To expand the study on the structures and biological activities of the anthracyclines anticancer drugs and reduce their toxic side effects,the new anthraquinone derivatives,9‑pyridylanthrahydrazone(9‑PAH)and 9,10‑bisp...To expand the study on the structures and biological activities of the anthracyclines anticancer drugs and reduce their toxic side effects,the new anthraquinone derivatives,9‑pyridylanthrahydrazone(9‑PAH)and 9,10‑bispyridylanthrahydrazone(9,10‑PAH)were designed and synthesized.Utilizing 9‑PAH and 9,10‑PAH as promising anticancer ligands,their respective copper complexes,namely[Cu(L1)Cl_(2)]Cl(1)and{[Cu_(4)(μ_(2)‑Cl)_(3)Cl_(4)(9,10‑PAH)_(2)(DMSO)_(2)]Cl_(2)}_(n)(2),were subsequently synthesized,where the new ligand L1 is formed by coupling two 9‑PAH ligands in the coordination reaction.The chemical and crystal structures of 1 and 2 were elucidated by IR,MS,elemental analysis,and single‑crystal X‑ray diffraction.Complex 1 forms a mononuclear structure.L1 coordinates with Cu through its three N atoms,together with two Cl atoms,to form a five‑coordinated square pyramidal geometry.Complex 2 constitutes a polymeric structure,wherein each structural unit centrosymmetrically encompasses two five‑coordinated binuclear copper complexes(Cu1,Cu2)of 9,10‑PAH,with similar square pyramidal geometry.A chlorine atom(Cl_(2)),located at the symmetry center,bridges Cu1 and Cu1A to connect the two binuclear copper structures.Meanwhile,the two five‑coordinated Cu2 atoms symmetrically bridge the adjacent structural units via one coordinated Cl atom,respectively,thus forming a 1D chain‑like polymeric structure.In vitro anticancer activity assessments revealed that 1 and 2 showed significant cytotoxicity even higher than cisplatin.Specifically,the IC_(50)values of 2 against HeLa‑229 and SK‑OV‑3 cancer cell lines were determined to be(5.92±0.32)μmol·L^(-1)and(6.48±0.39)μmol·L^(-1),respectively.2 could also block the proliferation of HeLa‑229 cells in S phase and significantly induce cell apoptosis.In addition,fluorescence quenching competition experiments suggested that 2 might interact with DNA by an intercalative binding mode,offering insights into its underlying anticancer mechanism.CCDC:2388918,1;2388919,2.展开更多
Two Gd_(2)complexes,namely[Gd_(2)(dbm)_(2)(HL_(1))_(2)(CH_(3)OH)_(2)]·4CH_(3)OH(1)and[Gd_(2)(dbm)_(2)(L_(2))_(2)(CH_(3)OH)_(2)]·2CH_(3)OH(2),where H_(3)L_(1)=(Z)-N'-[4-(diethylamino)-2-hydroxybenzylidene...Two Gd_(2)complexes,namely[Gd_(2)(dbm)_(2)(HL_(1))_(2)(CH_(3)OH)_(2)]·4CH_(3)OH(1)and[Gd_(2)(dbm)_(2)(L_(2))_(2)(CH_(3)OH)_(2)]·2CH_(3)OH(2),where H_(3)L_(1)=(Z)-N'-[4-(diethylamino)-2-hydroxybenzylidene]-2-hydroxyacetohydrazide,H_(2)L_(2)=(E)-N'-(5-bromo-2-hydroxy-3-methoxybenzylidene)nicotinohydrazide,Hdbm=dibenzoylmethane,have been constructed by adopting the solvothermal method.Structural characterization unveils that both complexes 1 and 2 are constituted by two Gd^(3+)ions,two dbm-ions,two CH_(3)OH molecules,and two polydentate Schiff-base ligands(HL_(1)^(2-)or L_(2)^(2-)).In addition,complex 1 contains four free methanol molecules,whereas complex 2 harbors two free methanol molecules.By investigating the interactions between complexes 1 and 2 and four types of bacteria(Bacillus subtilis,Escherichia coli,Staphylococcus aureus,Candida albicans),it was found that both complexes 1 and 2 exhibited potent antibacte-rial activities.The interaction mechanisms between the ligands H_(3)L_(1),H_(2)L_(2),complexes 1 and 2,and calf thymus DNA(CT-DNA)were studied using ultraviolet-visible spectroscopy,fluorescence titration,and cyclic voltammetry.The results demonstrated that both complexes 1 and 2 can intercalate into CT-DNA molecules,thereby inhibiting bacterial proliferation to achieve the antibacterial effects.CCDC:2401116,1;2401117,2.展开更多
