The jasmonic acid(JA)signaling pathway is used by plants to control wound responses.The persistent accumulation of JA inhibits plant growth,and the hydroxylation of JA to 12-hydroxy-JA by JASMONATE-INDUCED OXYGENASEs(...The jasmonic acid(JA)signaling pathway is used by plants to control wound responses.The persistent accumulation of JA inhibits plant growth,and the hydroxylation of JA to 12-hydroxy-JA by JASMONATE-INDUCED OXYGENASEs(JOXs,also named jasmonic acid oxidases)is therefore vital for plant growth,while structural details of JA recognition by JOXs are unknown.Here,we present the 2.65Åresolution X-ray crystal structure of Arabidopsis JOX2 in complex with its substrate JA and its co-substrates 2-oxoglutarate and Fe(Ⅱ).JOX2 contains a distorted double-stranded p helix(DSBH)core flanked by a helices and loops.JA is bound in the narrow substrate pocket by hydrogen bonds with the arginine triad R225,R350,and R354 and by hydrophobic interactions mainly with the phenylalanine triad F157,F317,and F346.The most critical residues for JA binding are F157 and R225,both from the DSBH core,which interact with the cyclopentane ring of JA.The spatial distribution of critical residues for JA binding and the shape of the substrate-binding pocket together define the substrate selectivity of the JOXs.Sequence alignment shows that these critical residues are conserved among JOXs from higher plants.Collectively,our study provides insights into the mechanism by which higher plants hydroxylate the hormone JA.展开更多
Efficient generation of singlet oxygen(1 O_(2)) by an excitonic ene rgy transfer process is highly desired on a semiconductor photocatalyst for selective oxidation of methyl phenyl sulfide(MPS).Herein,it is demonstrat...Efficient generation of singlet oxygen(1 O_(2)) by an excitonic ene rgy transfer process is highly desired on a semiconductor photocatalyst for selective oxidation of methyl phenyl sulfide(MPS).Herein,it is demonstrated that a large amount of 1 O_(2) is produced on pristine graphitic carbon nitride(CN) nanosheet compared with bismuth oxybromide(BiOBr) and comme rcial P25 titanium dioxide(TiO_(2)).This leads to a certain photoactivity of CN for MPS oxidation.The observed ~77% selectivity for CN depends on the competitive results of excitonic energy transfer for 1 O_(2) formation and charge carrier separation for superoxide radical(O_(2)·) production,which are based on the phosphorescence spectra and electron paramagnetic resonance signals,respectively.Moreover,ultrathin CN nanosheets are synthesized by thermal treatment with the cyanuric acid-melamine hydrogen bonded aggregates as precursors.It is confirmed that the amount of produced 1 O_(2) could be increased by decreasing the thickness of resultant CN nanosheets.The optimized ultrathin CN nanosheet(~4 nm) exhibits excellent photoactivity with high selectivity(~99%).It is suggested that the excitonic energy transfer for 1 O_(2) formation is close related to the intrinsic exciton binding energy and the two-dimensional quantum confinement effect.This work establishes a basic mechanistic understanding on the excitonic processes in CN,and develops a feasible route to design CN-based photocatalysts for efficient 1 O_(2) generation.展开更多
lmprovement of the charge separation of titanosilicate molecular sieves is critical to their use asphotocatalysts for oxidative organic transformations.In this work,MFI TS-1 molecular sievenanosheets(TS-1 NS)were synt...lmprovement of the charge separation of titanosilicate molecular sieves is critical to their use asphotocatalysts for oxidative organic transformations.In this work,MFI TS-1 molecular sievenanosheets(TS-1 NS)were synthesized by a low-temperature hydrothermal method using a tai-lored diquaternary ammonium surfactant as the structure-directing agent.Introducing Ni^2+cationsat the ion-exchange sites of the TS-1 NS framework significantly enhanced its photoactivity in aero-bic alcohol oxidation.The optimized Ni cation-functionalized TS-1 NS(Ni/TS-1 NS)provide impres-sive photoactivity,with a benzyl alcohol(BA)conversion of 78.9%and benzyl aldehyde(BAD)se-lectivity of 98.8%using O as the only oxidant under full light irradiation;this BAD yield is approx-imately six times greater than that obtained for bulk TS-1,and is maintained for five runs.The ex-cellent photoactivity of Ni/TS-1 NS is attributed to the significantly enlarged surface area of thetwo-dimensional morphology TS-1 NS,extra mesopores,and greatly improved charge separation.Compared with bulk TS-1,Ni/TS-1 NS has a much shorter charge transfer distance.Theas-introduced Ni species could capture the photoelectrons to further improve the charge separa-tion.This work opens the way to a class of highly selective,robust,and low-cost titanosilicate mo-lecular sieve-based photocatalysts with industrial potential for selective oxidative transformationsand pollutant degradation.展开更多
Air pollutant concentration is a function of emission rates and meteorology.To accurately evaluate the effect of control measures,the meteorological covariate must be corrected from the observations.This study quantif...Air pollutant concentration is a function of emission rates and meteorology.To accurately evaluate the effect of control measures,the meteorological covariate must be corrected from the observations.This study quantified the impacts of emission abatement and meteorological condition on the interannual variations of SO_(2),NO_(2),CO,O_(3),PM_(10) and PM_(2.5) concentrations in 31 major Chinese cities using an optimized machine learning-based meteorological normalization technique.Overall,the annual average concentrations of SO_(2),NO_(2),CO,PM_(10)and PM_(2.5)were reduced by 86%,51%,99%,86% and 88%from 2015 to 2020,respectively,in the studied cities,attributable to their emission reductions.However,the concentration of O_(3) was found with no significant decrease with the reduction of precursors.Emission abatement notably improved air quality between 2015 and 2018.Such a decline in emissions tended to progressively slow down since 2018.Overall,the meteorological conditions in 2016–2017 and 2018–2019 were unfavorable for a better air quality,while it became favorable in 2020–2021.Specifically,emission abatement in 2021 further lowered the concentrations of SO_(2),NO_(2),CO,and PM_(2.5),while the emission of PM_(10) increased.And changes in precursors emissions worsened O_(3) air quality.To meet the demand of improving air quality,more aggressive abatement measures need to be formulated to synergistically reduce NOx,volatile organic compounds,and coarse particles.展开更多
