Compared to reforming reactions using hydrocarbons,ethanol steam reforming(ESR)is a sustainable alternative for hydrogen(H_(2))production since ethanol can be produced sustainably using biomass.This work explores the ...Compared to reforming reactions using hydrocarbons,ethanol steam reforming(ESR)is a sustainable alternative for hydrogen(H_(2))production since ethanol can be produced sustainably using biomass.This work explores the catalyst design strategies for preparing the Ni supported on ZSM-5 zeolite catalysts to promote ESR.Specifically,two-dimensional ZSM-5 nanosheet and conventional ZSM-5 crystal were used as the catalyst carriers and two synthesis strategies,i.e.,in situ encapsulation and wet impregnation method,were employed to prepare the catalysts.Based on the comparative characterization of the catalysts and comparative catalytic assessments,it was found that the combination of the in situ encapsulation synthesis and the ZSM-5 nanosheet carrier was the effective strategy to develop catalysts for promoting H_(2) production via ESR due to the improved mass transfer(through the 2-D structure of ZSM-5 nanosheet)and formation of confined small Ni nanoparticles(resulted via the in situ encapsulation synthesis).In addition,the resulting ZSM-5 nanosheet supported Ni catalyst also showed high Ni dispersion and high accessibility to Ni sites by the reactants,being able to improve the activity and stability of catalysts and suppress metal sintering and coking during ESR at high reaction temperatures.Thus,the Ni supported on ZSM-5 nanosheet catalyst prepared by encapsulation showed the stable performance with~88% ethanol conversion and~65% H_(2) yield achieved during a 48-h longevity test at 550-C.展开更多
The endochondral ossification of hindlimb is essential to a bird’s ability to stand,walk and fly.Most hindlimb is ossified in the embryos before hatching in precocial birds.However,the molecular mechanisms of hindlim...The endochondral ossification of hindlimb is essential to a bird’s ability to stand,walk and fly.Most hindlimb is ossified in the embryos before hatching in precocial birds.However,the molecular mechanisms of hindlimb ossification in birds is still unclear.Therefore,we tried to examine the process of hindlimb ossification and its molecular regulation by using an animal model—Japanese Quail(Coturnix japonica).We selected four critical stages(Embryo Day:E6,E8,E12 and E16) of skeletal development of embryonic quails for hindlimb skeleton staining to show the process of endochondral ossification and to examine the molecular regulation of endochondral osteogenesis by RNA-Seq analysis.The results showed that ossification became increased with embryonic development and most hindlimb was ossified before hatching.RNA-Seq analysis revealed that various signaling pathways were involved with endochondral ossification with thyroid hormone signaling and WNT signaling pathway particularly enriched.Moreover,the expression levels of 42 genes were continuously upregulated and 14 genes were continuously downregulated from E6 to E16.The present study might provide new insights into complex molecular mechanisms in regulation of endochondral ossification.展开更多
Since the catalytic activity of most nanozymes is still far lower than the corresponding natural enzymes,there is urgent need to discover novel highly efficient enzyme-like materials.In this work,Co_(3)V_(2)O_(8)with ...Since the catalytic activity of most nanozymes is still far lower than the corresponding natural enzymes,there is urgent need to discover novel highly efficient enzyme-like materials.In this work,Co_(3)V_(2)O_(8)with hollow hexagonal prismatic pencil structures were prepared as novel artificial enzyme mimics.They were then decorated by photo-depositing Ag nanoparticles(Ag NPs)on the surface to further improve its catalytic activities.The Ag NPs decorated Co_(3)V_(2)O_(8)(ACVPs)showed both excellent oxidase-and peroxidase-like catalytic activities.They can oxidize the colorless 3,3’,5,5’-tetramethylbenzidine rapidly to induce a blue change.The enhanced enzyme mimetic activities can be attributed to the surface plasma resonance(SPR)effect of Ag NPs as well as the synergistic catalytic effect between Ag NPs and Co_(3)V_(2)O_(8),accelerating electron transfer and promoting the catalytic process.ACVPs were applied in constructing a colorimetric sensor,validating the occurrence of the Fenton reaction,and disinfection,presenting favorable catalytic performance.The enzyme-like catalytic mechanism was studied,indicating the chief role of⋅O_(2)-radicals in the catalytic process.This work not only discovers a novel functional material with double enzyme mimetic activity but also provides a new insight into exploiting artificial enzyme mimics with highly efficient catalytic ability.展开更多
SEMA7A belongs to the Semaphorin family and is involved in the oncogenesis and tumor progression.Aberrant glycosylation has been intricately linked with immune escape and tumor growth.SEMA7A is a highly glycosylated p...SEMA7A belongs to the Semaphorin family and is involved in the oncogenesis and tumor progression.Aberrant glycosylation has been intricately linked with immune escape and tumor growth.SEMA7A is a highly glycosylated protein with five glycosylated sites.The underlying mechanisms of SEMA7A glycosylation and its contribution to immunosuppression and tumorigenesis are unclear.Here,we identify overexpression and aberrant N-glycosylation of SEMA7A in head and neck squamous cell carcinoma,and elucidate fucosyltransferase FUT8 catalyzes aberrant core fucosylation in SEMA7A at N-linked oligosaccharides(Asn 105,157,258,330,and 602)via a direct protein‒protein interaction.A glycosylated statue of SEMA7A is necessary for its intra-cellular trafficking from the cytoplasm to the cytomembrane.Cytokine EGF triggers SEMA7A N-glycosylation through increasing the binding affinity of SEMA7A toward FUT8,whereas TGF-β1 promotes abnormal glycosylation of SEMA7A via induction of epithelial–mesenchymal transition.Aberrant N-glycosylation of SEMA7A leads to the differentiation of CD8^(+)T cells along a trajectory toward an exhausted state,thus shaping an immunosuppressive microenvironment and being resistant immunogenic cell death.Deglycosylation of SEMA7A significantly improves the clinical outcome of EGFR-targeted and anti-PD-L1-based immunotherapy.Finally,we also define RBM4,a splice regulator,as a downstream effector of glycosylated SEMA7A and a pivotal mediator of PD-L1 alternative splicing.These findings suggest that targeting FUT8-SEMA7A axis might be a promising strategy for improving antitumor responses in head and neck squamous cell carcinoma patients.展开更多