Integrating a heterogeneous structure can significantly enhance the strength-ductility synergy of composites.However,the relationship between hetero-deformation induced(HDI)strain hardening and dislocation activity ca...Integrating a heterogeneous structure can significantly enhance the strength-ductility synergy of composites.However,the relationship between hetero-deformation induced(HDI)strain hardening and dislocation activity caused by heterogeneous structures in the magnesium matrix composite remains unclear.In this study,a dual-heterogeneous TiC/AZ61 composite exhibits significantly improved plastic elongation(PEL)by nearly one time compared to uniform FG composite,meanwhile maintaining a high strength(UTS:417 MPa).This is because more severe deformation inhomogeneity in heterogeneous structure leads to more geometrically necessary dislocations(GNDs)accumulation and stronger HDI stress,resulting in higher HDI hardening compared to FG and CG composites.During the early stage of plastic deformation,the pile-up types of GND in the FG zone and CG zone are significantly different.GNDs tend to form substructures in the FG zone instead of the CG zone.They only accumulate at grain boundaries of the CG region,thereby leading to obviously increased back stress in the CG region.In the late deformation stage,the elevated HDI stress activates the new〈c+a〉dislocations in the CG region,resulting in dislocation entanglements and even the formation of substructures,further driving the high hardening in the heterogeneous composite.However,For CG composite,〈c+a〉dislocations are not activated even under large plastic strains,and only〈a〉dislocations pile up at grain boundaries and twin boundaries.Our work provides an in-depth understanding of dislocation variation and HDI hardening in heterogeneous magnesium-based composites.展开更多
Polymeric perylene diimide(PDI)has been evidenced as a good candidate for photocatalytic water oxidation,yet the origin of the photocatalytic oxygen evolution activity remains unclear and needs further exploration.Her...Polymeric perylene diimide(PDI)has been evidenced as a good candidate for photocatalytic water oxidation,yet the origin of the photocatalytic oxygen evolution activity remains unclear and needs further exploration.Herein,with crystal and atomic structures of the self-assembled PDI revealed from the X-ray diffraction pattern,the electronic structure is theoretically illustrated by the first-principles density functional theory calculations,suggesting the suitable band structure and the direct electronic transition for efficient photocatalytic oxygen evolution over PDI.It is confirmed that the carbonyl O atoms on the conjugation structure serve as the active sites for oxygen evolution reaction by the crystal orbital Hamiltonian group analysis.The calculations of reaction free energy changes indicate that the oxygen evolution reaction should follow the reaction pathway of H_(2)O→^(*)OH→^(*)O→^(*)OOH→^(*)O_(2)with an overpotential of 0.81 V.Through an in-depth theoretical computational analysis in the atomic and electronic structures,the origin of photocatalytic oxygen evolution activity for PDI is well illustrated,which would help the rational design and modification of polymeric photocatalysts for efficient oxygen evolution.展开更多
2-substituted-1-amino-o-carboranes 2-R-1-NH_(2)-o-C_(2)B_(10)H_(10)(R=CH_(3),1a;R=Ph,1b)were synthesized and the reactions of these compounds with the yttrium dialkyl complex[Y(L)(CH_(2)SiMe3)_(2)](L=[2-(2,5-Me_(2)C_(...2-substituted-1-amino-o-carboranes 2-R-1-NH_(2)-o-C_(2)B_(10)H_(10)(R=CH_(3),1a;R=Ph,1b)were synthesized and the reactions of these compounds with the yttrium dialkyl complex[Y(L)(CH_(2)SiMe3)_(2)](L=[2-(2,5-Me_(2)C_(4)H_(2)N)C_(6)H4NC(Ph)=NDipp]-,Dipp=2,6-iPr_(2)C_(6)H_(3))were investigated.The 1H NMR spectroscopy indicate that the reaction of ytrrium dialkyl complex with one equivalent of 2-R-1-NH_(2)-o-C_(2)B_(10)H_(10) produce the mixture of ytrrium alkyl-amido complex[Y(L)(2-R-1-NH-o-C_(2)B_(10)H_(10))(CH_(2)SiMe3)](R=CH_(3),2a;R=Ph,2b)and bis(amido)complex[Y(L)(2-R-1-NH-o-C_(2)B_(10)H_(10))_(2)](R=CH_(3),3a;R=Ph,3b).The yttrium bridging imido complex[Y(L)(2-CH_(3)-1-N-o-C_(2)B_(10)H_(10))]_(2)(4a)was obtained by heating the mixture at 55℃for 12 h.Complex 3a was isolated and characterized by treating the yttrium dialkyl complex with two equivalents of 1a.The structures of complexes 3a and 4a were verified by single-crystal Xray diffraction.CCDC:2424136,3a;2424137,4a.展开更多
