This study investigates the differences in pragmatic competence between Hong Kong and Chinese mainland university students.Participants included 19 native speakers of English,115 Chinese mainland students,divided into...This study investigates the differences in pragmatic competence between Hong Kong and Chinese mainland university students.Participants included 19 native speakers of English,115 Chinese mainland students,divided into those who had spent time abroad in an English-speaking country(CM A)and those who had not(CM NA),and 97 Hong Kong students,divided into those from an English-medium secondary school(Hong Kong EMI)and those from a Chinese-medium school(Hong Kong CMI).Linguistic proficiency was measured by a C-test,and pragmatic competence by a Metapragmatic Knowledge Test,an Irony Test and a Monologic Role Play.Group scores were compared using ANCOVAs to control for differences in proficiency.The results point to a continuum of pragmatic competence—EMI>CMI>CM A>CM NA—reflecting the groups’access to English in real-life contexts.The differences between the Hong Kong groups and the Chinese mainland groups were clearest in those tests measuring processing capacity(i.e.,Irony Response Time and the Monologic Role Play).CM A,but not CM NA,performed as well as the Hong Kong groups on measures of metapragmatic awareness.The results are discussed in terms of Bialystok’s(1993)distinction between analyzed representation and control of processing.展开更多
Araneiforms are spider-like ground patterns that are widespread in the southern polar regions of Mars.A gas erosion process driven by the seasonal sublimation of CO_(2) ice was proposed as an explanation for their for...Araneiforms are spider-like ground patterns that are widespread in the southern polar regions of Mars.A gas erosion process driven by the seasonal sublimation of CO_(2) ice was proposed as an explanation for their formation,which cannot occur on Earth due to the high climatic temperature.In this study,we propose an alternative mechanism that attrib-utes the araneiform formation to the erosion of upwelling salt water from the subsurface,relying on the identification of the first terrestrial analog found in a playa of the Qaidam Basin on the northern Tibetan Plateau.Morphological analysis indicates that the structures in the Qaidam Basin have fractal features comparable to araneiforms on Mars.A numerical model is developed to investigate the araneiform formation driven by the water-diffusion mechanism.The simulation res-ults indicate that the water-diffusion process,under varying ground conditions,may be responsible for the diverse aranei-form morphologies observed on both Earth and Mars.Our numerical simulations also demonstrate that the orientations of the saltwater diffusion networks are controlled by pre-existing polygonal cracks,which is consistent with observations of araneiforms on Mars and Earth.Our study thus suggests that a saltwater-related origin of the araneiform is possible and has significant implications for water searches on Mars.展开更多
Background,aim,and scope Environmentally persistent free radicals(EPFRs)have received significant attention due to their longer lifetime and stable existence in various environments.The strong environmental migration ...Background,aim,and scope Environmentally persistent free radicals(EPFRs)have received significant attention due to their longer lifetime and stable existence in various environments.The strong environmental migration ability of particulate matter allows EPFRs to migrate over long-distance transport,thereby impacting the quality of the local atmospheric environment.Additionally,EPFRs can also adhere to atmospheric particles and interact with typical gaseous pollutants to affect atmospheric chemical reactions.EPFRs can produce some reactive organic species,promoting oxidative stress in the human body,damaging biological macromolecules and ultimately affecting the organism health.EPFRs are considered as a novel type of pollutant that affects human health.Despite their significance,there are few literatures available on the characteristics and fate behaviors of EPFRs up to date.Therefore,supplemental reviews are crucial for providing comprehensive understanding of EPFRs.Materials and methods This review summarizes the characteristics of EPFRs in particulate matter,outlines the generation mechanism and influencing factors of EPFRs,and the impacts of EPFRs on environmental quality and organism health.Results The content of EPFRs in particulate matter ranges from 1017 to 1020 spins∙g−1.Due to the strong mobility of atmospheric particulate matter,the long-term exposure to high levels of EPFRs may aggravate the impact of particulate matter on human health.The interaction between EPFRs and typical gaseous pollutants can alter their fate and influence atmospheric chemical reactions.EPFRs are mainly produced by transition metal elements and substituted aromatic hydrocarbons through electron transfer.Additionally,the chemical bond rupture of organic substances through heat treatment or ultraviolet radiation can also produce EPFRs,and heterogeneous reactions are capable producing them as well.The production of EPFRs is not only influenced by transition metal elements and precursors,but also by various environmental factors such as oxygen,temperature,light radiation,and relative humidity.Discussion EPFRs in atmospheric particulates matters are usually rich in fine particulates with obvious seasonal and regional variations.They can easily enter the human respiratory tract and lungs with inhalable particulates,thereby increasing the risk of exposure.Additionally,EPFRs in atmospheric particulates can interact with some typical gaseous pollutants,impacting the life and fate of EPFRs in the atmosphere,and alter atmospheric chemical reactions.Traditionally,EPFRs are generated by transition metal elements and substituted aromatic hydrocarbons undergoing electron transfer in the post-flame and cool-zone regions of combustion systems and other thermal processes to remove HCl,H2O or CO groups,ultimately produce semiquinones,phenoxyls,and cyclopentadienyls.Recent studies have indicated that EPFRs can also be generated under the conditions of without transition metal elemental.Organics can also produce EPFRs through chemical bond rupture during heat treatment or light radiation conditions,as well as through some heterogeneous reactions and photochemical secondary generation of EPFRs.The presence or absence of oxygen has different effects on the type and yield of EPFRs.The concentration,type,and crystal type of transition metal elements will affect the type,content,and atmospheric lifetime of EPFRs.It is generally believed that the impact of transition metal element types on EPFRs is related to the oxidation-reduction potential.The combustion temperature or heat treatment process significantly affects the type and amount of EPFRs.Factors such as precursor loading content,pH conditions,light radiation and relative humidity also influence the generation of EPFRs.EPFRs can interact with pollutants in the environment during their migration and transformation process in environmental medium.This process accelerates the degradation of pollutants and plays a crucial role in the migration and transformation of organic pollutants in environmental media.The reaction process of EPFRs may lead to the production of reactive oxygen species(ROS)such as∙OH,which can induce oxidative stress,inflammation and immune response to biological lung cells and tissues,leading to chronic respiratory and cardiopulmonary dysfunction,cardiovascular damage and neurotoxic effects,ultimately impacting the health of organisms.Conclusions The interaction mechanism between EPFRs in particulate matter and gaseous pollutants remains unclear.Furthermore,research on the generation mechanism of EPFRs without the participation of transition metals is not comprehensive,and the detection of EPFRs is limited to simple qualitative categories and lack accurate qualitative analysis.Recommendations and perspectives Further research should be conducted on the generation mechanism,measurement techniques,migration pathways,and transformation process of EPFRs.It is also important to explore the interaction between EPFRs in atmospheric particulate matter and typical gaseous pollutants.展开更多