The application of Mg-based electrochemical energy storage materials in high performance supercapacitors is an essential step to promote the exploitation and utilization of magnesium resources in the field of energy s...The application of Mg-based electrochemical energy storage materials in high performance supercapacitors is an essential step to promote the exploitation and utilization of magnesium resources in the field of energy storage.Unfortunately,the inherent chemical properties of magnesium lead to poor cycling stability and electrochemical reactivity,which seriously limit the application of Mg-based materials in supercapacitors.Herein,in this review,more than 70 research papers published in recent 10 years were collected and analyzed.Some representative research works were selected,and the results of various regulative strategies to improve the electrochemical performance of Mg-based materials were discussed.The effects of various regulative strategies(such as constructing nanostructures,synthesizing composites,defect engineering,and binder-free synthesis,etc.)on the electrochemical performance and their mechanism are demonstrated using spinelstructured MgX_(2)O_(4) and layered structured Mg-X-LDHs as examples.In addition,the application of magnesium oxide and magnesium hydroxide in electrode materials,MXene's solid spacers and hard templates are introduced.Finally,the challenges and outlooks of Mg-based electrochemical energy storage materials in high performance supercapacitors are also discussed.展开更多
Integration of digital twin(DT)and wireless channel provides new solution of channel modeling and simulation,and can assist to design,optimize and evaluate intelligent wireless communication system and networks.With D...Integration of digital twin(DT)and wireless channel provides new solution of channel modeling and simulation,and can assist to design,optimize and evaluate intelligent wireless communication system and networks.With DT channel modeling,the generated channel data can be closer to realistic channel measurements without requiring a prior channel model,and amount of channel data can be significantly increased.Artificial intelligence(AI)based modeling approach shows outstanding performance to solve such problems.In this work,a channel modeling method based on generative adversarial networks is proposed for DT channel,which can generate identical statistical distribution with measured channel.Model validation is conducted by comparing DT channel characteristics with measurements,and results show that DT channel leads to fairly good agreement with measured channel.Finally,a link-layer simulation is implemented based on DT channel.It is found that the proposed DT channel model can be well used to conduct link-layer simulation and its performance is comparable to using measurement data.The observations and results can facilitate the development of DT channel modeling and provide new thoughts for DT channel applications,as well as improving the performance and reliability of intelligent communication networking.展开更多
Since the discovery of mesoporous silica in 1990s,there have been numerous mesoporous silica-based nanomaterials developed for catalytic applications,aiming at enhanced catalytic activity and stability.Recently,there ...Since the discovery of mesoporous silica in 1990s,there have been numerous mesoporous silica-based nanomaterials developed for catalytic applications,aiming at enhanced catalytic activity and stability.Recently,there have also been considerable interests in endowing them with hierarchical porosities to overcome the diffusional limitation for those with long unimodal channels.Present processes of making mesoporous silica largely rely on chemical sources which are relatively expensive and impose environmental concerns on their processes.In this regard,it is desirable to develop hierarchical silica supports from natural minerals.Herein,we present a series of work on surface reconstruction,modification,and functionalization to produce diatomite-based catalysts with original morphology and macro-meso-micro porosities and to test their suitability as catalyst supports for both liquid-and gas-phase reactions.Two wet-chemical routes were developed to introduce mesoporosity to both amorphous and crystalline diatomites.Importantly,we have used computational modeling to affirm that the diatomite morphology can improve catalytic performance based on fluid dynamics simulations.Thus,one could obtain this type of catalysts from numerous natural diatoms that have inherently intricate morphologies and shapes in micrometer scale.In principle,such catalytic nanocomposites acting as miniaturized industrial catalysts could be employed in microfluidic reactors for process intensification.展开更多
Characteristics of raindrop size distribution during summer are studied by using the data from six Parsivel disdrometers located in the northeastern Tibetan Plateau.The analysis focuses on convective and stratiform pr...Characteristics of raindrop size distribution during summer are studied by using the data from six Parsivel disdrometers located in the northeastern Tibetan Plateau.The analysis focuses on convective and stratiform precipitation at high altitudes from 2434 m to 4202 m.The results show that the contribution of stratiform and convective precipitation with rain rate between 1≤R<5 mm h^(-1) to the total precipitation increases with altitude,and the raindrop scale and number concentration of convective precipitation is larger than that for stratiform precipitation.The droplet size spectra of both stratiform and convective precipitation shows a single peak with a peak particle size between 0.31–0.50 mm,and they have essentially the same peak particle size and number concentration at the same altitude.The maximum spectral widths of stratiform clouds are between 4 mm and 5 mm,while those of convective clouds range from 4 mm to 8 mm.The Gamma distribution is more suitable than the Marshall-Palmer distribution in terms of the actual raindrop spectrum distribution.The stratiform precipitation particles are smaller with higher number concentration,while the opposite is true for the convective precipitation particles.The convective precipitation particles drop faster than stratiform precipitation particles when the particle size exceeds 2 mm,and the falling velocity of raindrops after standard curve fitting is underestimated during the observation period.Moreover,conventional radar estimation methods would underestimate the precipitation in the Northeastern Tibetan Plateau.展开更多
