With ongoing global warming and increasing energy demands,the CH_(4)-CO_(2)reforming reaction(dry reforming of methane,DRM)has garnered significant attention as a promising carbon capture and utilization technology.Ni...With ongoing global warming and increasing energy demands,the CH_(4)-CO_(2)reforming reaction(dry reforming of methane,DRM)has garnered significant attention as a promising carbon capture and utilization technology.Nickel-based catalysts are renowned for their outstanding activity and selectivity in this process.The impact of metal-support interaction(MSI),on Ni-based catalyst performance has been extensively researched and debated recently.This paper reviews the recent research progress of MSI on Ni-based catalysts and their characterization and modulation strategies in catalytic reactions.From the perspective of MSI,the effects of different carriers(metal oxides,carbon materials and molecular sieves,etc.)are introduced on the dispersion and surface structure of Ni active metal particles,and the effect of MSI on the activity and stability of DRM reactions on Ni-based catalysts is discussed in detail.Future research should focus on better understanding and controlling MSI to improve the performance and durability of nickel-based catalysts in CH_(4)-CO_(2)reforming,advancing cleaner energy technologies.展开更多
By simplifying catalyst-product separation and reducing phosphorus waste,heterogeneous hydroformylation offers a more sustainable alternative to homogeneous processes.However,heterogeneous hydroformylation catalysts d...By simplifying catalyst-product separation and reducing phosphorus waste,heterogeneous hydroformylation offers a more sustainable alternative to homogeneous processes.However,heterogeneous hydroformylation catalysts developed thus far still suffer from the issues of much lower activity and metal leaching,which severely hinder their practical application.Here,we demonstrate that incorporating phosphorus(P)atoms into graphitic carbon nitride(PCN)supports facilitates charge transfer from Rh to the PCN support,thus largely enhancing electronic metal-support interactions(EMSIs).In the styrene hydroformylation reaction,the activity of Rh_(1)/PCN single-atom catalysts(SACs)with varying P contents exhibited a volcano-shaped relationship with P doping,where the Rh_(1)/PCN SAC with optimal P doping showed exceptional activity,approximately 5.8-and 3.3-fold greater than that of the Rh_(1)/g-C_(3)N_(4)SAC without P doping and the industrial homogeneous catalyst HRh(CO)(PPh_(3))_(3),respectively.In addition,the optimal Rh_(1)/PCN SAC catalyst also demonstrated largely enhanced multicycle stability without any visible metal aggregation owing to the increased EMSIs,which sharply differed from the severe metal aggregation of large nanoparticles on the Rh_(1)/g-C_(3)N_(4)SAC.Mechan-istic studies revealed that the enhanced catalytic performance could be attributed to electron-deficient Rh species,which reduced CO adsorption while simultaneously promoting alkene adsorption through increased EMSIs.These findings suggest that tuning EMSIs is an effective way to achieve SACs with high activity and durability.展开更多
Metal-support interactions and hydrogen spillover effects in heterogeneous catalysts play a crucial role in aromatic hydrogenation reactions;however,these effects are limited by the metal dispersion on the catalyst an...Metal-support interactions and hydrogen spillover effects in heterogeneous catalysts play a crucial role in aromatic hydrogenation reactions;however,these effects are limited by the metal dispersion on the catalyst and the number of acceptable H*receptors.This study prepares highly dispersed Ni nanoparticles(NPs)catalysts on a Beta substrate via precursor structure topology transformation.In contrast to traditional support materials,the coordination and electronic structure changes between the Ni NPs and the support were achieved,further optimizing the active interface sites and enhancing hydrogen activation and hydrogenation performance.Additionally,the-OH groups at the strong acid sites in zeolite effectively intensified the hydrogen spillover effect as receptors for H^(*)migration and anchoring,accelerating the hydrogenation rate of aromatic rings.Under solvent-free conditions,this catalyst was used for the hydrogenation reaction of aromatic-rich oils,directly producing a C_(8)-C_(14)branched cycloalkanes mixture with an aromatic conversion rate of>99%.The cycloalkanes mixture produced by this method features high density(0.92 g/mL)and a low freezing point(<-60℃),making it suitable for use as high-density aviation fuel or as an additive to enhance the volumetric heat value of conventional aviation fuels in practical applications.展开更多
Maintaining high metal dispersion of supported metal catalysts to achieve superior reactivity under harsh conditions poses one of the main challenges for their practical applications.Constructing and regulating the st...Maintaining high metal dispersion of supported metal catalysts to achieve superior reactivity under harsh conditions poses one of the main challenges for their practical applications.Constructing and regulating the strong metal-support interactions(SMSI)by diverse methodologies has emerged as one of the promising approaches to fabricating robust supported metal catalysts.In this study,we report an L-ascorbic acid(AA)-inducing strategy to generate SMSI on a titania-supported gold(Au)catalyst after high-temperature treatment in an inert atmosphere(600℃,N_(2)).The AA-induced SMSI can efficiently stabilize Au nanoparticles(NPs)and preserve their catalytic performance.The detailed study reveals that the key to realizing this SMSI is the generation of oxygen vacancies within the TiO_(2) support induced by the adsorbed AA,which drives the formation of the Ti Oxpermeable layer onto the Au NPs.The strategy could be extended to TiO_(2)-supported Au catalysts with different crystal phases and platinum group metals,such as Pt,Pd,and Rh.This work offers a promising novel route to design stable and efficient supported noble metal catalysts by constructing SMSI using simple reducing organic adsorbent.展开更多
Photoelectrochemical(PEC)water splitting using bismuth vanadate(BiVO_(4))as a photoanode shows promise for renewable hydrogen production.Depositing cobalt phosphate(CoPi)on the BiVO_(4)photoanode as an oxygen evolutio...Photoelectrochemical(PEC)water splitting using bismuth vanadate(BiVO_(4))as a photoanode shows promise for renewable hydrogen production.Depositing cobalt phosphate(CoPi)on the BiVO_(4)photoanode as an oxygen evolution cocatalyst(OEC)is an effective method to improve the PEC performance.However,the CoPi/BiVO_(4)photoanode still faces challenges in terms of slow interface photogenerated carrier transport.Herein,we utilize the advantage of the classical strong metal-support interaction(SMSI)between Au and BiVO_(4)to prepare a CoPi/Au/BiVO_(4)(SMSI-CoPi/Au/BiVO_(4))photoanode.Due to the formation of SMSI,the accumulated electrons at the interface of CoPi/Au induce the accelerated extraction of photogenerated holes.Meanwhile,the active electron density of CoPi is increased,leading to improved water oxidation kinetic.As a result,the SMSI-CoPi/Au/BiVO_(4)photoanode exhibits a high photocurrent density of 5.01 m A cm^(-2)at 1.23 V versus the reversible hydrogen electrode and an applied bias photon-to-current efficiency of 1.78%.This work highlights a novel approach to enhance hole transfer and water oxidation kinetics of OEC/BiVO_(4)composite photoanodes,offering the great potential of using SMSI for PEC water splitting.展开更多