Sunlight-driven photocatalytic water-splitting for hydrogen(H2)evolution is a desirable strategy to utilize solar energy.However,this strategy is restricted by insufficient light harvesting and high photogenerated ele...Sunlight-driven photocatalytic water-splitting for hydrogen(H2)evolution is a desirable strategy to utilize solar energy.However,this strategy is restricted by insufficient light harvesting and high photogenerated electron-hole recombination rates of TiO2-based photocatalysts.Here,a graphene-modified WO3/TiO2 step-scheme heterojunction(S-scheme heterojunction)composite photocatalyst was fabricated by a facile one-step hydrothermal method.In the ternary composite,TiO2 and WO3 nanoparticles adhered closely to reduced graphene oxide(rGO)and formed a novel S-scheme heterojunction.Moreover,rGO in the composite not only supplied abundant adsorption and catalytically active sites as an ideal support but also promoted electron separation and transfer from the conduction band of TiO2 by forming a Schottky junction between TiO2 and rGO.The positive cooperative effect of the S-scheme heterojunction formed between WO3 and TiO2 and the Schottky heterojunction formed between TiO2 and graphene sheets suppressed the recombination of relatively useful electrons and holes.This effect also enhanced the light harvesting and promoted the reduction reaction at the active sites.Thus,the novel ternary WO3/TiO2/rGO composite demonstrated a remarkably enhanced photocatalytic H2 evolution rate of 245.8μmol g^-1 h^-1,which was approximately 3.5-fold that of pure TiO2.This work not only presents a low-cost graphene-based S-scheme heterojunction photocatalyst that was obtained via a feasible one-step hydrothermal approach to realize highly efficient H2 generation without using noble metals,but also provides new insights into the design of novel heterojunction photocatalysts.展开更多
Photocatalytic H2 production from water splitting is an effective method to solve energy crisis and environmental pollution simultaneously.Herein,carbon@CdS composite hollow spheres(C@CdS-HS)are fabricated via a facil...Photocatalytic H2 production from water splitting is an effective method to solve energy crisis and environmental pollution simultaneously.Herein,carbon@CdS composite hollow spheres(C@CdS-HS)are fabricated via a facile hydrothermal method using porous carbon hollow spheres(C-HS)as the template.The C@CdS-HS shows an excellent photocatalytic H2-generation rate of 20.9 mmol h^(−1) g^(−1)(apparent quantum efficiency of 15.3%at 420 nm),with 1.0 wt%Pt as a cocatalyst under simulated sunlight irradiation;this rate is 69.7,13.9,and 3.9 times higher than that obtained with pure CdS hollow spheres(CdS-HS),C@CdS-HS,and CdS-HS/Pt,respectively.The enhanced photocatalytic H_(2)-evolution activity of C@CdS-HS/Pt is due to the synergistic effect of C and Pt as the bi-cocatalyst.The C-HS serves not only as an active site provider but also as an electron transporter and reservoir.Moreover,C-HS has a strong photothermal effect that is induced by near infrared light,which kinetically accelerates the H_(2)-production reaction.Additionally,the underlying charge transfer pathway and process from CdS to C−HS is revealed.This work highlights the potential application of C-HS-based nanocomposites in solar-to-chemical energy conversion.展开更多
TiO2‐based Z‐scheme photocatalysts have attracted considerable attention because of the low recombination rate of their photogenerated electron–hole pairs and their high photocatalytic efficiency.In this review,the...TiO2‐based Z‐scheme photocatalysts have attracted considerable attention because of the low recombination rate of their photogenerated electron–hole pairs and their high photocatalytic efficiency.In this review,the reaction mechanism of Z‐scheme photocatalysts,recent research progress in the application of TiO2‐based Z‐scheme photocatalysts,and improved methods for photocatalytic performance enhancement are explored.Their applications,including water splitting,CO2reduction,decomposition of volatile organic compounds,and degradation of organic pollutants,are also described.The main factors affecting the photocatalytic performance of TiO2‐based Z‐scheme photocatalysts,such as pH,conductive medium,cocatalyst,architecture,and mass ratio,are discussed.Concluding remarks are presented,and some suggestions for the future development of TiO2‐based Z‐scheme photocatalysts are highlighted.展开更多
H2 is an important energy carrier for replacing fossil fuel in the future due to its high energy density and environmental friendliness.As a sustainable H2-generation method,photocatalytic H2 production by water split...H2 is an important energy carrier for replacing fossil fuel in the future due to its high energy density and environmental friendliness.As a sustainable H2-generation method,photocatalytic H2 production by water splitting has attracted much interest.Here,oil-soluble ZnxCd1-xS quantum dot(ZCS QD)with a uniform particle size distribution were prepared by a hot-injection method.However,no photocatalytic H2-production activity was observed for the oil-soluble ZCS QD due to its hydrophobicity.Thus,the oil-soluble ZCS QD was converted into a water-soluble ZCS QD by a ligand-exchange method.The water-soluble ZCS QD exhibited excellent photocatalytic H2-production performance in the presence of glycerin and Ni^2+,with an apparent quantum efficiency of 15.9%under irradiation of 420 nm light.Further,the photocatalytic H2-generation activity of the ZCS QD was~10.7 times higher than that of the ZnxCd1-xS relative samples prepared by the conventional co-precipitation method.This work will inspire the design and fabrication of other semiconductor QD photocatalysts because QD exhibits excellent separation efficiency for photogenerated electron-hole pairs due to its small crystallite size.展开更多
Alkaline water splitting is a promising technology for“green hydrogen”generation.To improve its efficiency,highly robust catalysts are required to reduce the overpotential for low electrical power consumption.Hetero...Alkaline water splitting is a promising technology for“green hydrogen”generation.To improve its efficiency,highly robust catalysts are required to reduce the overpotential for low electrical power consumption.Heteroatom modification is one of the most effective strategies for boosting catalytic performance,as it can regulate the physicochemical properties of host catalysts to improve their intrinsic activity.Herein,aiming to provide an overview of the impact of heteroatoms on catalytic activity at the atomic level,we present a review of the key role of heteroatoms in enhancing reaction kinetics based on the reaction pathways of the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)in alkaline media.In particular,the introduction of heteroatoms can directly and indirectly optimize the interactions between the active sites and intermediates,thus improving the intrinsic activity.To clearly illustrate this influence in detail,we have summarized a series of representative heteroatom-modified electrocatalysts and discussed the important roles of heteroatoms in the OER and HER reaction pathways.Finally,some challenges and perspectives for heteroatom-modified electrodes are discussed.We hope that this review will be helpful for the development of efficient and low-cost electrocatalysts for water electrolysis and other energy conversion applications.展开更多
Bismuth‐based photocatalysts are a class of excellent visible‐light photocatalysts;however,their redox activity is relatively poor and the efficiency of photogenerated carrier separation is low,limiting their develo...Bismuth‐based photocatalysts are a class of excellent visible‐light photocatalysts;however,their redox activity is relatively poor and the efficiency of photogenerated carrier separation is low,limiting their development and application in the field of photocatalysis.To address these issues,a series of polyoxometalate PW_(12)O_(40)^(3–)‐doped Bi_(2)O_(3–x)/Bi Schottky photocatalysts PW_(12)@Bi_(2)O_(3–x)/Bi‐n(PBOB‐n,where n is the amount of NaBH4,i.e.,6,12,18,24,and 48 mg)were prepared by a simple electrospinning/calcination/in‐situ NaBH4 reduction method.In this composite photocatalyst,the doping of PW_(12) could effectively adjust the electronic structure of Bi_(2)O_(3–x) and improve its redox properties.As a shallow electron trap,PW_(12) promoted the separation of the photogenerated carriers.Furthermore,desirable Schottky junction between the metal Bi nanoparticles and PW_(12)@Bi_(2)O_(3–x) further accelerated the separation of the photogenerated carriers.The synergistic effect of the aforementioned factors endowed PBOB‐n with excellent photocatalytic activity.Among the samples,PBOB‐18 exhibited superior photocatalytic activity.Under visible‐light irradiation,93.7%(20 mg catalyst)of 20 ppm tetrabromobisphenol A(TBBPA,20 mL)was degraded in 60 min.Its activity was 4.4 times higher than that of Bi_(2)O_(3).PBOB‐18 also exhibited an ultrahigh photocatalytic performance for the removal of NO.Its removal rate(600 ppb)reached 83.3%in 30 min,making it one of the most active Bi‐based photocatalysts.Furthermore,the photocatalytic mechanisms of PBOB‐18 for TBBPA and NO have been proposed.This work provides a new direction and reference for the design of low‐cost,efficient,stable,and versatile photocatalysts.展开更多