Grain boundaries in two-dimensional(2D)semiconductors generally induce distorted band alignment and interfacial charge,which impair their electronic properties for device applications.Here,we report the improvement of...Grain boundaries in two-dimensional(2D)semiconductors generally induce distorted band alignment and interfacial charge,which impair their electronic properties for device applications.Here,we report the improvement of band alignment at the grain boundaries of PtSe_(2),a 2D semiconductor,with selective adsorption of a presentative organic acceptor,tetracyanoquinodimethane(TCNQ).TCNQ molecules show selective adsorption at the PtSe_(2)grain boundary with strong interfacial charge.The adsorption of TCNQ distinctly improves the band alignment at the PtSe_(2)grain boundaries.With the charge transfer between the grain boundary and TCNQ,the local charge is inhibited,and the band bending at the grain boundary is suppressed,as revealed by the scanning tunneling microscopy and spectroscopy(STM/S)results.Our finding provides an effective method for the advancement of the band alignment at the grain boundary by functional molecules,improving the electronic properties of 2D semiconductors for their future applications.展开更多
Plant fungal pathogens secrete numerous proteins into the apoplast at the plant–fungus contact sites to facilitate colonization.However,only a few secretory proteins were functionally characterized in Magnaporthe ory...Plant fungal pathogens secrete numerous proteins into the apoplast at the plant–fungus contact sites to facilitate colonization.However,only a few secretory proteins were functionally characterized in Magnaporthe oryzae,the fungal pathogen causing rice blast disease worldwide.Asparagine-linked glycosylation 3(Alg3)is an a-1,3-mannosyltransferase functioning in the Nglycan synthesis of N-glycosylated secretory proteins.Fungal pathogenicity and cell wall integrity are impaired inΔalg3 mutants,but the secreted proteins affected inΔalg3 mutants are largely unknown.In this study,we compared the secretomes of the wild-type strain and theΔalg3 mutant and identified 51 proteins that require Alg3 for proper secretion.These proteins were predicted to be involved in metabolic processes,interspecies interactions,cell wall organization,and response to chemicals.Nine proteins were selected for further validation.We found that these proteins were localized at the apoplastic region surrounding the fungal infection hyphae.Moreover,the Nglycosylation of these proteins was significantly changed in theΔalg3 mutant,leading to the decreased protein secretion and abnormal protein localization.Furthermore,we tested the biological functions of two genes,INV1(encoding invertase 1,a secreted invertase)and AMCase(encoding acid mammalian chinitase,a secreted chitinase).The fungal virulence was significantly reduced,and the cell wall integrity was altered in theΔinv1 andΔamcase mutant strains.Moreover,the N-glycosylation was essential for the function and secretion of AMCase.Taken together,our study provides new insight into the role of N-glycosylated secretory proteins in fungal virulence and cell wall integrity.展开更多
Graft-versus-host disease (GVHD) significantly contributes to patient morbidity and mortality after allogeneic hematopoietic cell transplantation (allo-HSCT). Sphingosine-1-phosphate (S1P) signaling is involved in the...Graft-versus-host disease (GVHD) significantly contributes to patient morbidity and mortality after allogeneic hematopoietic cell transplantation (allo-HSCT). Sphingosine-1-phosphate (S1P) signaling is involved in the biogenetic processes of different immune cells. In the current study, we demonstrated that recipient sphingosine kinase 1 (Sphk1), but not Sphk2, was required for optimal S1PR1-dependent donor T-cell allogeneic responses by secreting S1P. Using genetic and pharmacologic approaches, we demonstrated that inhibition of Sphk1 or S1PR1 substantially attenuated acute GVHD (aGVHD) while retaining the graft-versus-leukemia (GVL) effect. At the cellular level, the Sphk1/S1P/S1PR1 pathway differentially modulated the alloreactivity of CD4+ and CD8+ T cells;it facilitated T-cell differentiation into Th1/Th17 cells but not Tregs and promoted CD4+ T-cell infiltration into GVHD target organs but was dispensable for the CTL activity of allogeneic CD8+ T cells. At the molecular level, the Sphk1/S1P/S1PR1 pathway augmented mitochondrial fission and increased mitochondrial mass in allogeneic CD4+ but not CD8+ T cells by activating the AMPK/AKT/mTOR/Drp1 pathway, providing a mechanistic basis for GVL maintenance when S1P signaling was inhibited. For translational purposes, we detected the regulatory efficacy of pharmacologic inhibitors of Sphk1 and S1PR1 in GVHD induced by human T cells in a xenograft model. Our study provides novel mechanistic insight into how the Sphk1/S1P/S1PR1 pathway modulates T-cell alloreactivity and validates Sphk1 or S1PR1 as a therapeutic target for the prevention of GVHD and leukemia relapse. This novel strategy may be readily translated into the clinic to benefit patients with hematologic malignancies and disorders.展开更多