A hierarchical superhydrophobic Al-Li layered double hydroxide(LDH)films with different Li^(+)/Al^(3+)molar ratios of 1:1,1:2,2:1,p H value of 11.5 and reaction temperature of 125°C,have been fabricated on the su...A hierarchical superhydrophobic Al-Li layered double hydroxide(LDH)films with different Li^(+)/Al^(3+)molar ratios of 1:1,1:2,2:1,p H value of 11.5 and reaction temperature of 125°C,have been fabricated on the surface of Mg-5Li-1Al(LA51)alloys by hydrothermal method following the characteristics of controllable cation structure and exchangeable anion between layers.The properties of the films were investigated by X-ray diffractometer(XRD),scanning electron microscope(SEM)and energy dispersive spectrometer(EDS).XRD and SEM results indicate that the Al-Li LDH films are successfully prepared on LA51 alloys.The contact angle(CA)was measured to be about100.7°,indicating that the surface wettability of the film converted from hydrophilic to hydrophobic by surface modification.The corrosion resistance of Al-Li LDH films was evaluated by Tafel polarization curve and electrochemical impedance spectroscopy(EIS).Surprisingly,Tafel polarization curve and EIS test reveal that the Al-Li LDH films prepared at the molar ratio of Li^(+)/Al^(3+)1:2,p H 11.5 and temperature125°C have better corrosion resistance in 0.1 M Na Cl neutral solution.In addition,the formation mechanism and corrosion mechanism of the films on the surface of LA51 alloy are also proposed.It provides innovative synthetic materials and novel design ideas for the preparation of high-efficiency anti-corrosion coatings on LA51 alloys,whose application can be extended in industrial fields.展开更多
Pure Zn coatings easily lose their protective performance after biofouling because they have no antibacterial effect under visible light.In this study,we fabricate a new antibacterial Zn composite coating using electr...Pure Zn coatings easily lose their protective performance after biofouling because they have no antibacterial effect under visible light.In this study,we fabricate a new antibacterial Zn composite coating using electrodeposition to couple Fe3+-doped alkalized g-C_(3)N_(4)(AKCN-Fe)into an existing Zn coating and show that the AKCN-Fe enhances antibacterial property of the Zn coating under visible light.We attribute this enhancement to the high photocatalytic performance,high loading content,and good dispersion of AKCN-Fe.In addition,the photocatalytic antibacterial mechanism of the composite coating is supported by scavenger experiments and electron paramagnetic resonance(EPR)measurements,suggesting that superoxide(·O_(2)^(-))and hydroxyl radical(·OH)play main and secondary roles,respectively.展开更多
With the development of human society and the depletion of non-renewable energy sources,alternate energy resources are becoming an urgent demand.In recent years,energy storage and conversion devices have drawn wide at...With the development of human society and the depletion of non-renewable energy sources,alternate energy resources are becoming an urgent demand.In recent years,energy storage and conversion devices have drawn wide attention as a bridge between sustainable energy sources and daily life.展开更多
Magnesium alloys,the advanced lightweight structural materials,have been successfully applied in the manufacturing field.Unfortunately,their poor corrosion resistance restrains the potential wide applications.In this ...Magnesium alloys,the advanced lightweight structural materials,have been successfully applied in the manufacturing field.Unfortunately,their poor corrosion resistance restrains the potential wide applications.In this work,anti-corrosion coatings were fabricated via the insitu growth of the corrosion inhibitors intercalated magnesium-aluminum layered double hydroxide(Mg-Al LDH)on AZ31 magnesium alloy and then post-sealing it by a super-hydrophobic coating.SEM,XRD,EDS,FTIR,XPS and contact angle test were conducted to analyze physical/chemical features of these coatings.Potentiodynamic polarization curves and electrochemical impedance spectroscopy were recorded to assess the anti-corrosion performance of prepared coatings.Surprisingly,Mg-Al LDH with molybdate intercalation and lauric acid modification achieves the excellent corrosion inhibition performance(99.99%)due to the multicomponent synergistic effect such as the physical protection of Mg-Al LDH,the corrosion inhibition of molybdate and super-hydrophobic properties of lauric acid.This work presents a scientific perspective and novel design philosophy to fabricate the efficient anti-corrosion coating to protect magnesium alloys and then expand their potential applications in other field.展开更多
A one-step electrodeposition method was used to construct a superhydrophobic coating on the surface of magnesium alloy.Using magne-sium nitrate and ethanol solution of stearic acid as electrolyte,four groups of electr...A one-step electrodeposition method was used to construct a superhydrophobic coating on the surface of magnesium alloy.Using magne-sium nitrate and ethanol solution of stearic acid as electrolyte,four groups of electrolytes with different ratios of stearic acid and magnesium nitrate were designed to explore the influence of electrolyte to the process.The contact angles of the four coating samples were 136.4±5.8°,152.7±2.8°,156.2±4.9°and 155.1±4.4°The addition of magnesium nitrate in the solution increased the hydrogen evolution reaction in the electrodeposition process,which was not conducive to electrodeposition process.During the deposition process,the sample prepared in a molar ratio of stearic acid to magnesium nitrate of 10:1 had the best corrosion resistance,and its corrosion circuit density was 3.74×10^(−8)A/cm^(2),far lower than the corrosion current density of the magnesium alloy substrate.展开更多