The development of low-cost semiconductor photocatalysts for highly efficient and durable photocatalytic H2 evolution under visible light is very challenging.In this study,we combine low-cost metallic Ni3C cocatalysts...The development of low-cost semiconductor photocatalysts for highly efficient and durable photocatalytic H2 evolution under visible light is very challenging.In this study,we combine low-cost metallic Ni3C cocatalysts with twin nanocrystal Zn0.5Cd0.5S(ZCS)solid solution homojunctions for an efficient visible-light-driven H2 production by a simple approach.As-synthesized Zn0.5Cd0.5S-1%Ni3C(ZCS-1)heterojunction/homojunction nanohybrid exhibited the highest photocatalytic H2-evolution rate of 783μmol h‒1 under visible light,which is 2.88 times higher than that of pristine twin nanocrystal ZCS solid solution.The apparent quantum efficiencies of ZCS and ZCS-1 are measured to be 6.13%and 19.25%at 420 nm,respectively.Specifically,the homojunctions between the zinc blende and wurtzite segments in twin nanocrystal ZCS solid solution can significantly improve the light absorption and separation of photogenerated electron-hole pairs.Furthermore,the heterojunction between ZCS and metallic Ni3C NP cocatalysts can efficiently trap excited electrons from ZCS solid solution and enhance the H2-evolution kinetics at the surface for improving catalytic activity.This study demonstrates a unique one-step strategy for constructing heterojunction/homojunction hybrid nanostructures for a more efficient photocatalytic H2 evolution compared to other noble metal photocatalytic systems.展开更多
A synergistic UV/TiO2/Fenton(PCF)process is investigated for the degradation of ibuprofen(IBP)at circumneutral pH.The IBP decay in the PCF process is much faster than that with the conventional UV,UV/H2O2,Fenton,photo...A synergistic UV/TiO2/Fenton(PCF)process is investigated for the degradation of ibuprofen(IBP)at circumneutral pH.The IBP decay in the PCF process is much faster than that with the conventional UV,UV/H2O2,Fenton,photo‐Fenton,and photocatalysis processes.The kinetics analysis showed that the IBP decay follows a two‐stage pseudo‐first order profile,that is,a fast IBP decay(k1)followed by a slow decay(k2).The effects of various parameters,including initial pH level,dosage of Fenton’s reagent and TiO2,wavelength of UV irradiation,and initial IBP concentration,are evaluated.The optimum pH level,[Fe2+]0,[Fe2+]0/[H2O2]0 molar ratio,and[TiO2]0 are determined to be approximately 4.22,0.20 mmol/L,1/40,and 1.0 g/L,respectively.The IBP decay at circumneutral pH(i.e.,6.0–8.0 for wastewater)shows the same IBP decay efficiency as that at the optimum pH of 4.22 after 30 min,which suggests that the PCF process is applicable for the treatment of wastewater in the circumneutral pH range.The lnk1 and lnk2 are observed to be linearly correlated to 1/pH0,[IBP]0,[H2O2]0,[H2O2]0/[Fe2+]0 and ln[TiO2]0.Mathematical models are therefore derived to predict the IBP decay.展开更多
The widespread utilization of fossil fuels has caused an associated increase in CO_(2) emissions over the past few decades,which has resulted in global warming and ocean acidification.CO hydrogenation(Fischer‐Tropsch...The widespread utilization of fossil fuels has caused an associated increase in CO_(2) emissions over the past few decades,which has resulted in global warming and ocean acidification.CO hydrogenation(Fischer‐Tropsch synthesis,FTS)is considered a significant route for the production of liquid fuels and chemicals from nonpetroleum sources to meet worldwide demand.Conversion of CO_(2) with renewable H_(2) into valuable hydrocarbons is beneficial for reducing dependence on fossil fuels and mitigating the negative effects of high CO_(2) concentrations in the atmosphere.Iron‐based catalysts exhibit superior catalytic performance in both FTS and CO_(2) hydrogenation to value‐added hydrocarbons.The abundance and low cost of iron‐based catalysts also promote their wide application in CO_(x) hydrogenation.This paper provides a comprehensive overview of the significant developments in the application of iron‐based catalysts in these two fields.The active phases,promoter effect,and support of iron‐based catalysts are discussed in the present paper.Based on understanding of these three essential aspects,we also cover recent advances in the design and preparation of novel iron‐based catalysts for FTS and CO_(2) hydrogenation.Current challenges and future catalytic applications are also outlined.展开更多
Artificial intelligence(AI) aims to mimic human cognitive functions and execute intellectual activities like that performed by humans dealing with an uncertain environment. The rapid development of AI technology provi...Artificial intelligence(AI) aims to mimic human cognitive functions and execute intellectual activities like that performed by humans dealing with an uncertain environment. The rapid development of AI technology provides powerful tools to analyze massive amounts of data, facilitating physicians to make better clinical decisions or even replace human judgment in healthcare.Advanced AI technology also creates novel opportunities for exploring the scientific basis of traditional Chinese medicine(TCM) and developing the standardization and digitization of TCM pulse diagnostic methodology. In the present study, we review and discuss the potential application of AI technology in TCM pulse diagnosis. The major contents include the following aspects:(1) a brief introduction of the general concepts and knowledge of TCM pulse diagnosis or palpation,(2) landmark developments in AI technology and the applications of common AI deep learning algorithms in medical practice,(3) the current progress of AI technology in TCM pulse diagnosis,(4) challenges and perspectives of AI technology in TCM pulse diagnosis. In conclusion, the pairing of TCM with modern AI technology will bring novel insights into understanding the scientific principles underlying TCM pulse diagnosis and creating opportunities for the development of AI deep learning technology for the standardization and digitalization of TCM pulse diagnosis.展开更多
The carbon nanotubes(CNTs) reinforced Al-Cu matrix composites were prepared by hot pressing sintering and hot rolling, and the effects of Cu content on the interfacial reaction between Al and CNTs, the precipitation b...The carbon nanotubes(CNTs) reinforced Al-Cu matrix composites were prepared by hot pressing sintering and hot rolling, and the effects of Cu content on the interfacial reaction between Al and CNTs, the precipitation behavior of Cu-containing precipitates, and the resultant mechanical properties of the composites were systematically investigated. The results showed that the increase of Cu content can not only increase the number and size of Cu-containing precipitate generated during the composite fabrication processes, but also promote the interfacial reaction between CNTs and Al matrix, leading to the intensified conversion of CNTs into Al_(4)C_(3). As a result, the composite containing 1 wt.% Cu possesses the highest strength, elastic modulus and hardness among all composites, due to the maintenance of the original structure of CNTs. Moreover, the increase of Cu content can change the dominant strengthening mechanisms for the enhanced strength of the fabricated composites.展开更多