Proteins, as the premier building blocks in nature, exhibit extraordinary ability in life activities during which process proteins mostly self-assemble into large complexes to exert prominent functions. Inspired by th...Proteins, as the premier building blocks in nature, exhibit extraordinary ability in life activities during which process proteins mostly self-assemble into large complexes to exert prominent functions. Inspired by this, recent chemical and biological stud- ies mainly focus on supramolecular self-assembly of proteins into high ordered architectures, especially the assembly suategy to unravel tile formation and function of protein nanostructures. In this review, we st, mmarize the progress made in the engi- neering of supramolecular protein architectures according to the strategies used to control the orient:ilion and the order of the assembly process. Furthermore, potential applications in biomedical areas of the supramolecular protein nanostructures will also be reviewed.展开更多
The nitrogen modified lignocelluloses(NML) produced under oxic ammoniation was metabolized by white rot fungus, NH + 4 N was released, NO - 3 N concentration was decreased and total nitrogen loss was blocked wi...The nitrogen modified lignocelluloses(NML) produced under oxic ammoniation was metabolized by white rot fungus, NH + 4 N was released, NO - 3 N concentration was decreased and total nitrogen loss was blocked within incubation period. During releasing nitrogen from the metabolism of NML, white rot fungus cometabolized recalcitrant environmental pollutants and showed higher degradation capability. Results indicated that this NML complex colonized by white rot fungus might be effective with economic feasibility when they are applied into the vast field ecosystem, it might stabilize NH + 4 nitrogen flux and bioremediate the polluted environmental sites.展开更多
Semiconducting heterojunctions(HJs),comprised of atomically thin transition metal dichalcogenides(TMDs),have shown great potentials in electronic and optoelectronic applications.Organic/TMD hybrid bilayers hold enhanc...Semiconducting heterojunctions(HJs),comprised of atomically thin transition metal dichalcogenides(TMDs),have shown great potentials in electronic and optoelectronic applications.Organic/TMD hybrid bilayers hold enhanced pumping efficiency of interfacial excitons,tunable electronic structures and optical properties,and other superior advantages to these inorganic HJs.Here,we report a direct probe of the interfacial electronic structures of a crystalline monolayer(ML)perylene-3,4,9,10-tetracarboxylic-dianhydride(PTCDA)/ML-WSe_(2) HJ using scanning tunneling microscopy,photoluminescence,and first-principle calculations.Strong PTCDAAA/Se_(2) interfacial interactions lead to appreciable hybridization of the WSe_(2) conduction band with PTCDA unoccupied states,accompanying with a significant amount of PTCDA-to-WSe_(2) charge transfer(by 0.06 e/PTCDA).A type-ll band alignment was directly determined with a valence band offset of-1.69 eV,and an apparent conduction band offset of-1.57 eV.Moreover,we found that the local stacking geometry at the HJ interface differentiates the hybridized interfacial states.展开更多
Water level fluctuation of is an important ecological character of lakes in monsoon climate zone.It is the key driver to seasonal change of the wetlands and associated habitats,which provide vital inhabiting condition...Water level fluctuation of is an important ecological character of lakes in monsoon climate zone.It is the key driver to seasonal change of the wetlands and associated habitats,which provide vital inhabiting conditions for different species in summer and winter,or,wet season and dry season.Due the hydrologic regime changes in the recent years after the operation of Three Gorges Dam,in 2012,the government of Hunan province proposed Chenglingji Hydraulic Project,aiming at water level control in dry season at Chenglingji,where the outlet of Dongting Lake located.Through different operations on water retreat process,five scenarios on the water level control from 21 m to 24 m were set in the plan.The potential ecological impacts of the project are under enormous public concern.To analyze potential impacts from different scenarios of water level control on the wetlands,this paper studied the topography of Dongting Lake bed and wetlands in dry season,by using Digital Elevation Model(DEM)and 15 images from HJ satellite and 1 image from Landsat TM.The wetlands at water levels of 19 m to 27 m were analyzed.The study revealed that there were 4 terrain steps on Dongting Lake bed from the West Dongting Lake to East Dongting Lake.Water level control at Chenglingji would increase area of open water in East Dongting Lake and Hengling Lake areas,while its effect on South Dongting Lake and West Dongting Lake areas due to higher terrain was weaker.Particularly,the area percentages of South Dongting Lake area did not change with water level fluctuation,due to its 2 elevation steps.The area percentages of various types of the wetlands in Dongting Lake area during the processes of water level rising and retreating were quite different,even in the relatively close water level interval.The retreating area of open water in autumn was larger than that during the spring flooding.The 23 m was the key water level,a turning point of the area change of the wetlands in Dongting Lake area.Areas of open water,mudflat,meadows and their percent展开更多
Myocardial infarction is a devastating disease worldwide.At present,nearly 40 million patients suffer from heart failure.Owing to a lack of adequate blood supply,25%of cardiomyocytes are subjected to apoptosis and nec...Myocardial infarction is a devastating disease worldwide.At present,nearly 40 million patients suffer from heart failure.Owing to a lack of adequate blood supply,25%of cardiomyocytes are subjected to apoptosis and necrosis within a few hours after infarction.It remains challenging to find effective therapeutic methods for heart failure.On the other hand,zebrafish and neonatal mouse hearts have a strong ability to regenerate(Poss et al.,2002;Raya et al.,2003;Porrello et al.,2011),and their regeneration derives from existing cardiomyocytes(Jopling et al.,2010;Kikuchi et al..展开更多