Water electrolysis poses a significant challenge for balancing catalytic activity and stability of oxygen evolution reaction(OER)electrocatalysts.In this study,we address this challenge by constructing asymmetric redo...Water electrolysis poses a significant challenge for balancing catalytic activity and stability of oxygen evolution reaction(OER)electrocatalysts.In this study,we address this challenge by constructing asymmetric redox chemistry through elaborate surface OO–Ru–OH and bulk Ru–O–Ni/Fe coordination moieties within single-atom Ru-decorated defective NiFe LDH nanosheets(Ru@d-NiFe LDH)in conjunction with strong metal-support interactions(SMSI).Rigorous spectroscopic characterization and theoretical calculations indicate that single-atom Ru can delocalize the O 2p electrons on the surface and optimize d-electron configurations of metal atoms in bulk through SMSI.The^(18)O isotope labeling experiment based on operando differential electrochemical mass spectrometry(DEMS),chemical probe experiments,and theoretical calculations confirm the encouraged surface lattice oxygen,stabilized bulk lattice oxygen,and enhanced adsorption of oxygen-containing intermediates for bulk metals in Ru@d-NiFe LDH,leading to asymmetric redox chemistry for OER.The Ru@d-NiFe LDH electrocatalyst exhibits exceptional performance with an overpotential of 230 mV to achieve 10 mA cm^(−2)and maintains high robustness under industrial current density.This approach for achieving asymmetric redox chemistry through SMSI presents a new avenue for developing high-performance electrocatalysts and instills confidence in its industrial applicability.展开更多
For supported metal catalyst systems,the impact on catalysis originates from the interaction between metal nanoparticles and their support.Metal-support interactions(MSI)can change electronic properties,geometric morp...For supported metal catalyst systems,the impact on catalysis originates from the interaction between metal nanoparticles and their support.Metal-support interactions(MSI)can change electronic properties,geometric morphologies,or chemical compositions of metal nanoparticles to make active sites have specific properties and catalytic activities.Fischer-Tropsch synthesis(FTS)is one of the most effective ways to convert cheap non-petroleum-based carbon sources into high value-added chemicals or ultraclean liquid fuels.In this review,we summarize and classify the impact of MSI on the catalytic activity,selectivity and stability of FTS catalysts.The strategies to tune MSI are introduced in detail,and the recent development of high-efficiency FTS catalysts through the manipulation of SMI strategies has been highlighted.It is emphasized that the active metal sites,which are endowed with special functions by MSI,can change the strength of adsorption bond of adsorbates,consequently controlling the product distribution.展开更多
Designing high-performance and low-cost electrocatalysts for oxygen evolu-tion reaction(OER)is critical for the conversion and storage of sustainable energy technologies.Inspired by the biomineralization process,we ut...Designing high-performance and low-cost electrocatalysts for oxygen evolu-tion reaction(OER)is critical for the conversion and storage of sustainable energy technologies.Inspired by the biomineralization process,we utilized the phosphorylation sites of collagen molecules to combine with cobalt-based mononuclear precursors at the molecular level and built a three-dimensional(3D)porous hierarchical material through a bottom-up biomimetic self-assembly strategy to obtain single-atom catalysts confined on carbonized biomimetic self-assembled carriers(Co SACs/cBSC)after subsequent high-temperature annealing.In this strategy,the biomolecule improved the anchoring efficiency of the metal precursor through precise functional groups;meanwhile,the binding-then-assembling strategy also effectively suppressed the nonspecific adsorption of metal ions,ultimately preventing atomic agglomeration and achieving strong electronic metal-support interactions(EMSIs).Experimental characterizations confirm that binding forms between cobalt metal and carbonized self-assembled substrate(Co–O_(4)–P).Theoretical calculations disclose that the local environment changes significantly tailored the Co d-band center,and optimized the binding energy of oxygenated intermediates and the energy barrier of oxygen release.As a result,the obtained Co SACs/cBSC catalyst can achieve remarkable OER activity and 24 h durability in 1 M KOH(η_(10) at 288 mV;Tafel slope of 44 mV dec^(-1)),better than other transition metal-based catalysts and commercial IrO_(2).Overall,we presented a self-assembly strategy to prepare transition metal SACs with strong EMSIs,providing a new avenue for the preparation of efficient catalysts with fine atomic structures.展开更多
In this study,two Ru/TiO_(2)samples with different TiO_(2)facets were prepared to investigate their photo-thermal catalytic CO_(2)+H_(2)reaction behavior.Without UV irradiation,the Ru/TiO_(2)with 67%{001}facet(3 RT)di...In this study,two Ru/TiO_(2)samples with different TiO_(2)facets were prepared to investigate their photo-thermal catalytic CO_(2)+H_(2)reaction behavior.Without UV irradiation,the Ru/TiO_(2)with 67%{001}facet(3 RT)displayed improved thermal catalytic activity for CO_(2)methanation than that of Ru/TiO_(2)with 30%{001}facet(0 RT).After H_(2)pretreatment,both samples exhibited enhanced thermal catalytic activities,but the H_(2)-treated 3 RT(3 RT-H)exhibited superior activity to that of the H_(2)-treated 0 RT(0 RT-H).Under UV irradiation,3 RT-H exhibited apparent photo-promoted thermal catalytic activity and stability,but the enhanced catalytic activity was lower than that of 0 RT-H.Based on the characterization results,it is proposed that both the surface oxygen vacancies(Vos)(activating CO_(2))and the metallic Ru nanoparticles(activating H_(2))were mainly responsible for CO_(2)methanation.For 0 RT,H_(2)pretreatment and subsequent UV irradiation did not promote the formation of Vos,resulting in low catalytic activity.For 3 RT,on the one hand,H_(2)pretreatment promoted the formation of Vos,which were regenerated under UV irradiation;on the other hand,the photogenerated electrons from TiO_(2)transferred to Ru to maintain the metallic Ru nanoparticles.Both behaviors promoted the activation of CO_(2)and H_(2)and enhanced CO_(2)methanation.Moreover,the photogenerated holes favored the dissociated H at Ru migrating to TiO_(2),also promoting CO_(2)methanation.These behaviors occurring on 3 RT-H may be attributed to the suitable metal-support interaction between the Ru nanoparticles and TiO_(2){001},resulting in the easy activation of lattice oxygen in TiO_(2)to Vos.With reference to the analysis of intermediates,a photo-thermal reaction mechanism is proposed for the Ru/TiO_(2){001}facet sample.展开更多
The interactions between metals and oxide supports,so-called metal-support interactions(MSI),are of great importance in heterogeneous catalysis.Pd-based automotive exhaust control catalysts,especially Pd-based three-w...The interactions between metals and oxide supports,so-called metal-support interactions(MSI),are of great importance in heterogeneous catalysis.Pd-based automotive exhaust control catalysts,especially Pd-based three-way catalysts (TWCs),have received considerable research attention owing to its prominent oxidation activity of HCs/CO,as well as excellent thermal stability.For Pd-based TWCs,the dispersion,chemical state and thermal stability of Pd species,which are crucial to the catalytic performance,are closely associated with interactions between metal nanoparticles and their supporting matrix.Progress on the research about MSI and utilization of MSI in advanced Pd-based three-way catalysts are reviewed here.Along with the development of advanced synthesis approaches and engine control technology,the study on MSI would play a notable role in further development of catalysts for automobile exhaust control.展开更多
Tuning metal-support interactions(MSIs)is an important strategy in heterogeneous catalysis to realize the desirable metal dispersion and redox ability of metal catalysts.Herein,we use pre-reduced Co_(3)O_(4)nanowires(...Tuning metal-support interactions(MSIs)is an important strategy in heterogeneous catalysis to realize the desirable metal dispersion and redox ability of metal catalysts.Herein,we use pre-reduced Co_(3)O_(4)nanowires(Co-NWs)in situ grown on monolithic Ni foam substrates to support Ag catalysts(Ag/Co-NW-R)for soot combustion.The macroporous structure of Ni foam with crossed Co_(3)O_(4)nanowires remarkably increases the soot-catalyst contact effi ciency.Our characterization results demonstrate that Ag species exist as Ag 0 because of the equation Ag^(+)+Co^(2+)=Ag^(0)+Co^(3+),and the pre-reduction treatment enhances interactions between Ag and Co_(3)O_(4).The number of active oxygen species on the Ag-loaded catalysts is approximately twice that on the supports,demonstrating the signifi cant role of Ag sites in generating active oxygen species.Additionally,the strengthened MSI on Ag/Co-NW-R further improves this number by increasing metal dispersion and the intrinsic activity determined by the turnover frequency of these oxygen species for soot oxidation compared with the catalyst without pre-reduction of Co-NW(Ag/Co-NW).In addition to high activity,Ag/Co-NW-R exhibits high catalytic stability and water resistance.The strategy used in this work might be applicable in related catalytic systems.展开更多