Surface plasmon resonance(SPR)of metals may provide a way to improve light absorption and utilization of semiconductors,achieving better solar light conversion and photocatalysis efficiency.This study uses the advanta...Surface plasmon resonance(SPR)of metals may provide a way to improve light absorption and utilization of semiconductors,achieving better solar light conversion and photocatalysis efficiency.This study uses the advantages of SPR in metallic Bi and artificial defects to cooperatively enhance the photocatalytic performance of BiOI.The catalysts were prepared by partial reduction of BiOI to form Bi@defective BiOI,which showed highly enhanced visible photocatalytic activity for NOx removal.The effects of reductant quantity on the photocatalytic performance of Bi@defective BiOI were investigated.The as-prepared photocatalyst(Bi/BiOI-2)using 2 mmol of reductant NaBH4 showed the most efficient visible light photocatalytic activity.This enhanced activity can be ascribed to the synergistic effects of metallic Bi and oxygen vacancies.The electrons from the valence band tend to accumulate at vacancy states;therefore,the increased charge density would cause the adsorbed oxygen to transform more easily into superoxide radicals and,further,into hydroxyl radicals.These radicals are the main active species that oxidize NO into final products.The SPR effect of elemental Bi enables the improvement of visible light absorption efficiency and the promotion of charge carrier separation,which are crucial factors in boosting photocatalysis.NO adsorption and reaction processes on Bi/BiOI-2 were dynamically monitored by in situ infrared spectroscopy(FT-IR).The Bi/BiOI photocatalysis mechanism co-mediated by elemental Bi and oxygen vacancies was proposed based on the analysis of intermediate products and DFT calculations.This present work could provide new insights into the design of high-performance photocatalysts and understanding of the photocatalysis reaction mechanism for air-purification applications.展开更多
Conservation of endangered or economic fish and control of invasive fish is a great challenge of hydraulic engineering worldwide.Flow velocity has been recognized to affect the spawning of fishes delivering drifting e...Conservation of endangered or economic fish and control of invasive fish is a great challenge of hydraulic engineering worldwide.Flow velocity has been recognized to affect the spawning of fishes delivering drifting eggs in rivers.However,solid scientific supports and associated mechanisms to establish quantitative relations between flow velocity and fish reproduction,taking into account spawning,fertilizing,hatching,as well as surviving,are lacking.In this paper,we quantified the relationship between flow velocity and reproduction of Chinese carps through both lab and field experiments.The results showed that a minimum velocity was required to trigger Hypophthalmichthys molitrix(H.molitrix)releasing eggs,and a velocity range was preferred to sustain spawning activity.However,the embryo incubation and larvae development of H.molitrix were found to be inhibited with the increase in flow velocity.Considering the requirements of spawning and hatching,as well as larvae surviving,an optimized flow velocity processes was identified for the reproduction of H.molitrix in rivers.These findings were of great significance to the adaptive operation of reservoirs to create reasonable and precise ecological flows for managing fish reproduction,as shown by the promising results in the engineering application to the Three Gorges Reservoir.展开更多
There is an increasing interest in bismuth carbonate(Bi2O2CO3,BOC)as a semiconductor photocatalyst.However,pure BOC strongly absorbs ultraviolet light,which drives a high recombination rate of charge carriers and ther...There is an increasing interest in bismuth carbonate(Bi2O2CO3,BOC)as a semiconductor photocatalyst.However,pure BOC strongly absorbs ultraviolet light,which drives a high recombination rate of charge carriers and thereby limits the overall photocatalysis efficiency.In this work,artificial oxygen vacancies(OV)were introduced into BOC(OV-BOC)to broaden the optical absorption range,increase the charge separation efficiency,and activate the reactants.The photocatalytic removal ratio of NO was increased significantly from 10.0%for pure BOC to 50.2%for OV-BOC because of the multiple roles played by the oxygen vacancies.These results imply that oxygen vacancies can facilitate the electron exchange between intermediates and the surface oxygen vacancies in OV-BOC,making them more easily destroyed by active radicals.In situ DRIFTS spectra in combination with electron spin resonance spectra and density functional theory calculations enabled unraveling of the conversion pathway for the photocatalytic NO oxidation on OV-BOC.It was found that oxygen vacancies could increase the production of active radicals and promote the transformation of NO into target products instead of toxic byproducts(NO2),thus the selectivity is significantly enhanced.This work provides a new strategy for enhancing photocatalytic activity and selectivity.展开更多
基金funding from the European Union's Horizon 2020 Research and Innovation Program(872102)P.S.thanks the Science Achievement Scholarship of Thailand(SAST)for her research secondment at The University of Manchester.Y.J.thanks the National Natural Science Foundation of China(22378407)for funding.
文摘Compared to reforming reactions using hydrocarbons,ethanol steam reforming(ESR)is a sustainable alternative for hydrogen(H_(2))production since ethanol can be produced sustainably using biomass.This work explores the catalyst design strategies for preparing the Ni supported on ZSM-5 zeolite catalysts to promote ESR.Specifically,two-dimensional ZSM-5 nanosheet and conventional ZSM-5 crystal were used as the catalyst carriers and two synthesis strategies,i.e.,in situ encapsulation and wet impregnation method,were employed to prepare the catalysts.Based on the comparative characterization of the catalysts and comparative catalytic assessments,it was found that the combination of the in situ encapsulation synthesis and the ZSM-5 nanosheet carrier was the effective strategy to develop catalysts for promoting H_(2) production via ESR due to the improved mass transfer(through the 2-D structure of ZSM-5 nanosheet)and formation of confined small Ni nanoparticles(resulted via the in situ encapsulation synthesis).In addition,the resulting ZSM-5 nanosheet supported Ni catalyst also showed high Ni dispersion and high accessibility to Ni sites by the reactants,being able to improve the activity and stability of catalysts and suppress metal sintering and coking during ESR at high reaction temperatures.Thus,the Ni supported on ZSM-5 nanosheet catalyst prepared by encapsulation showed the stable performance with~88% ethanol conversion and~65% H_(2) yield achieved during a 48-h longevity test at 550-C.