As a crucial biophysical property,red blood cell(RBC)deformability is pathologically altered in numerous disease states,and biochemical and structural changes occur over time in stored samples of otherwise normal RBCs...As a crucial biophysical property,red blood cell(RBC)deformability is pathologically altered in numerous disease states,and biochemical and structural changes occur over time in stored samples of otherwise normal RBCs.However,there is still a gap in applying it further to point-of-care blood devices due to the large external equipment(high-resolution microscope and microfluidic pump),associated operational difficulties,and professional analysis.Herein,we revolutionarily propose a smart optofluidic system to provide a differential diagnosis for blood testing via precise cell biophysics property recognition both mechanically and morphologically.Deformation of the RBC population is caused by pressing the hydrogel via an integrated mechanical transfer device.The biophysical properties of the cell population are obtained by the designed smartphone algorithm.Artificial intelligence-based modeling of cell biophysics properties related to blood diseases and quality was developed for online testing.We currently achieve 100%diagnostic accuracy for five typical clinical blood diseases(90 megaloblastic anemia,78 myelofibrosis,84 iron deficiency anemia,48 thrombotic thrombocytopenic purpura,and 48 thalassemias)via real-world prospective implementation;furthermore,personalized blood quality(for transfusion in cardiac surgery)monitoring is achieved with an accuracy of 96.9%.This work suggests a potential basis for next-generation blood smart health care devices.展开更多
Stimulator of interferon genes(STING)-mediated innate immune activation plays a key role in tumor-and self-DNA-elicited antitumor immunity and autoimmunity.However,STING can also suppress tumor immunity and autoimmuni...Stimulator of interferon genes(STING)-mediated innate immune activation plays a key role in tumor-and self-DNA-elicited antitumor immunity and autoimmunity.However,STING can also suppress tumor immunity and autoimmunity.STING signaling In host nonhematopoietic cells was reported to either protect against or promote graft-versus-host disease(GVHD),a major complication of allogeneic hematopoietic cell transplantation(allo-HCT).Host hematopoietic antigen-presenting cells(APCs)play key roles in donor T-cell priming during GVHD initiation.However,how STING regulates host hematopoietic APCs after allo-HCT remains unknown.We utilized murine models of allo-HCT to assess the role of STING in hematopoietic APCs.STING-deficient recipients developed more severe GVHD after major histocompatibility complex-mismatched allo-HCT.Using bone marrow chimeras,we found that STING deficiency in host hematopoietic cells was primarily responsible for exacerbating the disease.Furthermore,STING on host CD11c+cells played a dominant role in suppressing allogeneic T-cell responses.Mechanistically,STING deficiency resulted in increased survival,activation,and function of APCs,including macrophages and dendritic cells.Consistently,constitutive activation of STING attenuated the survival,activation,and function of APCs isolated from STING V154M knock-in mice.STING-deficient APCs augmented donor T-cell expansion,chemokine receptor expression,and migration into intestinal tissues,resulting in accelerated/exacerbated GVHD.Using pharmacologic approaches,we demonstrated that systemic administration of a STING agonist(bis-(3'-5')-cyclic dimeric guanosine monophosphate)to recipient mice before transplantation significantly reduced GVHD mortality.In conclusion,we revealed a novel role of STING in APC activity that dictates T-cell allogeneic responses and validated STING as a potential therapeutic target for controlling GVHD after allo-HCT.展开更多
Fe-Cr-Mn(W, V) austenite steels used as low radioactive structural materialsin fusion reactor have been investigated. The results show that the high temperature strength andthe creep fracture life of Fe-Cr-Mn(W, V) st...Fe-Cr-Mn(W, V) austenite steels used as low radioactive structural materialsin fusion reactor have been investigated. The results show that the high temperature strength andthe creep fracture life of Fe-Cr-Mn(W, V) steels can be effectively improved through (C+N)complex-strengthening, so can be the high temperature ductility. The strength and ductility of thesteels are superior to that of SUS316 steels and JPCAS below 673 K. The relationship betweenstrength, ductility and the formation temperature is related to the evolution of deformationmicrostructure. The fracture and microstructure observation above 673 K indicates that the main wayto further improve ductility at high temperature is the control of carbide coarsening at the grainboundaries.展开更多
In the seemingly unrelated regression systems, the existing quasi-likelihood is always involved in the difficult problem of calculating inverse of a high order matrix specially for large systems. To avoid this problem...In the seemingly unrelated regression systems, the existing quasi-likelihood is always involved in the difficult problem of calculating inverse of a high order matrix specially for large systems. To avoid this problem, the new quasi-likelihood proposed in this paper is based mainly on a linearly iterative process of some unbiased estimating functions.Some finite sample properties and asymptotic behaviours for this new quasi-likelihood are investigated. These results show that the new quasi-likelihood for parameter of interest is E-sufficient, iteratively efficient and approximately efficient. Some examples are given to illustrate the theoretical results.展开更多
基金supported by grants from the National Key Research and Development Program of China(grant no.2016YFD0300700)the National Natural Science Foundation of China(youth grant,no.32000859)+1 种基金the Project for Extramural Scientists of the State Key Laboratory of Agrobiotechnology(project ID:2020SKLAB6-26)The research of R.S.and G.V.d.A.was financed in part by grants from the Dutch Research Council(NWO).