Dry reforming of ethane(DRE)has received significant attention because of its potential to produce chemical raw materials and reduce carbon emissions.Herein,a composition-induced strong metal-support interaction(SMSI)...Dry reforming of ethane(DRE)has received significant attention because of its potential to produce chemical raw materials and reduce carbon emissions.Herein,a composition-induced strong metal-support interaction(SMSI)effect over FeNi/Al-Ce-O catalysts is revealed via X-ray photoelectron spectroscopy(XPS),H_(2)-temperature programmed reduction(TPR),and energy dispersive X-ray spectroscopy(EDS)elemental mapping.The introduction of Al into Al-Ce-O supports significantly influences the dispersion of surface active components and improves the catalytic performance for DRE over supported FeNi catalysts due to enhancement of the SMSI effect.The catalytic properties,for example,C_(2)H_(6) and CO_(2) conversion,CO selectivity and yield,and turnover frequencies(TOFs),of supported FeNi catalysts first increase and then decrease with increasing Al content,following the same trend as the theoretical effective surface area(TESA)of the corresponding catalysts.The FeNi/Ce-Al_(0.5) catalyst,with 50%Al content,exhibits the best DRE performance under steady-state conditions at 873 K.As observed by with in situ Fourier transform infrared spectroscopy(FTIR)analysis,the introduction of Al not only increases the content of surface Ce3+and oxygen vacancies but also promotes the dispersion of surface active components,which further alters the catalytic properties for DRE over supported FeNi catalysts.展开更多
The modulation of metal-support interfacial interaction is significant but challenging in the design of high-efficiency and high-stability supported catalysts.Here,we report a synthetic strategy to upgrade Cu-CeO_(2)i...The modulation of metal-support interfacial interaction is significant but challenging in the design of high-efficiency and high-stability supported catalysts.Here,we report a synthetic strategy to upgrade Cu-CeO_(2)interfacial interaction by the pyrolysis of mixed metal-organic framework(MOF)structure.The obtained highly dispersed Cu/CeO_(2)-MOF catalyst via this strategy was used to catalyze water-gas shift reaction(WGSR),which exhibited high activity of 40.5μmolCOgcat^(-1).s^(-1)at 300℃and high stability of about 120 h.Based on comprehensive studies of electronic structure,pyrolysis strategy has significant effect on enhancing metal-support interaction and then stabilizing interfacial Cu^(+)species under reaction conditions.Abundant Cu^(+)species and generated oxygen vacancies over Cu/CeO_(2)-MOF catalyst played a key role in CO molecule activation and H2O molecule dissociation,respectively.Both collaborated closely and then promoted WGSR catalytic performance in comparison with traditio nal supported catalysts.This study shall offer a robust approach to harvest highly dispersed catalysts with finely-tuned metal-support interactions for stabilizing the most interfacial active metal species in diverse heterogeneous catalytic reactions.展开更多
Oxidized copper(Cu)species have shown significant promise for electrocatalytic CO_(2)reduction reaction(CO_(2)RR),but they are hard to retain for longterm operation at negative potential.Herein,we developed a substrat...Oxidized copper(Cu)species have shown significant promise for electrocatalytic CO_(2)reduction reaction(CO_(2)RR),but they are hard to retain for longterm operation at negative potential.Herein,we developed a substrate-anchored thermal annealing strategy to synthesize a CuO/MgO catalyst for CO_(2)RR to CH_(4)with a Faradaic efficiency(FE)of 82.3%and a current density as high as 568.2 mA cm^(-2)at-1.0 V vs.reversible hydrogen electrode.This catalyst also demonstrates exceptional electrocatalytic durability and stability under industrially relevant conditions.In the membrane electrode assembly,the catalyst exhibited a CH_(4)FE of~70%at a current density of 500 mA cm^(-2),along with excellent stability,maintaining operation for 65 h at a cell voltage of~3.6 V.Detailed in-situ characterizations and theoretical calculations confirm that the strong electronic metal-support interactions between CuO clusters and MgO support not only stabilize the Cu^(2+)sites but also optimize the adsorption energies of the key intermediates to promote the CH_(4)pathway.Our insights guide the design of efficient and durable electrocatalyst for CO_(2)methanation.展开更多
Metal-support interaction(MSI) is crucial for fine-tuning the active-site structure of supported catalysts and enhancing performance.Here,we present an ammonia-directed reactive gas-metal-support interaction(RGMSI),in...Metal-support interaction(MSI) is crucial for fine-tuning the active-site structure of supported catalysts and enhancing performance.Here,we present an ammonia-directed reactive gas-metal-support interaction(RGMSI),in which NH_(3) reduces ZnO and assembles an anti-perovskite Ni_(3)ZnN structure with interstitial nitrogen,significantly boosting hydrogenation efficiency.Nitrogen incorporation expands the lattice parameter,increasing the(111) lattice spacing from 2.04Å in Ni to 2.18Å in Ni_(3)ZnN,with an extended Ni-Ni interatomic distance from 2.49Å to 2.65Å.Additionally,Ni-N coordination shifts the d-band center downward and induces electron deficiency in Ni via charge transfer.These modifications optimize reactant adsorption on the tailored Ni_(3)ZnN structure compared to Ni,leading to a remarkable increase in 1,3-butadiene hydrogenation selectivity from 30.0 % to 92.9 %,along with an enhanced TOF from 0.067 s^(-1) to 0.079 s^(-1).These findings highlight RGMSI as a versatile and effective strategy for designing supported metal catalysts,offering new insights into selective hydrogenation catalysis.展开更多
As a multidisciplinary phenomenon,panel aeroelasticity in shock-dominated flow is featured by two primary interactions:Fluid-Structure Interactions(FSIs)and Shock-Boundary Layer Interactions(SBLIs).The former raises s...As a multidisciplinary phenomenon,panel aeroelasticity in shock-dominated flow is featured by two primary interactions:Fluid-Structure Interactions(FSIs)and Shock-Boundary Layer Interactions(SBLIs).The former raises structural concerns,and the latter is of aerodynamic interest.Thus,panel aeroelasticity in shock-dominated flow represents a vital topic for the development and optimization of supersonic vehicles and propulsion systems.This review systematically summarizes recent advances in the methodologies applied to capture structural and fluid dynamics,including theoretical models,numerical simulations,and wind tunnel experiments.The application of data-driven modal decomposition,an advanced technique to extract physically crucial features,on the topic is introduced.From the perspective of FSIs,the distinctive aeroelastic behaviors in shock-dominated flow,including hysteresis phenomena and nonlinear responses,are highlighted.From the perspective of SBLIs,the modifications in their spatial and temporal characteristics imposed by the aeroelastic responses are emphasized.Motivated by the interaction between the shock waves and structural response,different strategies have been proposed to implement aeroelastic suppression and shock control,which have the potential to enhance structural safety and aerodynamic performance in the next generation of high-speed flight vehicles.展开更多