A novel 3D metal-organic framework(MOF)[Pr_(2)(L)_(3)(H_(2)O)5·H_(2)O]n(Pr-1),(H_(2)L=4,4'-oxybis(benzoic acid))with a rare structure of broken layer net,was constructed under the condition of solvothermal sy...A novel 3D metal-organic framework(MOF)[Pr_(2)(L)_(3)(H_(2)O)5·H_(2)O]n(Pr-1),(H_(2)L=4,4'-oxybis(benzoic acid))with a rare structure of broken layer net,was constructed under the condition of solvothermal synthesis.The struc-ture and crystal net were analyzed and characterized.This rod net of Pr-1 is new to both RCSR and ToposPro data-bases,and is named as rn-12 as suggested.Due to the luminescent properties of H_(2)L and Pr(Ⅲ),the solid-state fluo-rescence property and sensing performance(solvents and metal ions)of Pr-1 were investigated.The sensing experi-ments indicated that Pr-1 could act as a fluorescence sensor to detect Cd^(2+)ions with good sensitivity.In addition,antibacterial activities show that Pr-1 exhibited stronger antibacterial activity against Escherichia coli(E.coli),Staphylococcus aureus(S.aureus),and Bacillus subtilis(B.subtilis)compared to synthetic materials.展开更多
Controlled by the squeezing collision between the Yangtze block and the North China block and the left movement of the Tanlu fault, the Xu-Su region developed into an arc-shaped nappe structure, and many destructive e...Controlled by the squeezing collision between the Yangtze block and the North China block and the left movement of the Tanlu fault, the Xu-Su region developed into an arc-shaped nappe structure, and many destructive earthquakes occurred in its periphery. The geological structure of this area is complex, and there is the possibility of moderate and strong earthquakes. To further explore the crust density structure and identify the main faults and deep structural features in the Xu-Su region, based on the observed seismic data and gravity/GNSS co-site observation data, combined with the EGM2008 global gravity field model, we obtained the density of three-dimensional structure using cross gradient method joint inversion. Based on this, a geological model of the Xu-Su region was established. The results show that the crustal density anomaly amplitude within 0-25 km of the Xu-Su region ranges from-280 to 490 kg/m3, showing a zonal distribution in east-west direction and a segmented north-south direction. There are several density anomalies in the shallow(0-4 km) region at Tongshan, Huaibei, Xiayi, Woyang, etc. The density anomalies are significantly correlated with the distribution of regional faults. The density structure is divided into two large regions by Subei fault, which can be further divided along the eastwest Kouziji-Nanzhao fault and Guzhen-Huaiyuan fault. The earthquakes are obviously related to the regional fault activity and the spatial distribution of abnormal bodies. The earthquake-prone areas(5-15 km) correspond to the abnormal density mutation zone, upper uplift zone, and transformation zone near Xiaoxian, Tongshan, and Xushuanglou faults. The comprehensive results show three weak seismic activity areas in the whole region, which are located near the Huaibei, Xiaoxian, and Wohe faults. The results provide theoretical support for seismic risk analysis in this area, and these three areas should be emphasized in future seismic hazard analysis.展开更多