文摘The jasmonic acid(JA)signaling pathway is used by plants to control wound responses.The persistent accumulation of JA inhibits plant growth,and the hydroxylation of JA to 12-hydroxy-JA by JASMONATE-INDUCED OXYGENASEs(JOXs,also named jasmonic acid oxidases)is therefore vital for plant growth,while structural details of JA recognition by JOXs are unknown.Here,we present the 2.65Åresolution X-ray crystal structure of Arabidopsis JOX2 in complex with its substrate JA and its co-substrates 2-oxoglutarate and Fe(Ⅱ).JOX2 contains a distorted double-stranded p helix(DSBH)core flanked by a helices and loops.JA is bound in the narrow substrate pocket by hydrogen bonds with the arginine triad R225,R350,and R354 and by hydrophobic interactions mainly with the phenylalanine triad F157,F317,and F346.The most critical residues for JA binding are F157 and R225,both from the DSBH core,which interact with the cyclopentane ring of JA.The spatial distribution of critical residues for JA binding and the shape of the substrate-binding pocket together define the substrate selectivity of the JOXs.Sequence alignment shows that these critical residues are conserved among JOXs from higher plants.Collectively,our study provides insights into the mechanism by which higher plants hydroxylate the hormone JA.
基金NSFC(Nos.U1805255,11804086,21706044,21971057)General Financial Grant from the China Postdoctoral Science Foundation(No.2017M621316)+2 种基金the Natural Science Foundation of Heilongjiang Province,China(No.B2017006)the General Financial Grant from the Postdoctoral Science Foundation of Heilongjiang Province,China(No.LBHZ17187)the General Financial Grant from Heilongjiang Province for returned students from overseas in 2018。
文摘Efficient generation of singlet oxygen(1 O_(2)) by an excitonic ene rgy transfer process is highly desired on a semiconductor photocatalyst for selective oxidation of methyl phenyl sulfide(MPS).Herein,it is demonstrated that a large amount of 1 O_(2) is produced on pristine graphitic carbon nitride(CN) nanosheet compared with bismuth oxybromide(BiOBr) and comme rcial P25 titanium dioxide(TiO_(2)).This leads to a certain photoactivity of CN for MPS oxidation.The observed ~77% selectivity for CN depends on the competitive results of excitonic energy transfer for 1 O_(2) formation and charge carrier separation for superoxide radical(O_(2)·) production,which are based on the phosphorescence spectra and electron paramagnetic resonance signals,respectively.Moreover,ultrathin CN nanosheets are synthesized by thermal treatment with the cyanuric acid-melamine hydrogen bonded aggregates as precursors.It is confirmed that the amount of produced 1 O_(2) could be increased by decreasing the thickness of resultant CN nanosheets.The optimized ultrathin CN nanosheet(~4 nm) exhibits excellent photoactivity with high selectivity(~99%).It is suggested that the excitonic energy transfer for 1 O_(2) formation is close related to the intrinsic exciton binding energy and the two-dimensional quantum confinement effect.This work establishes a basic mechanistic understanding on the excitonic processes in CN,and develops a feasible route to design CN-based photocatalysts for efficient 1 O_(2) generation.
文摘lmprovement of the charge separation of titanosilicate molecular sieves is critical to their use asphotocatalysts for oxidative organic transformations.In this work,MFI TS-1 molecular sievenanosheets(TS-1 NS)were synthesized by a low-temperature hydrothermal method using a tai-lored diquaternary ammonium surfactant as the structure-directing agent.Introducing Ni^2+cationsat the ion-exchange sites of the TS-1 NS framework significantly enhanced its photoactivity in aero-bic alcohol oxidation.The optimized Ni cation-functionalized TS-1 NS(Ni/TS-1 NS)provide impres-sive photoactivity,with a benzyl alcohol(BA)conversion of 78.9%and benzyl aldehyde(BAD)se-lectivity of 98.8%using O as the only oxidant under full light irradiation;this BAD yield is approx-imately six times greater than that obtained for bulk TS-1,and is maintained for five runs.The ex-cellent photoactivity of Ni/TS-1 NS is attributed to the significantly enlarged surface area of thetwo-dimensional morphology TS-1 NS,extra mesopores,and greatly improved charge separation.Compared with bulk TS-1,Ni/TS-1 NS has a much shorter charge transfer distance.Theas-introduced Ni species could capture the photoelectrons to further improve the charge separa-tion.This work opens the way to a class of highly selective,robust,and low-cost titanosilicate mo-lecular sieve-based photocatalysts with industrial potential for selective oxidative transformationsand pollutant degradation.