This study reveals the critical role of multiscale interaction within the westerly wind bursts(WWBs)west of the MJO convection in modulating the prediction skill for the November MJO event during the DYNAMO(Dynamics o...This study reveals the critical role of multiscale interaction within the westerly wind bursts(WWBs)west of the MJO convection in modulating the prediction skill for the November MJO event during the DYNAMO(Dynamics of the Madden–Julian Oscillation)field campaign.The characteristics of the MJO convection envelope are obtained by the largescale precipitation tracking method,and a novel metric is introduced to quantify the prediction skill for the MJO convection in the ECMWF reforecast.The ECMWF forecast exhibits approximately 17 days in skillful prediction for the MJO convection—significantly lower than that derived from the global measure.The reforecast ensembles are further classified into high and low skill catalogs based on the mean prediction skill during the observed WWBs period.High-skill ensembles exhibit significantly enhanced low-level westerlies,amplified MJO convection,and reduced spatial separation between the low-level westerlies and MJO convection during the WWBs period,indicating stronger coupling between the large-scale circulation and the convection.Mechanistic analysis reveals that enhanced westerlies in high-skill ensembles can transfer more high-frequency energy to the MJO convection through the flux convergence of interaction energy for MJO convection development,resulting in better prediction skill.展开更多
Using observational and reanalysis datasets,this study explores the mechanisms by which the interactions among multi-timescale flows impacted the onset of rapid intensification(RI)of Typhoon Hato(2017).Hato(2017)forme...Using observational and reanalysis datasets,this study explores the mechanisms by which the interactions among multi-timescale flows impacted the onset of rapid intensification(RI)of Typhoon Hato(2017).Hato(2017)formed within a northwest–southeast-oriented synoptic-scale(with periods<10 days)wave train,concurring with a developing intraseasonal(10–90 days)oscillation and an elongated low-frequency(>90 days)monsoon trough in the western North Pacific.Impacted by continuously increasing vertical wind shear,the TC long maintained a highly asymmetric convective structure.Prior to RI onset,the synoptic-scale circulation and the inner-core asymmetric convection of Hato(2017)greatly strengthened,which are the key factors believed to trigger RI.A multi-timescale eddy kinetic energy budget indicates that the wind convergence associated with the intraseasonal circulation and monsoon trough led to barotropic energy conversion that largely enhanced the synoptic-scale cyclonic circulation.Besides,the pronounced increases in midlevel relative humidity(RH)and surface latent heat flux(LHF)were observed upshear before RI onset,which were primarily driven by the strong intraseasonal and synoptic-scale RH anomalies and the strengthened low-level wind speed,respectively.The increased LHF and midlevel RH,together with the enhanced downshear confluence between synoptic-scale and Intraseasonal Oscillation(ISO)/low-frequency winds,could have helped the intensification of asymmetric convection that supports RI onset.Overall,this study suggests that the interactions across multiple timescales may create favorable dynamic and thermodynamic conditions that promoted RI onset,offering new insights into RI processes for highly asymmetric tropical cyclones like Hato(2017).展开更多
Existing quantitative trait locus(QTL)mapping had low efficiency in identifying small-effect and closely linked QTL-by-environment interactions(QEIs)in recombinant inbred lines(RILs),especially in the era of global cl...Existing quantitative trait locus(QTL)mapping had low efficiency in identifying small-effect and closely linked QTL-by-environment interactions(QEIs)in recombinant inbred lines(RILs),especially in the era of global climate change.To address this challenge,here we integrate the compressed variance component mixed model with our GCIM to propose 3vGCIM for identifying QEIs in RILs,and extend 3vGCIM-random to 3vGCIM-fixed.3vGCIM integrates genome-wide scanning with machine learning,significantly improving power.In the mixed full model,we consider all possible effects and control for all possible polygenic backgrounds.In simulation studies,3vGCIM exhibits higher power(∼92.00%),higher accuracy of the estimates for QTL position(∼1.900 cM2)and effect(∼0.050),and lower false positive rate(∼0.48‰)and false negative rate(<8.10%)in three environments of 300 RILs each than ICIM(47.57%;3.607 cM2,0.583;2.81‰;52.43%)and MCIM(60.30%;5.279 cM2,0.274;2.17‰;39.70%).In the real data analysis of rice yield-related traits in 240 RILs,3vGCIM mines more known genes(57–60)and known gene-by-environment interactions(GEIs)(14–19)and candidate GEIs(21–23)than ICIM(27,2,and 7),and MCIM(21,1,and 3),especially in small-effect and linked QTLs and QEIs.This makes 3vGCIM a powerful and sensitive tool for QTL mapping and molecular QTL mapping.展开更多
The antioxidant activity of selenium-containing soybean peptides(SePPs)has been previously demonstrated,despite their limited absorption in the small intestine.This study investigates the antioxidant mechanism of a se...The antioxidant activity of selenium-containing soybean peptides(SePPs)has been previously demonstrated,despite their limited absorption in the small intestine.This study investigates the antioxidant mechanism of a selenium-containing tetrapeptide,Ser-Phe-Gln-SeM(SFQSeM),identified from SePPs,with particular emphasis on its interaction with the intestinal microbiota and its role in modulating host antioxidant defenses.The effects of SFQSeM were evaluated in a D-galactose-induced oxidative stress model and an antibiotictreated mouse model.SFQSeM supplementation significantly reduced the oxidative stress in D-galactosetreated mice.It also promoted the growth of beneficial bacteria and increased the levels of acetate,butyrate and lactate in the intestine(P<0.05).In the antibiotic-treated mouse model,depletion of the intestinal microbiota significantly reduced hepatic glutathione peroxidase(GSH-Px)activity(26.6%)and glutathione peroxidase 1(GPx-1)expression(48.77%)compared to normal mice supplemented with SFQSeM(P<0.05).In contrast to Na_(2)SeO_(3)and selenomethionine,SFQSeM effectively restored the diversity of the intestinal microbiota disrupted by antibiotics.Lactobacillus,Lachnospiraceae_NK4A136_group,and Muribaculaceae were identified as predominant bacteria in the SFQSeM group,and were strongly associated with increased hepatic GSH-Px activity and GPx-1 mRNA expression(P<0.05).In conclusion,intestinal microbiota enhances the antioxidant efficacy of SFQSeM by modulating microbial composition,producing active metabolites,and converting SFQSeM into a bioactive form of selenium.展开更多
基金supported by the Natural Science Foundation of Shanxi Province(202203021221155)the Foundation of National Key Laboratory of High Efficiency and Low Carbon Utilization of Coal(J23-24-902)。
文摘With ongoing global warming and increasing energy demands,the CH_(4)-CO_(2)reforming reaction(dry reforming of methane,DRM)has garnered significant attention as a promising carbon capture and utilization technology.Nickel-based catalysts are renowned for their outstanding activity and selectivity in this process.The impact of metal-support interaction(MSI),on Ni-based catalyst performance has been extensively researched and debated recently.This paper reviews the recent research progress of MSI on Ni-based catalysts and their characterization and modulation strategies in catalytic reactions.From the perspective of MSI,the effects of different carriers(metal oxides,carbon materials and molecular sieves,etc.)are introduced on the dispersion and surface structure of Ni active metal particles,and the effect of MSI on the activity and stability of DRM reactions on Ni-based catalysts is discussed in detail.Future research should focus on better understanding and controlling MSI to improve the performance and durability of nickel-based catalysts in CH_(4)-CO_(2)reforming,advancing cleaner energy technologies.