The electrochemical reduction of CO_(2) towards hydrocarbons is a promising technology that can utilize CO_(2) and prevent its atmospheric accumulation while simultaneously storing renewable en‐ergy.However,current C...The electrochemical reduction of CO_(2) towards hydrocarbons is a promising technology that can utilize CO_(2) and prevent its atmospheric accumulation while simultaneously storing renewable en‐ergy.However,current CO_(2) electrolyzers remain impractical on a large scale due to the low current densities and faradaic efficiencies(FE)on various electrocatalysts.In this study,hybrid HKUST‐1 metal‐organic framework‒fluorinated imidazolium‐based room temperature ionic liquid(RTIL)electrocatalysts are designed to selectively reduce CO_(2) to CH_(4).An impressive FE of 65.5%towards CH_(4) at-1.13 V is achieved for the HKUST‐1/[BMIM][PF_(6)]hybrid,with a stable FE greater than 50%maintained for at least 9 h in an H‐cell.The observed improvements are attributed to the increased local CO_(2) concentration and the improved CO_(2)‐to‐CH_(4) thermodynamics in the presence of the RTIL molecules adsorbed on the HKUST‐1‐derived Cu clusters.These findings offer a novel approach of immobilizing RTIL co‐catalysts within porous frameworks for CO_(2) electroreduction applications.展开更多
In this study,TiO_(2) nanosheets(NSs)grown in situ on extremely conductive Ti_(3)C_(2)T_(x) MXene to form TiO_(2)/Ti_(3)C_(2)T_(x) MXene composites with abundant active sites are proposed to effectively achieve elec‐...In this study,TiO_(2) nanosheets(NSs)grown in situ on extremely conductive Ti_(3)C_(2)T_(x) MXene to form TiO_(2)/Ti_(3)C_(2)T_(x) MXene composites with abundant active sites are proposed to effectively achieve elec‐trocatalytic NH_(3) synthesis.Electron transfer can be promoted by Ti_(3)C_(2)T_(x) MXene with high conduc‐tivity.Meanwhile,the TiO_(2) NSs in‐situ formation can not only avoid Ti_(3)C_(2)T_(x) MXene microstacking but also enhance the surface specific area of Ti_(3)C_(2)T_(x) MXene.The TiO_(2)/Ti_(3)C_(2)T_(x) MXene catalyst reach‐es a high Faradaic efϐiciency(FE)of 44.68%at−0.75 V vs.RHE and a large NH3 yield of 44.17µg h^(-1) mg^(-1)cat.at−0.95 V,with strong electrochemical durability.15N isotopic labeling experiments imply that the N in the produced NH3 originated from the N2 of the electrolyte.DFT calculations were conducted to determine the possible NRR reaction pathways for TiO_(2)/Ti_(3)C_(2)T_(x) MXene composites.MXene catalysts combined with other materials have been rationally designed for efficient ammonia production under ambient conditions。展开更多
Due to the shortage supply of propylene and the development of shale gas,there is increased interest in on-purpose propane dehydrogenation(PDH)technology for propylene production.Ga-based catalysts have great potentia...Due to the shortage supply of propylene and the development of shale gas,there is increased interest in on-purpose propane dehydrogenation(PDH)technology for propylene production.Ga-based catalysts have great potential in PDH,due to the high activity,low carbon deposit and deactivation.Ga-hydrides formed during PDH reduce the rate,selectivity and yield of propylene.In this contribution,CO_(2)is introduced into PDH as a soft oxidant to eliminate the unfavorable intermediate species Ga^(δ+)-Hx re-generating Ga^(3+)-O pairs,and also minimize coke deposition thereby improving the catalytic performance.In situ diffuse reflectance infrared Fourier transform(DRIFT)spectroscopy experiments show that CO_(2)can effectively eliminate Ga^(δ+)-Hx.At different temperatures,co-feeding CO_(2)during PDH over Ga_(2)O_(3)/SiO_(2)catalysts with different loadings significantly improves the stability of the conversion and selectivity,especially the latter,and provide a new dimension for improving the performance of PDH process.展开更多
Solar‐energy‐driven catalytic CO_(2) reduction for the production of value‐added carbon‐based materials and chemical raw materials has attracted great interest to alleviate the global climate change and energy cri...Solar‐energy‐driven catalytic CO_(2) reduction for the production of value‐added carbon‐based materials and chemical raw materials has attracted great interest to alleviate the global climate change and energy crisis.The production of multicarbon(C2)products through CO_(2) reduction is extremely attractive,however,the yield and selectivity of C2 products remain low because of the low reaction temperature required and the low photoelectron density of the substrate.Here,we introduce WO3–x,which contains oxygen vacancies and exhibits an excellent photothermal conversion efficiency,to improve the generation of C2 products(C2H4 and C2H6)under simulated sunlight(UV‐Vis‐IR)irradiation.WO3–x produced 5.30 and 0.93μmol·g^(–1)C2H4 and C2H6,respectively,after 4 h,with a selectivity exceeding 34%.In situ Fourier transform infrared spectra and theoretical calculations showed that the oxygen vacancies enhanced the water activation and hydrogenation of adsorbed CO for the formation of C2 products via C–C coupling from CH2/CH3 intermediates.The findings of this study could assist in the design of highly active solar‐energy‐driven catalysts to produce C–C coupling products through CO2 reduction.展开更多
Cardiovascular diseases(CVDs)are major disease burdens with high mortality worldwide.Early prediction of cardiovascular events can reduce the incidence of acute myocardial infarction and decrease the mortality rates o...Cardiovascular diseases(CVDs)are major disease burdens with high mortality worldwide.Early prediction of cardiovascular events can reduce the incidence of acute myocardial infarction and decrease the mortality rates of patients with CVDs.The pathological mechanisms and multiple factors involved in CVDs are complex;thus,traditional data analysis is insufficient and inefficient to manage multidimensional data for the risk prediction of CVDs and heart attacks,medical image interpretations,therapeutic decision-making,and disease prognosis prediction.Meanwhile,traditional Chinese medicine(TCM)has been widely used for treating CVDs.TCM offers unique theoretical and practical applications in the diagnosis and treatment of CVDs.Big data have been generated to investigate the scientific basis of TCM diagnostic methods.TCM formulae contain multiple herbal items.Elucidating the complicated interactions between the active compounds and network modulations requires advanced data-analysis capability.Recent progress in artificial intelligence(AI)technology has allowed these challenges to be resolved,which significantly facilitates the development of integrative diagnostic and therapeutic strategies for CVDs and the understanding of the therapeutic principles of TCM formulae.Herein,we briefly introduce the basic concept and current progress of AI and machine learning(ML)technology,and summarize the applications of advanced AI and ML for the diagnosis and treatment of CVDs.Furthermore,we review the progress of AI and ML technology for investigating the scientific basis of TCM diagnosis and treatment for CVDs.We expect the application of AI and ML technology to promote synergy between western medicine and TCM,which can then boost the development of integrative medicine for the diagnosis and treatment of CVDs.展开更多
Single-atom catalysts(SACs)have been widely used in heterogeneous catalysis owing to the maximum utilization of metal-active sites with controlled structures and well-defined locations.Upon tailored coordination with ...Single-atom catalysts(SACs)have been widely used in heterogeneous catalysis owing to the maximum utilization of metal-active sites with controlled structures and well-defined locations.Upon tailored coordination with nitrogen atom,the metal-nitrogen(M-N)-based SACs have demonstrated interesting physical,optical and electronic properties and have become intense in photocatalysis and electrocatalysis in the past decade.Despite substantial efforts in constructing various M–N-based SACs,the principles for modulating the intrinsic photocatalytic and electrocatalytic performance of their active sites and catalytic mechanism have not been sufficiently studied.Herein,the present review intends to shed some light on recent research made in studying the correlation between intrinsic electronic structure,catalytic mechanism,single-metal atom(SMA)confinement and their photocatalytic and electrocatalytic activities(conversion,selectivity,stability and etc).Based on the analysis of fundamentals of M–N-based SACs,theoretical calculations and experimental investigations,including synthetic methods and characterization techniques,are both included to provide an integral understanding of the underlying mechanisms behind improved coordination structure and observed activity.Finally,the challenges and perspectives for constructing highly active M–N based photocatalysis and electrocatalysis SACs are provided.In particular,extensive technical and mechanism aspects are thoroughly discussed,summarized and analyzed for promoting further advancement of M-N-based SACs in photocatalysis and electrocatalysis.展开更多