基金supported by the National Natural Science Foundationof China (No. 33372201)。
文摘The endochondral ossification of hindlimb is essential to a bird’s ability to stand,walk and fly.Most hindlimb is ossified in the embryos before hatching in precocial birds.However,the molecular mechanisms of hindlimb ossification in birds is still unclear.Therefore,we tried to examine the process of hindlimb ossification and its molecular regulation by using an animal model—Japanese Quail(Coturnix japonica).We selected four critical stages(Embryo Day:E6,E8,E12 and E16) of skeletal development of embryonic quails for hindlimb skeleton staining to show the process of endochondral ossification and to examine the molecular regulation of endochondral osteogenesis by RNA-Seq analysis.The results showed that ossification became increased with embryonic development and most hindlimb was ossified before hatching.RNA-Seq analysis revealed that various signaling pathways were involved with endochondral ossification with thyroid hormone signaling and WNT signaling pathway particularly enriched.Moreover,the expression levels of 42 genes were continuously upregulated and 14 genes were continuously downregulated from E6 to E16.The present study might provide new insights into complex molecular mechanisms in regulation of endochondral ossification.
基金supported by National Natural Science Foundation of China(52208272,41706080 and 51702328)the Basic Scientific Fund for National Public Research Institutes of China(2020S02 and 2019Y03)+3 种基金the Basic Frontier Science Research Program of Chinese Academy of Sciences(ZDBS-LY-DQC025)the Young Elite Scientists Sponsorship Program by CAST(No.YESS20210201)the Strategic Leading Science&Technology Program of the Chinese Academy of Sciences(XDA13040403)the Key Research and Development Program of Shandong Province(Major Scientific and Technological Innovation Project)(2019JZZY020711).
文摘Since the catalytic activity of most nanozymes is still far lower than the corresponding natural enzymes,there is urgent need to discover novel highly efficient enzyme-like materials.In this work,Co_(3)V_(2)O_(8)with hollow hexagonal prismatic pencil structures were prepared as novel artificial enzyme mimics.They were then decorated by photo-depositing Ag nanoparticles(Ag NPs)on the surface to further improve its catalytic activities.The Ag NPs decorated Co_(3)V_(2)O_(8)(ACVPs)showed both excellent oxidase-and peroxidase-like catalytic activities.They can oxidize the colorless 3,3’,5,5’-tetramethylbenzidine rapidly to induce a blue change.The enhanced enzyme mimetic activities can be attributed to the surface plasma resonance(SPR)effect of Ag NPs as well as the synergistic catalytic effect between Ag NPs and Co_(3)V_(2)O_(8),accelerating electron transfer and promoting the catalytic process.ACVPs were applied in constructing a colorimetric sensor,validating the occurrence of the Fenton reaction,and disinfection,presenting favorable catalytic performance.The enzyme-like catalytic mechanism was studied,indicating the chief role of⋅O_(2)-radicals in the catalytic process.This work not only discovers a novel functional material with double enzyme mimetic activity but also provides a new insight into exploiting artificial enzyme mimics with highly efficient catalytic ability.
基金supported by the National Natural Science Foundation of China(NSFC:82173451)Project of Biobank(YBKB202105)from Shanghai Ninth People’s Hospital,Shanghai Jiao Tong University School of Medicine,Shanghai Municipal Health Commission(No.2022LJ001)+1 种基金the Natural Science Foundation of Shanghai(22ZR1437600)Shanghai’s Top Priority Research Center(2022ZZ01017).
文摘SEMA7A belongs to the Semaphorin family and is involved in the oncogenesis and tumor progression.Aberrant glycosylation has been intricately linked with immune escape and tumor growth.SEMA7A is a highly glycosylated protein with five glycosylated sites.The underlying mechanisms of SEMA7A glycosylation and its contribution to immunosuppression and tumorigenesis are unclear.Here,we identify overexpression and aberrant N-glycosylation of SEMA7A in head and neck squamous cell carcinoma,and elucidate fucosyltransferase FUT8 catalyzes aberrant core fucosylation in SEMA7A at N-linked oligosaccharides(Asn 105,157,258,330,and 602)via a direct protein‒protein interaction.A glycosylated statue of SEMA7A is necessary for its intra-cellular trafficking from the cytoplasm to the cytomembrane.Cytokine EGF triggers SEMA7A N-glycosylation through increasing the binding affinity of SEMA7A toward FUT8,whereas TGF-β1 promotes abnormal glycosylation of SEMA7A via induction of epithelial–mesenchymal transition.Aberrant N-glycosylation of SEMA7A leads to the differentiation of CD8^(+)T cells along a trajectory toward an exhausted state,thus shaping an immunosuppressive microenvironment and being resistant immunogenic cell death.Deglycosylation of SEMA7A significantly improves the clinical outcome of EGFR-targeted and anti-PD-L1-based immunotherapy.Finally,we also define RBM4,a splice regulator,as a downstream effector of glycosylated SEMA7A and a pivotal mediator of PD-L1 alternative splicing.These findings suggest that targeting FUT8-SEMA7A axis might be a promising strategy for improving antitumor responses in head and neck squamous cell carcinoma patients.