基金supported by the Petrochemical Research Institute Foundation(21-CB-09-01)the National Natural Science Foundation of China(22302186,22025205)+1 种基金the China Postdoctoral Science Foundation(2022M713030,2023T160618)the Fundamental Research Funds for the Central Universities(WK2060000058,WK2060000038).
文摘By simplifying catalyst-product separation and reducing phosphorus waste,heterogeneous hydroformylation offers a more sustainable alternative to homogeneous processes.However,heterogeneous hydroformylation catalysts developed thus far still suffer from the issues of much lower activity and metal leaching,which severely hinder their practical application.Here,we demonstrate that incorporating phosphorus(P)atoms into graphitic carbon nitride(PCN)supports facilitates charge transfer from Rh to the PCN support,thus largely enhancing electronic metal-support interactions(EMSIs).In the styrene hydroformylation reaction,the activity of Rh_(1)/PCN single-atom catalysts(SACs)with varying P contents exhibited a volcano-shaped relationship with P doping,where the Rh_(1)/PCN SAC with optimal P doping showed exceptional activity,approximately 5.8-and 3.3-fold greater than that of the Rh_(1)/g-C_(3)N_(4)SAC without P doping and the industrial homogeneous catalyst HRh(CO)(PPh_(3))_(3),respectively.In addition,the optimal Rh_(1)/PCN SAC catalyst also demonstrated largely enhanced multicycle stability without any visible metal aggregation owing to the increased EMSIs,which sharply differed from the severe metal aggregation of large nanoparticles on the Rh_(1)/g-C_(3)N_(4)SAC.Mechan-istic studies revealed that the enhanced catalytic performance could be attributed to electron-deficient Rh species,which reduced CO adsorption while simultaneously promoting alkene adsorption through increased EMSIs.These findings suggest that tuning EMSIs is an effective way to achieve SACs with high activity and durability.
基金financially supported by the National Natural Science Foundation of China(Grant 22278439,21776313)the Shandong Province Higher Education Youth Innovation Technology Support Program(Grant 2022KJ074)。
文摘Metal-support interactions and hydrogen spillover effects in heterogeneous catalysts play a crucial role in aromatic hydrogenation reactions;however,these effects are limited by the metal dispersion on the catalyst and the number of acceptable H*receptors.This study prepares highly dispersed Ni nanoparticles(NPs)catalysts on a Beta substrate via precursor structure topology transformation.In contrast to traditional support materials,the coordination and electronic structure changes between the Ni NPs and the support were achieved,further optimizing the active interface sites and enhancing hydrogen activation and hydrogenation performance.Additionally,the-OH groups at the strong acid sites in zeolite effectively intensified the hydrogen spillover effect as receptors for H^(*)migration and anchoring,accelerating the hydrogenation rate of aromatic rings.Under solvent-free conditions,this catalyst was used for the hydrogenation reaction of aromatic-rich oils,directly producing a C_(8)-C_(14)branched cycloalkanes mixture with an aromatic conversion rate of>99%.The cycloalkanes mixture produced by this method features high density(0.92 g/mL)and a low freezing point(<-60℃),making it suitable for use as high-density aviation fuel or as an additive to enhance the volumetric heat value of conventional aviation fuels in practical applications.
基金supported by the National Natural Science Foundation of China(NSFC)the Japan Society for the Promotion of Science(JSPS)under the Joint Research Program(Nos.NSFC21961142006 and JPJSJRP20191804)+3 种基金NSFC(Nos.U22A20394 and 22375200)the DICP.CAS-Cardiff Joint Research Units(No.121421ZYLH20230008)the International Partnership Program of Chinese Academy of Sciences(No.028GJHZ2023097GC)the China Postdoctoral Science Foundation(No.2022M723086)。
文摘Maintaining high metal dispersion of supported metal catalysts to achieve superior reactivity under harsh conditions poses one of the main challenges for their practical applications.Constructing and regulating the strong metal-support interactions(SMSI)by diverse methodologies has emerged as one of the promising approaches to fabricating robust supported metal catalysts.In this study,we report an L-ascorbic acid(AA)-inducing strategy to generate SMSI on a titania-supported gold(Au)catalyst after high-temperature treatment in an inert atmosphere(600℃,N_(2)).The AA-induced SMSI can efficiently stabilize Au nanoparticles(NPs)and preserve their catalytic performance.The detailed study reveals that the key to realizing this SMSI is the generation of oxygen vacancies within the TiO_(2) support induced by the adsorbed AA,which drives the formation of the Ti Oxpermeable layer onto the Au NPs.The strategy could be extended to TiO_(2)-supported Au catalysts with different crystal phases and platinum group metals,such as Pt,Pd,and Rh.This work offers a promising novel route to design stable and efficient supported noble metal catalysts by constructing SMSI using simple reducing organic adsorbent.
基金supported by the National Natural Science Foundation of China(Nos.52472241,52403108 and 52301285)Department of Science and Technology of Hubei Province(Nos.2025AFA114 and 2024CSA076)+1 种基金Wuhan Science and Technology Bureau(Nos.2023020201010116 and 2024040801020319)Hubei Provincial Department of Education(No.Q20231703)。
文摘Photoelectrochemical(PEC)water splitting using bismuth vanadate(BiVO_(4))as a photoanode shows promise for renewable hydrogen production.Depositing cobalt phosphate(CoPi)on the BiVO_(4)photoanode as an oxygen evolution cocatalyst(OEC)is an effective method to improve the PEC performance.However,the CoPi/BiVO_(4)photoanode still faces challenges in terms of slow interface photogenerated carrier transport.Herein,we utilize the advantage of the classical strong metal-support interaction(SMSI)between Au and BiVO_(4)to prepare a CoPi/Au/BiVO_(4)(SMSI-CoPi/Au/BiVO_(4))photoanode.Due to the formation of SMSI,the accumulated electrons at the interface of CoPi/Au induce the accelerated extraction of photogenerated holes.Meanwhile,the active electron density of CoPi is increased,leading to improved water oxidation kinetic.As a result,the SMSI-CoPi/Au/BiVO_(4)photoanode exhibits a high photocurrent density of 5.01 m A cm^(-2)at 1.23 V versus the reversible hydrogen electrode and an applied bias photon-to-current efficiency of 1.78%.This work highlights a novel approach to enhance hole transfer and water oxidation kinetics of OEC/BiVO_(4)composite photoanodes,offering the great potential of using SMSI for PEC water splitting.
基金supported by the Guangdong Basic and Applied Basic Research Foundation(2021B1515120072)the Natural Science Foundation of China(22279096 and T2241003)the Fundamental Research Funds for the Central Universities(WUT:2023IVA094).