文摘This study investigates the differences in pragmatic competence between Hong Kong and Chinese mainland university students.Participants included 19 native speakers of English,115 Chinese mainland students,divided into those who had spent time abroad in an English-speaking country(CM A)and those who had not(CM NA),and 97 Hong Kong students,divided into those from an English-medium secondary school(Hong Kong EMI)and those from a Chinese-medium school(Hong Kong CMI).Linguistic proficiency was measured by a C-test,and pragmatic competence by a Metapragmatic Knowledge Test,an Irony Test and a Monologic Role Play.Group scores were compared using ANCOVAs to control for differences in proficiency.The results point to a continuum of pragmatic competence—EMI>CMI>CM A>CM NA—reflecting the groups’access to English in real-life contexts.The differences between the Hong Kong groups and the Chinese mainland groups were clearest in those tests measuring processing capacity(i.e.,Irony Response Time and the Monologic Role Play).CM A,but not CM NA,performed as well as the Hong Kong groups on measures of metapragmatic awareness.The results are discussed in terms of Bialystok’s(1993)distinction between analyzed representation and control of processing.
基金supported by the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB41000000)the Fundamental Research Funds for the Central Universities(WK2080000144)。
文摘Araneiforms are spider-like ground patterns that are widespread in the southern polar regions of Mars.A gas erosion process driven by the seasonal sublimation of CO_(2) ice was proposed as an explanation for their formation,which cannot occur on Earth due to the high climatic temperature.In this study,we propose an alternative mechanism that attrib-utes the araneiform formation to the erosion of upwelling salt water from the subsurface,relying on the identification of the first terrestrial analog found in a playa of the Qaidam Basin on the northern Tibetan Plateau.Morphological analysis indicates that the structures in the Qaidam Basin have fractal features comparable to araneiforms on Mars.A numerical model is developed to investigate the araneiform formation driven by the water-diffusion mechanism.The simulation res-ults indicate that the water-diffusion process,under varying ground conditions,may be responsible for the diverse aranei-form morphologies observed on both Earth and Mars.Our numerical simulations also demonstrate that the orientations of the saltwater diffusion networks are controlled by pre-existing polygonal cracks,which is consistent with observations of araneiforms on Mars and Earth.Our study thus suggests that a saltwater-related origin of the araneiform is possible and has significant implications for water searches on Mars.
文摘Background,aim,and scope Environmentally persistent free radicals(EPFRs)have received significant attention due to their longer lifetime and stable existence in various environments.The strong environmental migration ability of particulate matter allows EPFRs to migrate over long-distance transport,thereby impacting the quality of the local atmospheric environment.Additionally,EPFRs can also adhere to atmospheric particles and interact with typical gaseous pollutants to affect atmospheric chemical reactions.EPFRs can produce some reactive organic species,promoting oxidative stress in the human body,damaging biological macromolecules and ultimately affecting the organism health.EPFRs are considered as a novel type of pollutant that affects human health.Despite their significance,there are few literatures available on the characteristics and fate behaviors of EPFRs up to date.Therefore,supplemental reviews are crucial for providing comprehensive understanding of EPFRs.Materials and methods This review summarizes the characteristics of EPFRs in particulate matter,outlines the generation mechanism and influencing factors of EPFRs,and the impacts of EPFRs on environmental quality and organism health.Results The content of EPFRs in particulate matter ranges from 1017 to 1020 spins∙g−1.Due to the strong mobility of atmospheric particulate matter,the long-term exposure to high levels of EPFRs may aggravate the impact of particulate matter on human health.The interaction between EPFRs and typical gaseous pollutants can alter their fate and influence atmospheric chemical reactions.EPFRs are mainly produced by transition metal elements and substituted aromatic hydrocarbons through electron transfer.Additionally,the chemical bond rupture of organic substances through heat treatment or ultraviolet radiation can also produce EPFRs,and heterogeneous reactions are capable producing them as well.The production of EPFRs is not only influenced by transition metal elements and precursors,but also by various environmental factors such as oxygen,temperature,light radiation,and relative humidity.Discussion EPFRs in atmospheric particulates matters are usually rich in fine particulates with obvious seasonal and regional variations.They can easily enter the human respiratory tract and lungs with inhalable particulates,thereby increasing the risk of exposure.Additionally,EPFRs in atmospheric particulates can interact with some typical gaseous pollutants,impacting the life and fate of EPFRs in the atmosphere,and alter atmospheric chemical reactions.Traditionally,EPFRs are generated by transition metal elements and substituted aromatic hydrocarbons undergoing electron transfer in the post-flame and cool-zone regions of combustion systems and other thermal processes to remove HCl,H2O or CO groups,ultimately produce semiquinones,phenoxyls,and cyclopentadienyls.Recent studies have indicated that EPFRs can also be generated under the conditions of without transition metal elemental.Organics can also produce EPFRs through chemical bond rupture during heat treatment or light radiation conditions,as well as through some heterogeneous reactions and photochemical secondary generation of EPFRs.The presence or absence of oxygen has different effects on the type and yield of EPFRs.The concentration,type,and crystal type of transition metal elements will affect the type,content,and atmospheric lifetime of EPFRs.It is generally believed that the impact of transition metal element types on EPFRs is related to the oxidation-reduction potential.The combustion temperature or heat treatment process significantly affects the type and amount of EPFRs.Factors such as precursor loading content,pH conditions,light radiation and relative humidity also influence the generation of EPFRs.EPFRs can interact with pollutants in the environment during their migration and transformation process in environmental medium.This process accelerates the degradation of pollutants and plays a crucial role in the migration and transformation of organic pollutants in environmental media.The reaction process of EPFRs may lead to the production of reactive oxygen species(ROS)such as∙OH,which can induce oxidative stress,inflammation and immune response to biological lung cells and tissues,leading to chronic respiratory and cardiopulmonary dysfunction,cardiovascular damage and neurotoxic effects,ultimately impacting the health of organisms.Conclusions The interaction mechanism between EPFRs in particulate matter and gaseous pollutants remains unclear.Furthermore,research on the generation mechanism of EPFRs without the participation of transition metals is not comprehensive,and the detection of EPFRs is limited to simple qualitative categories and lack accurate qualitative analysis.Recommendations and perspectives Further research should be conducted on the generation mechanism,measurement techniques,migration pathways,and transformation process of EPFRs.It is also important to explore the interaction between EPFRs in atmospheric particulate matter and typical gaseous pollutants.