To develop new environmentally friendly fungicides,we designed and synthesized a novel series of D/Lconfigured camphor oxime ester derivatives based on the natural product camphor as a lead compound.We investigated th...To develop new environmentally friendly fungicides,we designed and synthesized a novel series of D/Lconfigured camphor oxime ester derivatives based on the natural product camphor as a lead compound.We investigated the in vitro antifungal activity of these compounds against six common plant pathogenic fungi.Among them,compounds B1-6,B1-17 and B2-6 displayed great in vitro activity against Rhizoctonia solani with EC50 values of 7.28,4.64,and 7.62μg/mL.The HOMO and LUMO calculations indicated that strong electronwithdrawing halogen elements exhibit better activity compared to electron-donating alkyl groups.Preliminary mechanistic studies,using SEM and TEM,indicated that compound B1-17 induced disordered entanglement of hyphae,shrinkage of hyphal surfaces,and vacuole swelling and rupture,which disrupted normal hyphal growth.Additionally,compound B1-17 induced the production and accumulation of ROS,disrupted MMP,and effectively inhibited the germination and formation of sclerotia in Rhizoctonia solani.These compounds hold potential as new antifungal agents for further research.展开更多
Hydrocracking technology represents a crucial position in the conversion of heavy oil and the transformation development from oil refining to the chemical industry.The properties of catalysts are one of the key factor...Hydrocracking technology represents a crucial position in the conversion of heavy oil and the transformation development from oil refining to the chemical industry.The properties of catalysts are one of the key factors in the hydrocracking process.As the main acidic component of hydrocracking catalyst,the influence of zeolite properties on the reaction performance has been the focus of research.In this study,a series of NiMo/Al_(2)O_(3)-Y catalysts were prepared using different Y zeolites as acidic components,and their performances in the hydrocracking of n-C_(10)were also evaluated.The structure-activity relationship between Y zeolite and the cracking performance of n-C_(10)was investigated with machine learning.First,a database of the physical and chemical properties of Y zeolite and their performance was established,and the correlation analysis was also conducted.Parameters such as the cell constant,acid content,acid strength,B/L ratio,mesopore volume,micropore volume of Y zeolite,and the reaction temperature were selected as independent variables.The conversion of n-C_(10)and the ratios of products C_(3)/C_(7)and i-C_(4)/n-C_(4)were selected as dependent variables.A model was established by the random forest algorithm and a new zeolite was predicted based on it.The results of model prediction were in good agreement with the experimental results.The R^(2)of the n-C_(10)conversion,C_(3)/C_(7)ratio,and i-C_(4)/n-C_(4)ratio were 0.9866,0.9845,and 0.9922,and the minimum root mean square error values were 0.0163,0.101,and 0.0211,respectively.These results can provide reference for the development of high performance hydrocracking catalyst and technology.展开更多
In this work,we employed a ring-opening strategy to develop a series of novel N-benzyl arylamide derivatives as tubulin polymerization inhibitors.Notably,13n(MY-1388)exhibited remarkable antiproliferative potency on f...In this work,we employed a ring-opening strategy to develop a series of novel N-benzyl arylamide derivatives as tubulin polymerization inhibitors.Notably,13n(MY-1388)exhibited remarkable antiproliferative potency on fifteen human cancer cell lines,with half maximal inhibitory concentration(IC_(50))values ranging from 8 nmol/L to 48 nmol/L.Furthermore,13n effectively suppressed tubulin polymerization by targeting the colchicine-binding site(IC_(50)=0.62μmol/L).13n also exhibited significant inhibition of cell colony formation,as well as displayed potent effects on inducing G2/M phase cell cycle arrest and promoting apoptosis.Importantly,13n exhibited enhanced and adequate liver microsomal stability in human and rat liver microsomes,and also exhibited a moderate half-life(T_(1/2)=0.938 h)in vivo.Meanwhile,13n demonstrated effective antitumor effects in vivo in suppressing tumor growth in the MGC-803xenograft model(tumor growth inhibition(TGI)value was 76.4%at the dosage of 30 mg kg^(-1)day^(-1))with a good safety profile.Collectively,these results revealed that 13n represents a promising tubulin polymerization inhibitor that deserves further investigation for its efficacy in treating gastric cancers.展开更多