文摘Water electrolysis poses a significant challenge for balancing catalytic activity and stability of oxygen evolution reaction(OER)electrocatalysts.In this study,we address this challenge by constructing asymmetric redox chemistry through elaborate surface OO–Ru–OH and bulk Ru–O–Ni/Fe coordination moieties within single-atom Ru-decorated defective NiFe LDH nanosheets(Ru@d-NiFe LDH)in conjunction with strong metal-support interactions(SMSI).Rigorous spectroscopic characterization and theoretical calculations indicate that single-atom Ru can delocalize the O 2p electrons on the surface and optimize d-electron configurations of metal atoms in bulk through SMSI.The^(18)O isotope labeling experiment based on operando differential electrochemical mass spectrometry(DEMS),chemical probe experiments,and theoretical calculations confirm the encouraged surface lattice oxygen,stabilized bulk lattice oxygen,and enhanced adsorption of oxygen-containing intermediates for bulk metals in Ru@d-NiFe LDH,leading to asymmetric redox chemistry for OER.The Ru@d-NiFe LDH electrocatalyst exhibits exceptional performance with an overpotential of 230 mV to achieve 10 mA cm^(−2)and maintains high robustness under industrial current density.This approach for achieving asymmetric redox chemistry through SMSI presents a new avenue for developing high-performance electrocatalysts and instills confidence in its industrial applicability.
基金financial support from the National Natural Science Foundation of China(21676182 and 21476159)the Program for Introducing Talents of Discipline to Universities of China(BP0618007)+1 种基金State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering(2020-KF-26)open foundation of State Key Laboratory of Chemical Engineering(SKL-ChE-20B01)。
文摘For supported metal catalyst systems,the impact on catalysis originates from the interaction between metal nanoparticles and their support.Metal-support interactions(MSI)can change electronic properties,geometric morphologies,or chemical compositions of metal nanoparticles to make active sites have specific properties and catalytic activities.Fischer-Tropsch synthesis(FTS)is one of the most effective ways to convert cheap non-petroleum-based carbon sources into high value-added chemicals or ultraclean liquid fuels.In this review,we summarize and classify the impact of MSI on the catalytic activity,selectivity and stability of FTS catalysts.The strategies to tune MSI are introduced in detail,and the recent development of high-efficiency FTS catalysts through the manipulation of SMI strategies has been highlighted.It is emphasized that the active metal sites,which are endowed with special functions by MSI,can change the strength of adsorption bond of adsorbates,consequently controlling the product distribution.
基金The work was supported by the National Natural Science Foundation of China(52372174)Carbon Neutrality Research Institute Fund(CNIF20230204)Special Project of Strategic Cooperation between China National Petroleum Corporation and China University of Petroleum(Beijing)(ZLZX-2020-04).
文摘Designing high-performance and low-cost electrocatalysts for oxygen evolu-tion reaction(OER)is critical for the conversion and storage of sustainable energy technologies.Inspired by the biomineralization process,we utilized the phosphorylation sites of collagen molecules to combine with cobalt-based mononuclear precursors at the molecular level and built a three-dimensional(3D)porous hierarchical material through a bottom-up biomimetic self-assembly strategy to obtain single-atom catalysts confined on carbonized biomimetic self-assembled carriers(Co SACs/cBSC)after subsequent high-temperature annealing.In this strategy,the biomolecule improved the anchoring efficiency of the metal precursor through precise functional groups;meanwhile,the binding-then-assembling strategy also effectively suppressed the nonspecific adsorption of metal ions,ultimately preventing atomic agglomeration and achieving strong electronic metal-support interactions(EMSIs).Experimental characterizations confirm that binding forms between cobalt metal and carbonized self-assembled substrate(Co–O_(4)–P).Theoretical calculations disclose that the local environment changes significantly tailored the Co d-band center,and optimized the binding energy of oxygenated intermediates and the energy barrier of oxygen release.As a result,the obtained Co SACs/cBSC catalyst can achieve remarkable OER activity and 24 h durability in 1 M KOH(η_(10) at 288 mV;Tafel slope of 44 mV dec^(-1)),better than other transition metal-based catalysts and commercial IrO_(2).Overall,we presented a self-assembly strategy to prepare transition metal SACs with strong EMSIs,providing a new avenue for the preparation of efficient catalysts with fine atomic structures.
文摘In this study,two Ru/TiO_(2)samples with different TiO_(2)facets were prepared to investigate their photo-thermal catalytic CO_(2)+H_(2)reaction behavior.Without UV irradiation,the Ru/TiO_(2)with 67%{001}facet(3 RT)displayed improved thermal catalytic activity for CO_(2)methanation than that of Ru/TiO_(2)with 30%{001}facet(0 RT).After H_(2)pretreatment,both samples exhibited enhanced thermal catalytic activities,but the H_(2)-treated 3 RT(3 RT-H)exhibited superior activity to that of the H_(2)-treated 0 RT(0 RT-H).Under UV irradiation,3 RT-H exhibited apparent photo-promoted thermal catalytic activity and stability,but the enhanced catalytic activity was lower than that of 0 RT-H.Based on the characterization results,it is proposed that both the surface oxygen vacancies(Vos)(activating CO_(2))and the metallic Ru nanoparticles(activating H_(2))were mainly responsible for CO_(2)methanation.For 0 RT,H_(2)pretreatment and subsequent UV irradiation did not promote the formation of Vos,resulting in low catalytic activity.For 3 RT,on the one hand,H_(2)pretreatment promoted the formation of Vos,which were regenerated under UV irradiation;on the other hand,the photogenerated electrons from TiO_(2)transferred to Ru to maintain the metallic Ru nanoparticles.Both behaviors promoted the activation of CO_(2)and H_(2)and enhanced CO_(2)methanation.Moreover,the photogenerated holes favored the dissociated H at Ru migrating to TiO_(2),also promoting CO_(2)methanation.These behaviors occurring on 3 RT-H may be attributed to the suitable metal-support interaction between the Ru nanoparticles and TiO_(2){001},resulting in the easy activation of lattice oxygen in TiO_(2)to Vos.With reference to the analysis of intermediates,a photo-thermal reaction mechanism is proposed for the Ru/TiO_(2){001}facet sample.
基金supported by the National Key R&D Program of China (Nos.2017YFC0211102 and 2017YFC0211202)Guangdong Basic and Applied Basic Research Foundation (No.2019A1515110530)+1 种基金Shenzhen Science and Technology Program (No.JCYJ20210324140804013)Tsinghua Shenzhen International Graduate School (Nos.QD2021005N and JC_(2)021007)。
文摘The interactions between metals and oxide supports,so-called metal-support interactions(MSI),are of great importance in heterogeneous catalysis.Pd-based automotive exhaust control catalysts,especially Pd-based three-way catalysts (TWCs),have received considerable research attention owing to its prominent oxidation activity of HCs/CO,as well as excellent thermal stability.For Pd-based TWCs,the dispersion,chemical state and thermal stability of Pd species,which are crucial to the catalytic performance,are closely associated with interactions between metal nanoparticles and their supporting matrix.Progress on the research about MSI and utilization of MSI in advanced Pd-based three-way catalysts are reviewed here.Along with the development of advanced synthesis approaches and engine control technology,the study on MSI would play a notable role in further development of catalysts for automobile exhaust control.
基金supported by the National Natu-ral Science Foundation of China(Nos.21878213,21808211)the open foundation of the State Key Laboratory of Chemical Engineer-ing(SKL-ChE-20B01)Authors are also grateful to the Program of Introducing Talents of Disciplines to China Universities(BP0618007).