基金supported by the National Natural Science Foundation of China(U1705251,21871217,21573170,21433007)the National Key Research and Development Program of China(2018YFB1502001)~~
文摘Sunlight-driven photocatalytic water-splitting for hydrogen(H2)evolution is a desirable strategy to utilize solar energy.However,this strategy is restricted by insufficient light harvesting and high photogenerated electron-hole recombination rates of TiO2-based photocatalysts.Here,a graphene-modified WO3/TiO2 step-scheme heterojunction(S-scheme heterojunction)composite photocatalyst was fabricated by a facile one-step hydrothermal method.In the ternary composite,TiO2 and WO3 nanoparticles adhered closely to reduced graphene oxide(rGO)and formed a novel S-scheme heterojunction.Moreover,rGO in the composite not only supplied abundant adsorption and catalytically active sites as an ideal support but also promoted electron separation and transfer from the conduction band of TiO2 by forming a Schottky junction between TiO2 and rGO.The positive cooperative effect of the S-scheme heterojunction formed between WO3 and TiO2 and the Schottky heterojunction formed between TiO2 and graphene sheets suppressed the recombination of relatively useful electrons and holes.This effect also enhanced the light harvesting and promoted the reduction reaction at the active sites.Thus,the novel ternary WO3/TiO2/rGO composite demonstrated a remarkably enhanced photocatalytic H2 evolution rate of 245.8μmol g^-1 h^-1,which was approximately 3.5-fold that of pure TiO2.This work not only presents a low-cost graphene-based S-scheme heterojunction photocatalyst that was obtained via a feasible one-step hydrothermal approach to realize highly efficient H2 generation without using noble metals,but also provides new insights into the design of novel heterojunction photocatalysts.
文摘Photocatalytic H2 production from water splitting is an effective method to solve energy crisis and environmental pollution simultaneously.Herein,carbon@CdS composite hollow spheres(C@CdS-HS)are fabricated via a facile hydrothermal method using porous carbon hollow spheres(C-HS)as the template.The C@CdS-HS shows an excellent photocatalytic H2-generation rate of 20.9 mmol h^(−1) g^(−1)(apparent quantum efficiency of 15.3%at 420 nm),with 1.0 wt%Pt as a cocatalyst under simulated sunlight irradiation;this rate is 69.7,13.9,and 3.9 times higher than that obtained with pure CdS hollow spheres(CdS-HS),C@CdS-HS,and CdS-HS/Pt,respectively.The enhanced photocatalytic H_(2)-evolution activity of C@CdS-HS/Pt is due to the synergistic effect of C and Pt as the bi-cocatalyst.The C-HS serves not only as an active site provider but also as an electron transporter and reservoir.Moreover,C-HS has a strong photothermal effect that is induced by near infrared light,which kinetically accelerates the H_(2)-production reaction.Additionally,the underlying charge transfer pathway and process from CdS to C−HS is revealed.This work highlights the potential application of C-HS-based nanocomposites in solar-to-chemical energy conversion.
基金supported by the National Natural Science Foundation of China(51602207,21433007,51320105001,21573170)the Self-determined and Innovative Research Funds of SKLWUT(2017-ZD-4,2016-KF-17)the Natural Science Foundation of Hubei Province of China(2015CFA001)~~
文摘TiO2‐based Z‐scheme photocatalysts have attracted considerable attention because of the low recombination rate of their photogenerated electron–hole pairs and their high photocatalytic efficiency.In this review,the reaction mechanism of Z‐scheme photocatalysts,recent research progress in the application of TiO2‐based Z‐scheme photocatalysts,and improved methods for photocatalytic performance enhancement are explored.Their applications,including water splitting,CO2reduction,decomposition of volatile organic compounds,and degradation of organic pollutants,are also described.The main factors affecting the photocatalytic performance of TiO2‐based Z‐scheme photocatalysts,such as pH,conductive medium,cocatalyst,architecture,and mass ratio,are discussed.Concluding remarks are presented,and some suggestions for the future development of TiO2‐based Z‐scheme photocatalysts are highlighted.
文摘H2 is an important energy carrier for replacing fossil fuel in the future due to its high energy density and environmental friendliness.As a sustainable H2-generation method,photocatalytic H2 production by water splitting has attracted much interest.Here,oil-soluble ZnxCd1-xS quantum dot(ZCS QD)with a uniform particle size distribution were prepared by a hot-injection method.However,no photocatalytic H2-production activity was observed for the oil-soluble ZCS QD due to its hydrophobicity.Thus,the oil-soluble ZCS QD was converted into a water-soluble ZCS QD by a ligand-exchange method.The water-soluble ZCS QD exhibited excellent photocatalytic H2-production performance in the presence of glycerin and Ni^2+,with an apparent quantum efficiency of 15.9%under irradiation of 420 nm light.Further,the photocatalytic H2-generation activity of the ZCS QD was~10.7 times higher than that of the ZnxCd1-xS relative samples prepared by the conventional co-precipitation method.This work will inspire the design and fabrication of other semiconductor QD photocatalysts because QD exhibits excellent separation efficiency for photogenerated electron-hole pairs due to its small crystallite size.
文摘Alkaline water splitting is a promising technology for“green hydrogen”generation.To improve its efficiency,highly robust catalysts are required to reduce the overpotential for low electrical power consumption.Heteroatom modification is one of the most effective strategies for boosting catalytic performance,as it can regulate the physicochemical properties of host catalysts to improve their intrinsic activity.Herein,aiming to provide an overview of the impact of heteroatoms on catalytic activity at the atomic level,we present a review of the key role of heteroatoms in enhancing reaction kinetics based on the reaction pathways of the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)in alkaline media.In particular,the introduction of heteroatoms can directly and indirectly optimize the interactions between the active sites and intermediates,thus improving the intrinsic activity.To clearly illustrate this influence in detail,we have summarized a series of representative heteroatom-modified electrocatalysts and discussed the important roles of heteroatoms in the OER and HER reaction pathways.Finally,some challenges and perspectives for heteroatom-modified electrodes are discussed.We hope that this review will be helpful for the development of efficient and low-cost electrocatalysts for water electrolysis and other energy conversion applications.