基金financial support provided by Projects(no.2020CDJXZ001)the Fundamental Research Funds for the Central Universities+1 种基金the Technology Innovation and Application Development Special Project of Chongqing(Z20211350 and Z20211351)Scientific Research Project of Chongqing Ecological Environment Bureau(no.CQEE2022-STHBZZ118)。
文摘The application of Mg-based electrochemical energy storage materials in high performance supercapacitors is an essential step to promote the exploitation and utilization of magnesium resources in the field of energy storage.Unfortunately,the inherent chemical properties of magnesium lead to poor cycling stability and electrochemical reactivity,which seriously limit the application of Mg-based materials in supercapacitors.Herein,in this review,more than 70 research papers published in recent 10 years were collected and analyzed.Some representative research works were selected,and the results of various regulative strategies to improve the electrochemical performance of Mg-based materials were discussed.The effects of various regulative strategies(such as constructing nanostructures,synthesizing composites,defect engineering,and binder-free synthesis,etc.)on the electrochemical performance and their mechanism are demonstrated using spinelstructured MgX_(2)O_(4) and layered structured Mg-X-LDHs as examples.In addition,the application of magnesium oxide and magnesium hydroxide in electrode materials,MXene's solid spacers and hard templates are introduced.Finally,the challenges and outlooks of Mg-based electrochemical energy storage materials in high performance supercapacitors are also discussed.
基金supported by National Key R&D Program of China under Grant 2021YFB3901302 and 2021YFB2900301the National Natural Science Foundation of China under Grant 62271037,62001519,62221001,and U21A20445+1 种基金the State Key Laboratory of Advanced Rail Autonomous Operation under Grant RCS2022ZZ004the Fundamental Research Funds for the Central Universities under Grant 2022JBQY004.
文摘Integration of digital twin(DT)and wireless channel provides new solution of channel modeling and simulation,and can assist to design,optimize and evaluate intelligent wireless communication system and networks.With DT channel modeling,the generated channel data can be closer to realistic channel measurements without requiring a prior channel model,and amount of channel data can be significantly increased.Artificial intelligence(AI)based modeling approach shows outstanding performance to solve such problems.In this work,a channel modeling method based on generative adversarial networks is proposed for DT channel,which can generate identical statistical distribution with measured channel.Model validation is conducted by comparing DT channel characteristics with measurements,and results show that DT channel leads to fairly good agreement with measured channel.Finally,a link-layer simulation is implemented based on DT channel.It is found that the proposed DT channel model can be well used to conduct link-layer simulation and its performance is comparable to using measurement data.The observations and results can facilitate the development of DT channel modeling and provide new thoughts for DT channel applications,as well as improving the performance and reliability of intelligent communication networking.
基金the financial support provided by the National Research Foundation (NRF), Prime Minister’s Office, Singapore, under its Campus for Research Excellence and Technological Enterprise (CREATE) programpartially funded by the National University of Singapore under its Flagship Green Energy Program (GEP), Agency for Science, Technology and Research (A*STAR) under its Low Carbon Energy Research Funding Initiative (LCER-FI)Chongqing Science and Technology Research and Development Base Construction Project (cstc2013gjhz0029)
文摘Since the discovery of mesoporous silica in 1990s,there have been numerous mesoporous silica-based nanomaterials developed for catalytic applications,aiming at enhanced catalytic activity and stability.Recently,there have also been considerable interests in endowing them with hierarchical porosities to overcome the diffusional limitation for those with long unimodal channels.Present processes of making mesoporous silica largely rely on chemical sources which are relatively expensive and impose environmental concerns on their processes.In this regard,it is desirable to develop hierarchical silica supports from natural minerals.Herein,we present a series of work on surface reconstruction,modification,and functionalization to produce diatomite-based catalysts with original morphology and macro-meso-micro porosities and to test their suitability as catalyst supports for both liquid-and gas-phase reactions.Two wet-chemical routes were developed to introduce mesoporosity to both amorphous and crystalline diatomites.Importantly,we have used computational modeling to affirm that the diatomite morphology can improve catalytic performance based on fluid dynamics simulations.Thus,one could obtain this type of catalysts from numerous natural diatoms that have inherently intricate morphologies and shapes in micrometer scale.In principle,such catalytic nanocomposites acting as miniaturized industrial catalysts could be employed in microfluidic reactors for process intensification.
基金jointly sponsored by the Second Tibetan Plateau Atmospheric Sciences Experiment(STEP)(Grant No.2019QZKK010406)the National Natural Science Foundation of China(Grant No.42165008)Natural Science Foundation of Technology Department of Qinghai Province(Grant No.2021-ZJ-745)。
文摘Characteristics of raindrop size distribution during summer are studied by using the data from six Parsivel disdrometers located in the northeastern Tibetan Plateau.The analysis focuses on convective and stratiform precipitation at high altitudes from 2434 m to 4202 m.The results show that the contribution of stratiform and convective precipitation with rain rate between 1≤R<5 mm h^(-1) to the total precipitation increases with altitude,and the raindrop scale and number concentration of convective precipitation is larger than that for stratiform precipitation.The droplet size spectra of both stratiform and convective precipitation shows a single peak with a peak particle size between 0.31–0.50 mm,and they have essentially the same peak particle size and number concentration at the same altitude.The maximum spectral widths of stratiform clouds are between 4 mm and 5 mm,while those of convective clouds range from 4 mm to 8 mm.The Gamma distribution is more suitable than the Marshall-Palmer distribution in terms of the actual raindrop spectrum distribution.The stratiform precipitation particles are smaller with higher number concentration,while the opposite is true for the convective precipitation particles.The convective precipitation particles drop faster than stratiform precipitation particles when the particle size exceeds 2 mm,and the falling velocity of raindrops after standard curve fitting is underestimated during the observation period.Moreover,conventional radar estimation methods would underestimate the precipitation in the Northeastern Tibetan Plateau.