基金supported by the National Key R&D Program of China (Grant No. 2022YFC3703001)the China Postdoctoral Science Foundation (Grant No. 2022T150334)the National Natural Science Foundation of China (Grant Nos. 42177085 & 42177465)。
文摘Air pollutant concentration is a function of emission rates and meteorology.To accurately evaluate the effect of control measures,the meteorological covariate must be corrected from the observations.This study quantified the impacts of emission abatement and meteorological condition on the interannual variations of SO_(2),NO_(2),CO,O_(3),PM_(10) and PM_(2.5) concentrations in 31 major Chinese cities using an optimized machine learning-based meteorological normalization technique.Overall,the annual average concentrations of SO_(2),NO_(2),CO,PM_(10)and PM_(2.5)were reduced by 86%,51%,99%,86% and 88%from 2015 to 2020,respectively,in the studied cities,attributable to their emission reductions.However,the concentration of O_(3) was found with no significant decrease with the reduction of precursors.Emission abatement notably improved air quality between 2015 and 2018.Such a decline in emissions tended to progressively slow down since 2018.Overall,the meteorological conditions in 2016–2017 and 2018–2019 were unfavorable for a better air quality,while it became favorable in 2020–2021.Specifically,emission abatement in 2021 further lowered the concentrations of SO_(2),NO_(2),CO,and PM_(2.5),while the emission of PM_(10) increased.And changes in precursors emissions worsened O_(3) air quality.To meet the demand of improving air quality,more aggressive abatement measures need to be formulated to synergistically reduce NOx,volatile organic compounds,and coarse particles.
基金the National Key Research and Development Program of China(Nos.2021YFA1400100,2020YFA0308800,and 2019YFA0308000)the National Natural Science Foundation of China(Nos.92163206 and 62171035)+2 种基金the Beijing Nova Program from Beijing Municipal Science&Technology Commission(No.Z211100002121072)the Beijing Natural Science Foundation(Nos.Z190006 and 4192054)Calculations were performed at the Physics Lab of High-Performance Computing of Renmin University of China,and Beijing Super Cloud Computing Center.
文摘Grain boundaries in two-dimensional(2D)semiconductors generally induce distorted band alignment and interfacial charge,which impair their electronic properties for device applications.Here,we report the improvement of band alignment at the grain boundaries of PtSe_(2),a 2D semiconductor,with selective adsorption of a presentative organic acceptor,tetracyanoquinodimethane(TCNQ).TCNQ molecules show selective adsorption at the PtSe_(2)grain boundary with strong interfacial charge.The adsorption of TCNQ distinctly improves the band alignment at the PtSe_(2)grain boundaries.With the charge transfer between the grain boundary and TCNQ,the local charge is inhibited,and the band bending at the grain boundary is suppressed,as revealed by the scanning tunneling microscopy and spectroscopy(STM/S)results.Our finding provides an effective method for the advancement of the band alignment at the grain boundary by functional molecules,improving the electronic properties of 2D semiconductors for their future applications.
基金supported by the National Key R&D Plan of China(Grant No.2016YFD0300703)the China Agricultural Research System(Grant No.CARS-01-33)+2 种基金the Program for Changjiang Scholars and Innovative Research Team in University(Grant No.IRT1042)the 111 Project(Grant No.B13006)to YLPthe National Natural Science Foundation of China(Grant No.32001848)to XL。
文摘Plant fungal pathogens secrete numerous proteins into the apoplast at the plant–fungus contact sites to facilitate colonization.However,only a few secretory proteins were functionally characterized in Magnaporthe oryzae,the fungal pathogen causing rice blast disease worldwide.Asparagine-linked glycosylation 3(Alg3)is an a-1,3-mannosyltransferase functioning in the Nglycan synthesis of N-glycosylated secretory proteins.Fungal pathogenicity and cell wall integrity are impaired inΔalg3 mutants,but the secreted proteins affected inΔalg3 mutants are largely unknown.In this study,we compared the secretomes of the wild-type strain and theΔalg3 mutant and identified 51 proteins that require Alg3 for proper secretion.These proteins were predicted to be involved in metabolic processes,interspecies interactions,cell wall organization,and response to chemicals.Nine proteins were selected for further validation.We found that these proteins were localized at the apoplastic region surrounding the fungal infection hyphae.Moreover,the Nglycosylation of these proteins was significantly changed in theΔalg3 mutant,leading to the decreased protein secretion and abnormal protein localization.Furthermore,we tested the biological functions of two genes,INV1(encoding invertase 1,a secreted invertase)and AMCase(encoding acid mammalian chinitase,a secreted chitinase).The fungal virulence was significantly reduced,and the cell wall integrity was altered in theΔinv1 andΔamcase mutant strains.Moreover,the N-glycosylation was essential for the function and secretion of AMCase.Taken together,our study provides new insight into the role of N-glycosylated secretory proteins in fungal virulence and cell wall integrity.
基金This work is supported in part by SmartState Cancer Stem Cell Biology&Therapy Program and by R01 grants from the National Institutes of Health,including AI118305,HL140953 and CA258440(X.-Z.Y.).
文摘Graft-versus-host disease (GVHD) significantly contributes to patient morbidity and mortality after allogeneic hematopoietic cell transplantation (allo-HSCT). Sphingosine-1-phosphate (S1P) signaling is involved in the biogenetic processes of different immune cells. In the current study, we demonstrated that recipient sphingosine kinase 1 (Sphk1), but not Sphk2, was required for optimal S1PR1-dependent donor T-cell allogeneic responses by secreting S1P. Using genetic and pharmacologic approaches, we demonstrated that inhibition of Sphk1 or S1PR1 substantially attenuated acute GVHD (aGVHD) while retaining the graft-versus-leukemia (GVL) effect. At the cellular level, the Sphk1/S1P/S1PR1 pathway differentially modulated the alloreactivity of CD4+ and CD8+ T cells;it facilitated T-cell differentiation into Th1/Th17 cells but not Tregs and promoted CD4+ T-cell infiltration into GVHD target organs but was dispensable for the CTL activity of allogeneic CD8+ T cells. At the molecular level, the Sphk1/S1P/S1PR1 pathway augmented mitochondrial fission and increased mitochondrial mass in allogeneic CD4+ but not CD8+ T cells by activating the AMPK/AKT/mTOR/Drp1 pathway, providing a mechanistic basis for GVL maintenance when S1P signaling was inhibited. For translational purposes, we detected the regulatory efficacy of pharmacologic inhibitors of Sphk1 and S1PR1 in GVHD induced by human T cells in a xenograft model. Our study provides novel mechanistic insight into how the Sphk1/S1P/S1PR1 pathway modulates T-cell alloreactivity and validates Sphk1 or S1PR1 as a therapeutic target for the prevention of GVHD and leukemia relapse. This novel strategy may be readily translated into the clinic to benefit patients with hematologic malignancies and disorders.