文摘Bismuth‐based photocatalysts are a class of excellent visible‐light photocatalysts;however,their redox activity is relatively poor and the efficiency of photogenerated carrier separation is low,limiting their development and application in the field of photocatalysis.To address these issues,a series of polyoxometalate PW_(12)O_(40)^(3–)‐doped Bi_(2)O_(3–x)/Bi Schottky photocatalysts PW_(12)@Bi_(2)O_(3–x)/Bi‐n(PBOB‐n,where n is the amount of NaBH4,i.e.,6,12,18,24,and 48 mg)were prepared by a simple electrospinning/calcination/in‐situ NaBH4 reduction method.In this composite photocatalyst,the doping of PW_(12) could effectively adjust the electronic structure of Bi_(2)O_(3–x) and improve its redox properties.As a shallow electron trap,PW_(12) promoted the separation of the photogenerated carriers.Furthermore,desirable Schottky junction between the metal Bi nanoparticles and PW_(12)@Bi_(2)O_(3–x) further accelerated the separation of the photogenerated carriers.The synergistic effect of the aforementioned factors endowed PBOB‐n with excellent photocatalytic activity.Among the samples,PBOB‐18 exhibited superior photocatalytic activity.Under visible‐light irradiation,93.7%(20 mg catalyst)of 20 ppm tetrabromobisphenol A(TBBPA,20 mL)was degraded in 60 min.Its activity was 4.4 times higher than that of Bi_(2)O_(3).PBOB‐18 also exhibited an ultrahigh photocatalytic performance for the removal of NO.Its removal rate(600 ppb)reached 83.3%in 30 min,making it one of the most active Bi‐based photocatalysts.Furthermore,the photocatalytic mechanisms of PBOB‐18 for TBBPA and NO have been proposed.This work provides a new direction and reference for the design of low‐cost,efficient,stable,and versatile photocatalysts.
文摘The development of low-cost semiconductor photocatalysts for highly efficient and durable photocatalytic H2 evolution under visible light is very challenging.In this study,we combine low-cost metallic Ni3C cocatalysts with twin nanocrystal Zn0.5Cd0.5S(ZCS)solid solution homojunctions for an efficient visible-light-driven H2 production by a simple approach.As-synthesized Zn0.5Cd0.5S-1%Ni3C(ZCS-1)heterojunction/homojunction nanohybrid exhibited the highest photocatalytic H2-evolution rate of 783μmol h‒1 under visible light,which is 2.88 times higher than that of pristine twin nanocrystal ZCS solid solution.The apparent quantum efficiencies of ZCS and ZCS-1 are measured to be 6.13%and 19.25%at 420 nm,respectively.Specifically,the homojunctions between the zinc blende and wurtzite segments in twin nanocrystal ZCS solid solution can significantly improve the light absorption and separation of photogenerated electron-hole pairs.Furthermore,the heterojunction between ZCS and metallic Ni3C NP cocatalysts can efficiently trap excited electrons from ZCS solid solution and enhance the H2-evolution kinetics at the surface for improving catalytic activity.This study demonstrates a unique one-step strategy for constructing heterojunction/homojunction hybrid nanostructures for a more efficient photocatalytic H2 evolution compared to other noble metal photocatalytic systems.
文摘A synergistic UV/TiO2/Fenton(PCF)process is investigated for the degradation of ibuprofen(IBP)at circumneutral pH.The IBP decay in the PCF process is much faster than that with the conventional UV,UV/H2O2,Fenton,photo‐Fenton,and photocatalysis processes.The kinetics analysis showed that the IBP decay follows a two‐stage pseudo‐first order profile,that is,a fast IBP decay(k1)followed by a slow decay(k2).The effects of various parameters,including initial pH level,dosage of Fenton’s reagent and TiO2,wavelength of UV irradiation,and initial IBP concentration,are evaluated.The optimum pH level,[Fe2+]0,[Fe2+]0/[H2O2]0 molar ratio,and[TiO2]0 are determined to be approximately 4.22,0.20 mmol/L,1/40,and 1.0 g/L,respectively.The IBP decay at circumneutral pH(i.e.,6.0–8.0 for wastewater)shows the same IBP decay efficiency as that at the optimum pH of 4.22 after 30 min,which suggests that the PCF process is applicable for the treatment of wastewater in the circumneutral pH range.The lnk1 and lnk2 are observed to be linearly correlated to 1/pH0,[IBP]0,[H2O2]0,[H2O2]0/[Fe2+]0 and ln[TiO2]0.Mathematical models are therefore derived to predict the IBP decay.
文摘The widespread utilization of fossil fuels has caused an associated increase in CO_(2) emissions over the past few decades,which has resulted in global warming and ocean acidification.CO hydrogenation(Fischer‐Tropsch synthesis,FTS)is considered a significant route for the production of liquid fuels and chemicals from nonpetroleum sources to meet worldwide demand.Conversion of CO_(2) with renewable H_(2) into valuable hydrocarbons is beneficial for reducing dependence on fossil fuels and mitigating the negative effects of high CO_(2) concentrations in the atmosphere.Iron‐based catalysts exhibit superior catalytic performance in both FTS and CO_(2) hydrogenation to value‐added hydrocarbons.The abundance and low cost of iron‐based catalysts also promote their wide application in CO_(x) hydrogenation.This paper provides a comprehensive overview of the significant developments in the application of iron‐based catalysts in these two fields.The active phases,promoter effect,and support of iron‐based catalysts are discussed in the present paper.Based on understanding of these three essential aspects,we also cover recent advances in the design and preparation of novel iron‐based catalysts for FTS and CO_(2) hydrogenation.Current challenges and future catalytic applications are also outlined.
基金We thank for the funding support form the Health and Medical Research Fund,Hong Kong SAR(No.17181811).
文摘Artificial intelligence(AI) aims to mimic human cognitive functions and execute intellectual activities like that performed by humans dealing with an uncertain environment. The rapid development of AI technology provides powerful tools to analyze massive amounts of data, facilitating physicians to make better clinical decisions or even replace human judgment in healthcare.Advanced AI technology also creates novel opportunities for exploring the scientific basis of traditional Chinese medicine(TCM) and developing the standardization and digitization of TCM pulse diagnostic methodology. In the present study, we review and discuss the potential application of AI technology in TCM pulse diagnosis. The major contents include the following aspects:(1) a brief introduction of the general concepts and knowledge of TCM pulse diagnosis or palpation,(2) landmark developments in AI technology and the applications of common AI deep learning algorithms in medical practice,(3) the current progress of AI technology in TCM pulse diagnosis,(4) challenges and perspectives of AI technology in TCM pulse diagnosis. In conclusion, the pairing of TCM with modern AI technology will bring novel insights into understanding the scientific principles underlying TCM pulse diagnosis and creating opportunities for the development of AI deep learning technology for the standardization and digitalization of TCM pulse diagnosis.
基金The financial supports from the National Natural Science Foundation of China (Nos. 52004101 and 52071269)the Chinese Postdoctoral Science Foundation (No. 2020T130246)+2 种基金the Fund of the State Key Laboratory of Solidification Processing in NWPU, China (No. SKLSP202121)the Guangdong Basic and Applied Basic Research Foundation, China (No. 2020A1515110621)the Fundamental Research Funds for the Central Universities, China (No. 11620345)。
文摘The carbon nanotubes(CNTs) reinforced Al-Cu matrix composites were prepared by hot pressing sintering and hot rolling, and the effects of Cu content on the interfacial reaction between Al and CNTs, the precipitation behavior of Cu-containing precipitates, and the resultant mechanical properties of the composites were systematically investigated. The results showed that the increase of Cu content can not only increase the number and size of Cu-containing precipitate generated during the composite fabrication processes, but also promote the interfacial reaction between CNTs and Al matrix, leading to the intensified conversion of CNTs into Al_(4)C_(3). As a result, the composite containing 1 wt.% Cu possesses the highest strength, elastic modulus and hardness among all composites, due to the maintenance of the original structure of CNTs. Moreover, the increase of Cu content can change the dominant strengthening mechanisms for the enhanced strength of the fabricated composites.