基金the financial support of the Natural Science Foundation of Inner Mongolia Autonomous Region(Grant NO.2019MS05037)Chunhui Program of Ministry of Education of China(Grant NO.CHJH2018)+5 种基金Key Technology Project of Inner Mongolia Autonomous Region(Grant NO.2021GG0094)Supported by Youth project of science and technology research program of Chongqing Education Commission of China(KJ201903136636560)provided by the National Natural Science Foundation of China(Grant No.51908092),Projects(No.2020CDJXZ001 and 2021CDJJMRH-005)the Fundamental Research Funds for the Central Universitiesthe Joint Funds of the National Natural Science Foundation of China-Guangdong(Grant No.U1801254)the project funded by Chongqing Special Postdoctoral Science Foundation(Xm T2018043)
文摘A hierarchical superhydrophobic Al-Li layered double hydroxide(LDH)films with different Li^(+)/Al^(3+)molar ratios of 1:1,1:2,2:1,p H value of 11.5 and reaction temperature of 125°C,have been fabricated on the surface of Mg-5Li-1Al(LA51)alloys by hydrothermal method following the characteristics of controllable cation structure and exchangeable anion between layers.The properties of the films were investigated by X-ray diffractometer(XRD),scanning electron microscope(SEM)and energy dispersive spectrometer(EDS).XRD and SEM results indicate that the Al-Li LDH films are successfully prepared on LA51 alloys.The contact angle(CA)was measured to be about100.7°,indicating that the surface wettability of the film converted from hydrophilic to hydrophobic by surface modification.The corrosion resistance of Al-Li LDH films was evaluated by Tafel polarization curve and electrochemical impedance spectroscopy(EIS).Surprisingly,Tafel polarization curve and EIS test reveal that the Al-Li LDH films prepared at the molar ratio of Li^(+)/Al^(3+)1:2,p H 11.5 and temperature125°C have better corrosion resistance in 0.1 M Na Cl neutral solution.In addition,the formation mechanism and corrosion mechanism of the films on the surface of LA51 alloy are also proposed.It provides innovative synthetic materials and novel design ideas for the preparation of high-efficiency anti-corrosion coatings on LA51 alloys,whose application can be extended in industrial fields.
基金financially supported by the National Natural Science Foundation of China(No.41706080)the Basic Frontier Science Research Program of the Chinese Academy of Sciences(No.ZDBS-LYDQC025)+1 种基金the Strategic Leading Science and Technology Program of the Chinese Academy of Sciences(No.XDA13040403)the Shandong Key Laboratory of Corrosion Science。
文摘Pure Zn coatings easily lose their protective performance after biofouling because they have no antibacterial effect under visible light.In this study,we fabricate a new antibacterial Zn composite coating using electrodeposition to couple Fe3+-doped alkalized g-C_(3)N_(4)(AKCN-Fe)into an existing Zn coating and show that the AKCN-Fe enhances antibacterial property of the Zn coating under visible light.We attribute this enhancement to the high photocatalytic performance,high loading content,and good dispersion of AKCN-Fe.In addition,the photocatalytic antibacterial mechanism of the composite coating is supported by scavenger experiments and electron paramagnetic resonance(EPR)measurements,suggesting that superoxide(·O_(2)^(-))and hydroxyl radical(·OH)play main and secondary roles,respectively.
文摘With the development of human society and the depletion of non-renewable energy sources,alternate energy resources are becoming an urgent demand.In recent years,energy storage and conversion devices have drawn wide attention as a bridge between sustainable energy sources and daily life.
基金This work is financially supported by the Graduate Research and Innovation of Chongqing,China(Grant No.CYB18002)the National Natural Science Foundation of China(Grant No.21576034)+2 种基金the State Education Ministry and Fundamental Research Funds for the Central Universities(2019CDQYCL042,106112017CDJXSYY0001,2018CDYJSY0055,106112017CDJQJ138802,106112017CDJSK04XK11,2018CDQYCL0027)the Joint Funds of the National Natural Science Foundation of China-Guangdong(Grant No.U1801254)Fundamental Re-search Funds for the Central Universities(NO.2018CDJDCD0001).
文摘Magnesium alloys,the advanced lightweight structural materials,have been successfully applied in the manufacturing field.Unfortunately,their poor corrosion resistance restrains the potential wide applications.In this work,anti-corrosion coatings were fabricated via the insitu growth of the corrosion inhibitors intercalated magnesium-aluminum layered double hydroxide(Mg-Al LDH)on AZ31 magnesium alloy and then post-sealing it by a super-hydrophobic coating.SEM,XRD,EDS,FTIR,XPS and contact angle test were conducted to analyze physical/chemical features of these coatings.Potentiodynamic polarization curves and electrochemical impedance spectroscopy were recorded to assess the anti-corrosion performance of prepared coatings.Surprisingly,Mg-Al LDH with molybdate intercalation and lauric acid modification achieves the excellent corrosion inhibition performance(99.99%)due to the multicomponent synergistic effect such as the physical protection of Mg-Al LDH,the corrosion inhibition of molybdate and super-hydrophobic properties of lauric acid.This work presents a scientific perspective and novel design philosophy to fabricate the efficient anti-corrosion coating to protect magnesium alloys and then expand their potential applications in other field.
基金The authors are very grateful for the support from the National Key Research and Development Program of China(No.2016YFB0301102)the Fundamental Research Funds for the Central Universities(No.2018CDGFCL0005)the Postgraduate Education Fund of Chongqing University(No.201704020).
