,leading to osteoarthritis.The natural architecture and composition of native OC interfaces can be replicated using biomaterial scaffolds via regenerative engineering approaches.A novel one-step bioextrusion process was employed to fabricate a unitary synthetic graft(USG),which mimics the native OC interface’s mineral concentration gradient.This novel USG is composed of an agarose-based cartilage layer and a bone layer,consisting of agarose enriched with 20%(200 g/L)hydroxyapatite.The USG features a gradient interface with mineral concentrations transitioning from 0%to 20%(mass fraction),mimicking the transition between the cartilage and bone.Thermogravimetric analysis revealed that the gradient transition lengths of the graft and native OC tissue harvested from bovine knees were similar((647±21)vs.(633±124)μm).The linear viscoelastic properties of the grafts,which were evaluated using strain sweep and frequency sweep tests with oscillatory shear,indicated a dominant storage modulus over loss modulus similar to that of native OC tissues.The compressive and stress relaxation behaviors of the USGs demonstrated that the graft maintained structural integrity under mechanical stress.Viability assays performed after bioextrusion showed that chondrocytes and human fetal osteoblast cells successfully integrated and survived within their designated regions of the graft.The novel USGs exhibit properties similar to native OC tissue and are promising candidates for regenerating OC defects and restoring knee joint functionality.
基金supported by National Natural Science Foundation of China(22278241)a grant from the Institute Guo Qiang,Tsinghua University(2021GQG1016).
文摘Space exploration and manufacturing are of critical importance for scientific advancement,technological innovation,national security,and the acquisition of extraterrestrial resources.In view of this,chemical and biological nano-/micro-/meso-scale manufacturing provide complementary approaches to overcome key space exploration challenges by enabling the in-situ production of essential life-support materials,propellants,and other resources.This review examines the origin and historical evolution of space manufacturing and the latest advances across different environments—from orbital space stations and the lunar surface to Mars and asteroids.It is structured to present the current state of research,outline key manufacturing strategies and technologies,assess the technical and environmental challenges,and discuss emerging trends and future directions.Besides,the potential applications of emerging technologies such as synthetic biology and artificial intelligence in overcoming the limitations of microgravity,limited resources,and extreme conditions are discussed.Ultimately,this integrative review could serve to guide future development,from advancing space science and disruptive manufacturing to enabling interdisciplinary and application-level innovations.