文摘The electrochemical reduction of CO_(2) towards hydrocarbons is a promising technology that can utilize CO_(2) and prevent its atmospheric accumulation while simultaneously storing renewable en‐ergy.However,current CO_(2) electrolyzers remain impractical on a large scale due to the low current densities and faradaic efficiencies(FE)on various electrocatalysts.In this study,hybrid HKUST‐1 metal‐organic framework‒fluorinated imidazolium‐based room temperature ionic liquid(RTIL)electrocatalysts are designed to selectively reduce CO_(2) to CH_(4).An impressive FE of 65.5%towards CH_(4) at-1.13 V is achieved for the HKUST‐1/[BMIM][PF_(6)]hybrid,with a stable FE greater than 50%maintained for at least 9 h in an H‐cell.The observed improvements are attributed to the increased local CO_(2) concentration and the improved CO_(2)‐to‐CH_(4) thermodynamics in the presence of the RTIL molecules adsorbed on the HKUST‐1‐derived Cu clusters.These findings offer a novel approach of immobilizing RTIL co‐catalysts within porous frameworks for CO_(2) electroreduction applications.
文摘In this study,TiO_(2) nanosheets(NSs)grown in situ on extremely conductive Ti_(3)C_(2)T_(x) MXene to form TiO_(2)/Ti_(3)C_(2)T_(x) MXene composites with abundant active sites are proposed to effectively achieve elec‐trocatalytic NH_(3) synthesis.Electron transfer can be promoted by Ti_(3)C_(2)T_(x) MXene with high conduc‐tivity.Meanwhile,the TiO_(2) NSs in‐situ formation can not only avoid Ti_(3)C_(2)T_(x) MXene microstacking but also enhance the surface specific area of Ti_(3)C_(2)T_(x) MXene.The TiO_(2)/Ti_(3)C_(2)T_(x) MXene catalyst reach‐es a high Faradaic efϐiciency(FE)of 44.68%at−0.75 V vs.RHE and a large NH3 yield of 44.17µg h^(-1) mg^(-1)cat.at−0.95 V,with strong electrochemical durability.15N isotopic labeling experiments imply that the N in the produced NH3 originated from the N2 of the electrolyte.DFT calculations were conducted to determine the possible NRR reaction pathways for TiO_(2)/Ti_(3)C_(2)T_(x) MXene composites.MXene catalysts combined with other materials have been rationally designed for efficient ammonia production under ambient conditions。
文摘Due to the shortage supply of propylene and the development of shale gas,there is increased interest in on-purpose propane dehydrogenation(PDH)technology for propylene production.Ga-based catalysts have great potential in PDH,due to the high activity,low carbon deposit and deactivation.Ga-hydrides formed during PDH reduce the rate,selectivity and yield of propylene.In this contribution,CO_(2)is introduced into PDH as a soft oxidant to eliminate the unfavorable intermediate species Ga^(δ+)-Hx re-generating Ga^(3+)-O pairs,and also minimize coke deposition thereby improving the catalytic performance.In situ diffuse reflectance infrared Fourier transform(DRIFT)spectroscopy experiments show that CO_(2)can effectively eliminate Ga^(δ+)-Hx.At different temperatures,co-feeding CO_(2)during PDH over Ga_(2)O_(3)/SiO_(2)catalysts with different loadings significantly improves the stability of the conversion and selectivity,especially the latter,and provide a new dimension for improving the performance of PDH process.
文摘Solar‐energy‐driven catalytic CO_(2) reduction for the production of value‐added carbon‐based materials and chemical raw materials has attracted great interest to alleviate the global climate change and energy crisis.The production of multicarbon(C2)products through CO_(2) reduction is extremely attractive,however,the yield and selectivity of C2 products remain low because of the low reaction temperature required and the low photoelectron density of the substrate.Here,we introduce WO3–x,which contains oxygen vacancies and exhibits an excellent photothermal conversion efficiency,to improve the generation of C2 products(C2H4 and C2H6)under simulated sunlight(UV‐Vis‐IR)irradiation.WO3–x produced 5.30 and 0.93μmol·g^(–1)C2H4 and C2H6,respectively,after 4 h,with a selectivity exceeding 34%.In situ Fourier transform infrared spectra and theoretical calculations showed that the oxygen vacancies enhanced the water activation and hydrogenation of adsorbed CO for the formation of C2 products via C–C coupling from CH2/CH3 intermediates.The findings of this study could assist in the design of highly active solar‐energy‐driven catalysts to produce C–C coupling products through CO2 reduction.
基金The Health and Medical Research Fund,Hong Kong(17181811)。
文摘Cardiovascular diseases(CVDs)are major disease burdens with high mortality worldwide.Early prediction of cardiovascular events can reduce the incidence of acute myocardial infarction and decrease the mortality rates of patients with CVDs.The pathological mechanisms and multiple factors involved in CVDs are complex;thus,traditional data analysis is insufficient and inefficient to manage multidimensional data for the risk prediction of CVDs and heart attacks,medical image interpretations,therapeutic decision-making,and disease prognosis prediction.Meanwhile,traditional Chinese medicine(TCM)has been widely used for treating CVDs.TCM offers unique theoretical and practical applications in the diagnosis and treatment of CVDs.Big data have been generated to investigate the scientific basis of TCM diagnostic methods.TCM formulae contain multiple herbal items.Elucidating the complicated interactions between the active compounds and network modulations requires advanced data-analysis capability.Recent progress in artificial intelligence(AI)technology has allowed these challenges to be resolved,which significantly facilitates the development of integrative diagnostic and therapeutic strategies for CVDs and the understanding of the therapeutic principles of TCM formulae.Herein,we briefly introduce the basic concept and current progress of AI and machine learning(ML)technology,and summarize the applications of advanced AI and ML for the diagnosis and treatment of CVDs.Furthermore,we review the progress of AI and ML technology for investigating the scientific basis of TCM diagnosis and treatment for CVDs.We expect the application of AI and ML technology to promote synergy between western medicine and TCM,which can then boost the development of integrative medicine for the diagnosis and treatment of CVDs.
文摘Single-atom catalysts(SACs)have been widely used in heterogeneous catalysis owing to the maximum utilization of metal-active sites with controlled structures and well-defined locations.Upon tailored coordination with nitrogen atom,the metal-nitrogen(M-N)-based SACs have demonstrated interesting physical,optical and electronic properties and have become intense in photocatalysis and electrocatalysis in the past decade.Despite substantial efforts in constructing various M–N-based SACs,the principles for modulating the intrinsic photocatalytic and electrocatalytic performance of their active sites and catalytic mechanism have not been sufficiently studied.Herein,the present review intends to shed some light on recent research made in studying the correlation between intrinsic electronic structure,catalytic mechanism,single-metal atom(SMA)confinement and their photocatalytic and electrocatalytic activities(conversion,selectivity,stability and etc).Based on the analysis of fundamentals of M–N-based SACs,theoretical calculations and experimental investigations,including synthetic methods and characterization techniques,are both included to provide an integral understanding of the underlying mechanisms behind improved coordination structure and observed activity.Finally,the challenges and perspectives for constructing highly active M–N based photocatalysis and electrocatalysis SACs are provided.In particular,extensive technical and mechanism aspects are thoroughly discussed,summarized and analyzed for promoting further advancement of M-N-based SACs in photocatalysis and electrocatalysis.