The Eurasian beaver(Castor fiber Linnaeus,1758)can be considered a hydrological ecosystem engineer as it shapes environmental characteristics through its building activities and feeding behaviour.Even if several studi...The Eurasian beaver(Castor fiber Linnaeus,1758)can be considered a hydrological ecosystem engineer as it shapes environmental characteristics through its building activities and feeding behaviour.Even if several studies have so far reported beaver impact on multi-taxon biodiversity and forest regeneration,there is a lack of research on forest stand structure evolution following beaver direct activity on trees.This represents a pivotal topic for predicting restoration outcomes and reccommending sound silvicultural and management practices to maintain specific forest conditions.Specifically,the study aims at investigating forest stand structure and tree species diversity changes considering river variability,distance from the riverbank and beaver's gnawing activity intensity.The Eurasian beaver is only recently recolonising the three analysed Mediterranean rivers,but stand structure seems to be already significantly impacted by the species.The number of trees was reduced,increasing mean diameter at breast height at stand level,as most of the youngest and/or smaller trees are entirely cut down.Strongest structural variations can be detected in intensively impacted stands and in the forest portions closer to the riverbank.The absence of a significant effect on most of the diversity indices is likely due to the initially homogeneous composition of the tree layer in each stand and to the limited variety of beaver's diet within the sites.Future resprouting of secondary tree shoots,as well as beaver gnawing activity changes in intensity over time and space,can further produce variations in structural parameters and woody species diversity in the medium-and long-term period.Therefore,it will be crucial to further monitor the long-term effects,as structural shifts can produce significant effects on riparian ecosystem functions.展开更多
As a catalyst of the air cathode in zinc-air batteries,tungstic acid ferrous(FeWO_(4)),a nanoscale transition metal tungstate,shows a broad application prospect in the oxygen reduction reaction(ORR).While FeWO_(4)poss...As a catalyst of the air cathode in zinc-air batteries,tungstic acid ferrous(FeWO_(4)),a nanoscale transition metal tungstate,shows a broad application prospect in the oxygen reduction reaction(ORR).While FeWO_(4)possesses favorable electrochemical properties and thermodynamic stability,its intrinsic semiconductor characteristics result in a relatively slow electron transfer rate,limiting the ORR catalytic activity.In this work,the electronic structure of FeWO_(4)is significantly modulated by introducing phosphorus(P)atoms with abundant valence electrons.The P doping can adjust the electronic structure of FeWO_(4)and then optimize oxygen-containing intermediates'absorption/desorption efficiency to achieve improved ORR activity.Furthermore,the sodium chloride template is utilized to construct a porous carbon framework for anchoring phosphorus-doped iron tungstate(P-FeWO_(4)/PNC).The porous carbon skeleton provides numerous active sites for the absorption/desorption and redox reactions on the P-FeWO_(4)/PNC surface and serves as mass transport channels for reactants and intermediates.The P-FeWO_(4)/PNC demonstrates ORR performance(E1/2=0.86 V vs.RHE).Furthermore,the zinc-air batteries incorporating the P-FeWO_(4)/PNC composite demonstrate an increased peak power density(172.2 mW·cm^(-2)),high specific capacity(810.1 mAh·g^(-1)),and sustained long-term cycling stability lasting up to 240 h.This research not only contributes to the advancement of cost-effective tungsten-based non-precious metallic ORR catalysts,but also guides their utilization in zinc-air batteries.展开更多