文摘A one-step electrodeposition method was used to construct a superhydrophobic coating on the surface of magnesium alloy.Using magne-sium nitrate and ethanol solution of stearic acid as electrolyte,four groups of electrolytes with different ratios of stearic acid and magnesium nitrate were designed to explore the influence of electrolyte to the process.The contact angles of the four coating samples were 136.4±5.8°,152.7±2.8°,156.2±4.9°and 155.1±4.4°The addition of magnesium nitrate in the solution increased the hydrogen evolution reaction in the electrodeposition process,which was not conducive to electrodeposition process.During the deposition process,the sample prepared in a molar ratio of stearic acid to magnesium nitrate of 10:1 had the best corrosion resistance,and its corrosion circuit density was 3.74×10^(−8)A/cm^(2),far lower than the corrosion current density of the magnesium alloy substrate.
基金supported by the National Natural Science Foundation of China(21501016,21777011 and 21822601)the National Key R&D Program of China(2016YFC02047)+2 种基金the Innovative Research Team of Chongqing(CXTDG201602014)the Key Natural Science Foundation of Chongqing(cstc2017jcyj BX0052)the National Ten Thousand Talent Program of China~~
文摘Surface plasmon resonance(SPR)of metals may provide a way to improve light absorption and utilization of semiconductors,achieving better solar light conversion and photocatalysis efficiency.This study uses the advantages of SPR in metallic Bi and artificial defects to cooperatively enhance the photocatalytic performance of BiOI.The catalysts were prepared by partial reduction of BiOI to form Bi@defective BiOI,which showed highly enhanced visible photocatalytic activity for NOx removal.The effects of reductant quantity on the photocatalytic performance of Bi@defective BiOI were investigated.The as-prepared photocatalyst(Bi/BiOI-2)using 2 mmol of reductant NaBH4 showed the most efficient visible light photocatalytic activity.This enhanced activity can be ascribed to the synergistic effects of metallic Bi and oxygen vacancies.The electrons from the valence band tend to accumulate at vacancy states;therefore,the increased charge density would cause the adsorbed oxygen to transform more easily into superoxide radicals and,further,into hydroxyl radicals.These radicals are the main active species that oxidize NO into final products.The SPR effect of elemental Bi enables the improvement of visible light absorption efficiency and the promotion of charge carrier separation,which are crucial factors in boosting photocatalysis.NO adsorption and reaction processes on Bi/BiOI-2 were dynamically monitored by in situ infrared spectroscopy(FT-IR).The Bi/BiOI photocatalysis mechanism co-mediated by elemental Bi and oxygen vacancies was proposed based on the analysis of intermediate products and DFT calculations.This present work could provide new insights into the design of high-performance photocatalysts and understanding of the photocatalysis reaction mechanism for air-purification applications.
基金This work is supported by the National Key Research and Development Program of China(2016YFC0502205)the National Natural Science Foundation of China(51425902).
文摘Conservation of endangered or economic fish and control of invasive fish is a great challenge of hydraulic engineering worldwide.Flow velocity has been recognized to affect the spawning of fishes delivering drifting eggs in rivers.However,solid scientific supports and associated mechanisms to establish quantitative relations between flow velocity and fish reproduction,taking into account spawning,fertilizing,hatching,as well as surviving,are lacking.In this paper,we quantified the relationship between flow velocity and reproduction of Chinese carps through both lab and field experiments.The results showed that a minimum velocity was required to trigger Hypophthalmichthys molitrix(H.molitrix)releasing eggs,and a velocity range was preferred to sustain spawning activity.However,the embryo incubation and larvae development of H.molitrix were found to be inhibited with the increase in flow velocity.Considering the requirements of spawning and hatching,as well as larvae surviving,an optimized flow velocity processes was identified for the reproduction of H.molitrix in rivers.These findings were of great significance to the adaptive operation of reservoirs to create reasonable and precise ecological flows for managing fish reproduction,as shown by the promising results in the engineering application to the Three Gorges Reservoir.
基金supported by the National Key R&D Program of China(2016YFC02047)the National Natural Science Foundation of China(21822601,21777011,and 21501016)+3 种基金the Graduate Research and Innovation Foundation of Chongqing(CYS18019)the Innovative Research Team of Chongqing(CXTDG201602014)the Natural Science Foundation of Chongqing(cstc2017jcyjBX0052)the National Special Supporting National Plan for High-Level~~
文摘There is an increasing interest in bismuth carbonate(Bi2O2CO3,BOC)as a semiconductor photocatalyst.However,pure BOC strongly absorbs ultraviolet light,which drives a high recombination rate of charge carriers and thereby limits the overall photocatalysis efficiency.In this work,artificial oxygen vacancies(OV)were introduced into BOC(OV-BOC)to broaden the optical absorption range,increase the charge separation efficiency,and activate the reactants.The photocatalytic removal ratio of NO was increased significantly from 10.0%for pure BOC to 50.2%for OV-BOC because of the multiple roles played by the oxygen vacancies.These results imply that oxygen vacancies can facilitate the electron exchange between intermediates and the surface oxygen vacancies in OV-BOC,making them more easily destroyed by active radicals.In situ DRIFTS spectra in combination with electron spin resonance spectra and density functional theory calculations enabled unraveling of the conversion pathway for the photocatalytic NO oxidation on OV-BOC.It was found that oxygen vacancies could increase the production of active radicals and promote the transformation of NO into target products instead of toxic byproducts(NO2),thus the selectivity is significantly enhanced.This work provides a new strategy for enhancing photocatalytic activity and selectivity.