文摘Tuning metal-support interactions(MSIs)is an important strategy in heterogeneous catalysis to realize the desirable metal dispersion and redox ability of metal catalysts.Herein,we use pre-reduced Co_(3)O_(4)nanowires(Co-NWs)in situ grown on monolithic Ni foam substrates to support Ag catalysts(Ag/Co-NW-R)for soot combustion.The macroporous structure of Ni foam with crossed Co_(3)O_(4)nanowires remarkably increases the soot-catalyst contact effi ciency.Our characterization results demonstrate that Ag species exist as Ag 0 because of the equation Ag^(+)+Co^(2+)=Ag^(0)+Co^(3+),and the pre-reduction treatment enhances interactions between Ag and Co_(3)O_(4).The number of active oxygen species on the Ag-loaded catalysts is approximately twice that on the supports,demonstrating the signifi cant role of Ag sites in generating active oxygen species.Additionally,the strengthened MSI on Ag/Co-NW-R further improves this number by increasing metal dispersion and the intrinsic activity determined by the turnover frequency of these oxygen species for soot oxidation compared with the catalyst without pre-reduction of Co-NW(Ag/Co-NW).In addition to high activity,Ag/Co-NW-R exhibits high catalytic stability and water resistance.The strategy used in this work might be applicable in related catalytic systems.
基金support from the National Key Research and Development Program of China(2017YFB0702800)the China Petrochemical Corporation(Sinopec Group)the National Natural Science Foundation of China(91434102 and U1663221)。
文摘Dry reforming of ethane(DRE)has received significant attention because of its potential to produce chemical raw materials and reduce carbon emissions.Herein,a composition-induced strong metal-support interaction(SMSI)effect over FeNi/Al-Ce-O catalysts is revealed via X-ray photoelectron spectroscopy(XPS),H_(2)-temperature programmed reduction(TPR),and energy dispersive X-ray spectroscopy(EDS)elemental mapping.The introduction of Al into Al-Ce-O supports significantly influences the dispersion of surface active components and improves the catalytic performance for DRE over supported FeNi catalysts due to enhancement of the SMSI effect.The catalytic properties,for example,C_(2)H_(6) and CO_(2) conversion,CO selectivity and yield,and turnover frequencies(TOFs),of supported FeNi catalysts first increase and then decrease with increasing Al content,following the same trend as the theoretical effective surface area(TESA)of the corresponding catalysts.The FeNi/Ce-Al_(0.5) catalyst,with 50%Al content,exhibits the best DRE performance under steady-state conditions at 873 K.As observed by with in situ Fourier transform infrared spectroscopy(FTIR)analysis,the introduction of Al not only increases the content of surface Ce3+and oxygen vacancies but also promotes the dispersion of surface active components,which further alters the catalytic properties for DRE over supported FeNi catalysts.
基金sponsored by the National Key R&D Program of China(2021YFA1501100)the National Natural Science Foundation of China(21832001 and 22293042)the Beijing National Laboratory for Molecular Sciences(BNLMS-CXXM-202104)。
文摘The modulation of metal-support interfacial interaction is significant but challenging in the design of high-efficiency and high-stability supported catalysts.Here,we report a synthetic strategy to upgrade Cu-CeO_(2)interfacial interaction by the pyrolysis of mixed metal-organic framework(MOF)structure.The obtained highly dispersed Cu/CeO_(2)-MOF catalyst via this strategy was used to catalyze water-gas shift reaction(WGSR),which exhibited high activity of 40.5μmolCOgcat^(-1).s^(-1)at 300℃and high stability of about 120 h.Based on comprehensive studies of electronic structure,pyrolysis strategy has significant effect on enhancing metal-support interaction and then stabilizing interfacial Cu^(+)species under reaction conditions.Abundant Cu^(+)species and generated oxygen vacancies over Cu/CeO_(2)-MOF catalyst played a key role in CO molecule activation and H2O molecule dissociation,respectively.Both collaborated closely and then promoted WGSR catalytic performance in comparison with traditio nal supported catalysts.This study shall offer a robust approach to harvest highly dispersed catalysts with finely-tuned metal-support interactions for stabilizing the most interfacial active metal species in diverse heterogeneous catalytic reactions.
基金the National Key Research and Development Program of China(2023YFA1507400)the National Natural Science Foundation of China(22102192,22279146,22033009,22293015,22121002)+2 种基金the CAS Project for Young Scientists in Basic Research(YSBR-050)the Photon Science Center for Carbon Neutralitythe S&T Program of Hebei(B2021208074)for the support。
文摘Oxidized copper(Cu)species have shown significant promise for electrocatalytic CO_(2)reduction reaction(CO_(2)RR),but they are hard to retain for longterm operation at negative potential.Herein,we developed a substrate-anchored thermal annealing strategy to synthesize a CuO/MgO catalyst for CO_(2)RR to CH_(4)with a Faradaic efficiency(FE)of 82.3%and a current density as high as 568.2 mA cm^(-2)at-1.0 V vs.reversible hydrogen electrode.This catalyst also demonstrates exceptional electrocatalytic durability and stability under industrially relevant conditions.In the membrane electrode assembly,the catalyst exhibited a CH_(4)FE of~70%at a current density of 500 mA cm^(-2),along with excellent stability,maintaining operation for 65 h at a cell voltage of~3.6 V.Detailed in-situ characterizations and theoretical calculations confirm that the strong electronic metal-support interactions between CuO clusters and MgO support not only stabilize the Cu^(2+)sites but also optimize the adsorption energies of the key intermediates to promote the CH_(4)pathway.Our insights guide the design of efficient and durable electrocatalyst for CO_(2)methanation.
基金the financial support provided by the National Natural Science Foundation of China (Nos.22072164,22472180,22002173)Energy Revolution S&T Program of Yulin Innovation Institute of Clean Energy (No.E411030705)+2 种基金Natural Science Foundation of Liaoning Province (No.2022-MS004)China Postdoctoral Science Foundation (No.2020M680999)the Research Fund of Shenyang National Laboratory for Materials Science。
文摘Metal-support interaction(MSI) is crucial for fine-tuning the active-site structure of supported catalysts and enhancing performance.Here,we present an ammonia-directed reactive gas-metal-support interaction(RGMSI),in which NH_(3) reduces ZnO and assembles an anti-perovskite Ni_(3)ZnN structure with interstitial nitrogen,significantly boosting hydrogenation efficiency.Nitrogen incorporation expands the lattice parameter,increasing the(111) lattice spacing from 2.04Å in Ni to 2.18Å in Ni_(3)ZnN,with an extended Ni-Ni interatomic distance from 2.49Å to 2.65Å.Additionally,Ni-N coordination shifts the d-band center downward and induces electron deficiency in Ni via charge transfer.These modifications optimize reactant adsorption on the tailored Ni_(3)ZnN structure compared to Ni,leading to a remarkable increase in 1,3-butadiene hydrogenation selectivity from 30.0 % to 92.9 %,along with an enhanced TOF from 0.067 s^(-1) to 0.079 s^(-1).These findings highlight RGMSI as a versatile and effective strategy for designing supported metal catalysts,offering new insights into selective hydrogenation catalysis.