基金supported by the National Natural Science Foundation of China(21234004,21420102007,21574056,91527302)the Chang Jiang Scholars Program of China
文摘Proteins, as the premier building blocks in nature, exhibit extraordinary ability in life activities during which process proteins mostly self-assemble into large complexes to exert prominent functions. Inspired by this, recent chemical and biological stud- ies mainly focus on supramolecular self-assembly of proteins into high ordered architectures, especially the assembly suategy to unravel tile formation and function of protein nanostructures. In this review, we st, mmarize the progress made in the engi- neering of supramolecular protein architectures according to the strategies used to control the orient:ilion and the order of the assembly process. Furthermore, potential applications in biomedical areas of the supramolecular protein nanostructures will also be reviewed.
文摘The nitrogen modified lignocelluloses(NML) produced under oxic ammoniation was metabolized by white rot fungus, NH + 4 N was released, NO - 3 N concentration was decreased and total nitrogen loss was blocked within incubation period. During releasing nitrogen from the metabolism of NML, white rot fungus cometabolized recalcitrant environmental pollutants and showed higher degradation capability. Results indicated that this NML complex colonized by white rot fungus might be effective with economic feasibility when they are applied into the vast field ecosystem, it might stabilize NH + 4 nitrogen flux and bioremediate the polluted environmental sites.
基金supported by the National Key R&D Program of China(Nos.2018FYA0305800 and 2018YFA0703700)the National Natural Science Foundation of China(Nos.11774268 and 11974012)+2 种基金the Strategic Priority Research Program of Chinese Academy of Sciences(No.XDB30000000)support from the Fundamental Research Funds for the Central Universities,Chinathe Research Funds of Renmin University of China(Nos.16XNLQ01 and 19XNQ025)。
文摘Semiconducting heterojunctions(HJs),comprised of atomically thin transition metal dichalcogenides(TMDs),have shown great potentials in electronic and optoelectronic applications.Organic/TMD hybrid bilayers hold enhanced pumping efficiency of interfacial excitons,tunable electronic structures and optical properties,and other superior advantages to these inorganic HJs.Here,we report a direct probe of the interfacial electronic structures of a crystalline monolayer(ML)perylene-3,4,9,10-tetracarboxylic-dianhydride(PTCDA)/ML-WSe_(2) HJ using scanning tunneling microscopy,photoluminescence,and first-principle calculations.Strong PTCDAAA/Se_(2) interfacial interactions lead to appreciable hybridization of the WSe_(2) conduction band with PTCDA unoccupied states,accompanying with a significant amount of PTCDA-to-WSe_(2) charge transfer(by 0.06 e/PTCDA).A type-ll band alignment was directly determined with a valence band offset of-1.69 eV,and an apparent conduction band offset of-1.57 eV.Moreover,we found that the local stacking geometry at the HJ interface differentiates the hybridized interfacial states.
基金Under the auspices of National Key R&D Program of China(2017YFC0405300)
文摘Water level fluctuation of is an important ecological character of lakes in monsoon climate zone.It is the key driver to seasonal change of the wetlands and associated habitats,which provide vital inhabiting conditions for different species in summer and winter,or,wet season and dry season.Due the hydrologic regime changes in the recent years after the operation of Three Gorges Dam,in 2012,the government of Hunan province proposed Chenglingji Hydraulic Project,aiming at water level control in dry season at Chenglingji,where the outlet of Dongting Lake located.Through different operations on water retreat process,five scenarios on the water level control from 21 m to 24 m were set in the plan.The potential ecological impacts of the project are under enormous public concern.To analyze potential impacts from different scenarios of water level control on the wetlands,this paper studied the topography of Dongting Lake bed and wetlands in dry season,by using Digital Elevation Model(DEM)and 15 images from HJ satellite and 1 image from Landsat TM.The wetlands at water levels of 19 m to 27 m were analyzed.The study revealed that there were 4 terrain steps on Dongting Lake bed from the West Dongting Lake to East Dongting Lake.Water level control at Chenglingji would increase area of open water in East Dongting Lake and Hengling Lake areas,while its effect on South Dongting Lake and West Dongting Lake areas due to higher terrain was weaker.Particularly,the area percentages of South Dongting Lake area did not change with water level fluctuation,due to its 2 elevation steps.The area percentages of various types of the wetlands in Dongting Lake area during the processes of water level rising and retreating were quite different,even in the relatively close water level interval.The retreating area of open water in autumn was larger than that during the spring flooding.The 23 m was the key water level,a turning point of the area change of the wetlands in Dongting Lake area.Areas of open water,mudflat,meadows and their percent
基金supported by grants from the National Natural Science Foundation of China(Nos.31730061,81870198 and 31821091)the National Key R&D Program of China(2018YFA080050 and 2019YFA0801602)
文摘Myocardial infarction is a devastating disease worldwide.At present,nearly 40 million patients suffer from heart failure.Owing to a lack of adequate blood supply,25%of cardiomyocytes are subjected to apoptosis and necrosis within a few hours after infarction.It remains challenging to find effective therapeutic methods for heart failure.On the other hand,zebrafish and neonatal mouse hearts have a strong ability to regenerate(Poss et al.,2002;Raya et al.,2003;Porrello et al.,2011),and their regeneration derives from existing cardiomyocytes(Jopling et al.,2010;Kikuchi et al..
基金This work was supported by the National Key R&D Program of China(2018YFC1003200)the National Natural Science Foundation of China(Nos.62175190,11774274,81860276,and 81770179)+1 种基金Foundation Research Fund of Shenzhen Science and Technology Program(No.JCYJ20190808154409678)Support Projects of Medical Science and Technology Innovation Platform of Wuhan University Zhongnan Hospital in 2020(lcyf202010).
文摘As a crucial biophysical property,red blood cell(RBC)deformability is pathologically altered in numerous disease states,and biochemical and structural changes occur over time in stored samples of otherwise normal RBCs.However,there is still a gap in applying it further to point-of-care blood devices due to the large external equipment(high-resolution microscope and microfluidic pump),associated operational difficulties,and professional analysis.Herein,we revolutionarily propose a smart optofluidic system to provide a differential diagnosis for blood testing via precise cell biophysics property recognition both mechanically and morphologically.Deformation of the RBC population is caused by pressing the hydrogel via an integrated mechanical transfer device.The biophysical properties of the cell population are obtained by the designed smartphone algorithm.Artificial intelligence-based modeling of cell biophysics properties related to blood diseases and quality was developed for online testing.We currently achieve 100%diagnostic accuracy for five typical clinical blood diseases(90 megaloblastic anemia,78 myelofibrosis,84 iron deficiency anemia,48 thrombotic thrombocytopenic purpura,and 48 thalassemias)via real-world prospective implementation;furthermore,personalized blood quality(for transfusion in cardiac surgery)monitoring is achieved with an accuracy of 96.9%.This work suggests a potential basis for next-generation blood smart health care devices.
基金supported in part by the Hollings Cancer Center Fellowship(to V.W.)NIH Grant R01CA163910(to C.-CAH.)NIH ROIs AI118305,HL137373,and HL140953(to X.-Z.Y.).
文摘Stimulator of interferon genes(STING)-mediated innate immune activation plays a key role in tumor-and self-DNA-elicited antitumor immunity and autoimmunity.However,STING can also suppress tumor immunity and autoimmunity.STING signaling In host nonhematopoietic cells was reported to either protect against or promote graft-versus-host disease(GVHD),a major complication of allogeneic hematopoietic cell transplantation(allo-HCT).Host hematopoietic antigen-presenting cells(APCs)play key roles in donor T-cell priming during GVHD initiation.However,how STING regulates host hematopoietic APCs after allo-HCT remains unknown.We utilized murine models of allo-HCT to assess the role of STING in hematopoietic APCs.STING-deficient recipients developed more severe GVHD after major histocompatibility complex-mismatched allo-HCT.Using bone marrow chimeras,we found that STING deficiency in host hematopoietic cells was primarily responsible for exacerbating the disease.Furthermore,STING on host CD11c+cells played a dominant role in suppressing allogeneic T-cell responses.Mechanistically,STING deficiency resulted in increased survival,activation,and function of APCs,including macrophages and dendritic cells.Consistently,constitutive activation of STING attenuated the survival,activation,and function of APCs isolated from STING V154M knock-in mice.STING-deficient APCs augmented donor T-cell expansion,chemokine receptor expression,and migration into intestinal tissues,resulting in accelerated/exacerbated GVHD.Using pharmacologic approaches,we demonstrated that systemic administration of a STING agonist(bis-(3'-5')-cyclic dimeric guanosine monophosphate)to recipient mice before transplantation significantly reduced GVHD mortality.In conclusion,we revealed a novel role of STING in APC activity that dictates T-cell allogeneic responses and validated STING as a potential therapeutic target for controlling GVHD after allo-HCT.
文摘Fe-Cr-Mn(W, V) austenite steels used as low radioactive structural materialsin fusion reactor have been investigated. The results show that the high temperature strength andthe creep fracture life of Fe-Cr-Mn(W, V) steels can be effectively improved through (C+N)complex-strengthening, so can be the high temperature ductility. The strength and ductility of thesteels are superior to that of SUS316 steels and JPCAS below 673 K. The relationship betweenstrength, ductility and the formation temperature is related to the evolution of deformationmicrostructure. The fracture and microstructure observation above 673 K indicates that the main wayto further improve ductility at high temperature is the control of carbide coarsening at the grainboundaries.
基金Project supported by the National Natural Science Foundation of China (No.10371059, No.10171051).
文摘In the seemingly unrelated regression systems, the existing quasi-likelihood is always involved in the difficult problem of calculating inverse of a high order matrix specially for large systems. To avoid this problem, the new quasi-likelihood proposed in this paper is based mainly on a linearly iterative process of some unbiased estimating functions.Some finite sample properties and asymptotic behaviours for this new quasi-likelihood are investigated. These results show that the new quasi-likelihood for parameter of interest is E-sufficient, iteratively efficient and approximately efficient. Some examples are given to illustrate the theoretical results.