基金supported by the National Natural Science Foundation of China(No.12372233)the Innovation Foundation for Doctor Dissertation of Northwestern Polytechnical University,China(No.25GH01020005)the“111 Project”of China(No.B17037)。
文摘As a multidisciplinary phenomenon,panel aeroelasticity in shock-dominated flow is featured by two primary interactions:Fluid-Structure Interactions(FSIs)and Shock-Boundary Layer Interactions(SBLIs).The former raises structural concerns,and the latter is of aerodynamic interest.Thus,panel aeroelasticity in shock-dominated flow represents a vital topic for the development and optimization of supersonic vehicles and propulsion systems.This review systematically summarizes recent advances in the methodologies applied to capture structural and fluid dynamics,including theoretical models,numerical simulations,and wind tunnel experiments.The application of data-driven modal decomposition,an advanced technique to extract physically crucial features,on the topic is introduced.From the perspective of FSIs,the distinctive aeroelastic behaviors in shock-dominated flow,including hysteresis phenomena and nonlinear responses,are highlighted.From the perspective of SBLIs,the modifications in their spatial and temporal characteristics imposed by the aeroelastic responses are emphasized.Motivated by the interaction between the shock waves and structural response,different strategies have been proposed to implement aeroelastic suppression and shock control,which have the potential to enhance structural safety and aerodynamic performance in the next generation of high-speed flight vehicles.
基金sponsored by the National Natural Science Foundation of China(Grant Nos.U2442206,42205067,and 41922035)the National Key R&D Program of China(Grant No.2024YFC3013100)the Key Research Program of Frontier Sciences of CAS(Grant No.QYZDB-SSW-DQC017).
文摘This study reveals the critical role of multiscale interaction within the westerly wind bursts(WWBs)west of the MJO convection in modulating the prediction skill for the November MJO event during the DYNAMO(Dynamics of the Madden–Julian Oscillation)field campaign.The characteristics of the MJO convection envelope are obtained by the largescale precipitation tracking method,and a novel metric is introduced to quantify the prediction skill for the MJO convection in the ECMWF reforecast.The ECMWF forecast exhibits approximately 17 days in skillful prediction for the MJO convection—significantly lower than that derived from the global measure.The reforecast ensembles are further classified into high and low skill catalogs based on the mean prediction skill during the observed WWBs period.High-skill ensembles exhibit significantly enhanced low-level westerlies,amplified MJO convection,and reduced spatial separation between the low-level westerlies and MJO convection during the WWBs period,indicating stronger coupling between the large-scale circulation and the convection.Mechanistic analysis reveals that enhanced westerlies in high-skill ensembles can transfer more high-frequency energy to the MJO convection through the flux convergence of interaction energy for MJO convection development,resulting in better prediction skill.
基金supported by the National Key Research and Development Program of China(Grant No.2023YFF0807000)supported by the National Natural Science Foundation of China(Grant Nos.42305004,42175073 and 42175013)supported partly by the China Postdoctoral Science Foundation(Grant No.2023M743283).
文摘Using observational and reanalysis datasets,this study explores the mechanisms by which the interactions among multi-timescale flows impacted the onset of rapid intensification(RI)of Typhoon Hato(2017).Hato(2017)formed within a northwest–southeast-oriented synoptic-scale(with periods<10 days)wave train,concurring with a developing intraseasonal(10–90 days)oscillation and an elongated low-frequency(>90 days)monsoon trough in the western North Pacific.Impacted by continuously increasing vertical wind shear,the TC long maintained a highly asymmetric convective structure.Prior to RI onset,the synoptic-scale circulation and the inner-core asymmetric convection of Hato(2017)greatly strengthened,which are the key factors believed to trigger RI.A multi-timescale eddy kinetic energy budget indicates that the wind convergence associated with the intraseasonal circulation and monsoon trough led to barotropic energy conversion that largely enhanced the synoptic-scale cyclonic circulation.Besides,the pronounced increases in midlevel relative humidity(RH)and surface latent heat flux(LHF)were observed upshear before RI onset,which were primarily driven by the strong intraseasonal and synoptic-scale RH anomalies and the strengthened low-level wind speed,respectively.The increased LHF and midlevel RH,together with the enhanced downshear confluence between synoptic-scale and Intraseasonal Oscillation(ISO)/low-frequency winds,could have helped the intensification of asymmetric convection that supports RI onset.Overall,this study suggests that the interactions across multiple timescales may create favorable dynamic and thermodynamic conditions that promoted RI onset,offering new insights into RI processes for highly asymmetric tropical cyclones like Hato(2017).
基金supported by the National Natural Science Foundation of China(32270673 and 32470657).
文摘Existing quantitative trait locus(QTL)mapping had low efficiency in identifying small-effect and closely linked QTL-by-environment interactions(QEIs)in recombinant inbred lines(RILs),especially in the era of global climate change.To address this challenge,here we integrate the compressed variance component mixed model with our GCIM to propose 3vGCIM for identifying QEIs in RILs,and extend 3vGCIM-random to 3vGCIM-fixed.3vGCIM integrates genome-wide scanning with machine learning,significantly improving power.In the mixed full model,we consider all possible effects and control for all possible polygenic backgrounds.In simulation studies,3vGCIM exhibits higher power(∼92.00%),higher accuracy of the estimates for QTL position(∼1.900 cM2)and effect(∼0.050),and lower false positive rate(∼0.48‰)and false negative rate(<8.10%)in three environments of 300 RILs each than ICIM(47.57%;3.607 cM2,0.583;2.81‰;52.43%)and MCIM(60.30%;5.279 cM2,0.274;2.17‰;39.70%).In the real data analysis of rice yield-related traits in 240 RILs,3vGCIM mines more known genes(57–60)and known gene-by-environment interactions(GEIs)(14–19)and candidate GEIs(21–23)than ICIM(27,2,and 7),and MCIM(21,1,and 3),especially in small-effect and linked QTLs and QEIs.This makes 3vGCIM a powerful and sensitive tool for QTL mapping and molecular QTL mapping.
基金Financial support from the National Natural Science Foundation of China(32502106)One health Interdisciplinary Research Project,Institute of One Health Science,Ningbo University(NBUOH202502)the Ningbo Top Talent Project(215-432094250).
文摘The antioxidant activity of selenium-containing soybean peptides(SePPs)has been previously demonstrated,despite their limited absorption in the small intestine.This study investigates the antioxidant mechanism of a selenium-containing tetrapeptide,Ser-Phe-Gln-SeM(SFQSeM),identified from SePPs,with particular emphasis on its interaction with the intestinal microbiota and its role in modulating host antioxidant defenses.The effects of SFQSeM were evaluated in a D-galactose-induced oxidative stress model and an antibiotictreated mouse model.SFQSeM supplementation significantly reduced the oxidative stress in D-galactosetreated mice.It also promoted the growth of beneficial bacteria and increased the levels of acetate,butyrate and lactate in the intestine(P<0.05).In the antibiotic-treated mouse model,depletion of the intestinal microbiota significantly reduced hepatic glutathione peroxidase(GSH-Px)activity(26.6%)and glutathione peroxidase 1(GPx-1)expression(48.77%)compared to normal mice supplemented with SFQSeM(P<0.05).In contrast to Na_(2)SeO_(3)and selenomethionine,SFQSeM effectively restored the diversity of the intestinal microbiota disrupted by antibiotics.Lactobacillus,Lachnospiraceae_NK4A136_group,and Muribaculaceae were identified as predominant bacteria in the SFQSeM group,and were strongly associated with increased hepatic GSH-Px activity and GPx-1 mRNA expression(P<0.05).In conclusion,intestinal microbiota enhances the antioxidant efficacy of SFQSeM by modulating microbial composition,producing active metabolites,and converting SFQSeM into a bioactive form of selenium.