Pore structure engineering has been acknowledged as suitable approach to creating active sites and en-hancing ion transport capabilities of hard carbon anodes.However,conventional porous carbon materials exhibit high ...Pore structure engineering has been acknowledged as suitable approach to creating active sites and en-hancing ion transport capabilities of hard carbon anodes.However,conventional porous carbon materials exhibit high BET and surface defects.Additionally,the sodium storage mechanism predominantly occurs in the slope region.This contradicts practical application requirements because the capacity of the plateau region is crucial for determining the actual capacity of batteries.In our work,we prepared a novel“core-shell”carbon framework(CNA1200).Introducingclosedporesand carboxylgroupsinto coal-basedcarbon materials to enhance its sodium storage performance.The closed pore structure dominates in the“core”structure,which is attributed to the timely removal of sodium hydroxide(NaOH)to prevent further for-mation of active carbon structure.The presence of closed pores is beneficial for increasing sodium ion storage in the low-voltage plateau region.And the“shell”structure originates from coal tar pitch,it not only uniformly connects hard carbon particles together to improve cycling stability,but is also rich in carboxyl groups to enhance the reversible sodium storage performance in slope region.CNA1200 has ex-cellent electrochemical performance,it exhibits a specific capacity of 335.2 mAh g^(−1)at a current density of 20 mA g^(−1)with ICE=51.53%.In addition,CNA1200 has outstanding cycling stability with a capac-ity retention of 91.8%even when cycling over 200 times.When CNA1200 is used as anode paired with Na_(3)V_(2)(PO_(4))_(3)cathode,it demonstrates a capacity of 109.54 mAh g^(−1)at 0.1 C and capacity retention of 94.64%at 0.5 C.This work provides valuable methods for regulating the structure of sodium-ion battery(SIBs)anode and enhances the potential for commercialization.展开更多
In this study,polysaccharides were extracted from blueberry fruit(BFP)and isolated to 3 components(BFP-1,BFP-2 and BFP-3).The molecular weight,monosaccharide composition,characteristic groups,microscopic morphology,an...In this study,polysaccharides were extracted from blueberry fruit(BFP)and isolated to 3 components(BFP-1,BFP-2 and BFP-3).The molecular weight,monosaccharide composition,characteristic groups,microscopic morphology,and triple helical conformation of the polysaccharides were characterized using high performance permeation chromatography,high performance liquid chromatography,gas chromatographymass spectrometry,Fourier transform infrared spectrometer,scanning electron microscope and Congo red staining.Moreover,the hypolipidemic and immunological activities of the polysaccharides were also assessed.Results showed that the molecular weights of polysaccharides BFP-1,BFP-2,and BFP-3 were 5.547×10^(4),5.671×10^(4),and 3.951×10^(4)Da,respectively,the main monosaccharides were glucose(Glc),galactose(Gal)and arabinose(Ara),but BFP-3 was mainly composed of galacturonic acid(Gal A),Glc,Gal,and Ara.The backbone of BFP-1 was→4)-Glcp-(1→,which branches to Ara and xylose(Xyl)residues,while the backbone of BFP-2 was→5)-Araf-(1→,which branches to Xyl,Glc,rhamnose(Rha)and Gal residues,in particularly,BFP-3 has a more complex branching with a→3,6)-Galp-(1→)backbone,the side chain is dominated by Araf-(1→).Blueberry polysaccharides are pyran-type polysaccharides withα-glycosidic bonds,and BFP-1 has a typical triple-helical structure.The activity assay revealed that the binding of BFP-3 to sodium glycylcholate hydrate and sodium taurocholate was 79.95%and 78.50%,respectively,indicating that it had better hypolipidemic activity than the others.Immunoactivity assay showed that BFP promoted NO secretion through activating the NF-κB signalling pathway in RAW264.7 cells,which played a role in enhancing the immune function of the organism.These findings may provide a reference for the development and application of blueberry polysaccharides in functional food and medicine.展开更多
Situated in the southwestern Pacific,the Tonga-Kermadec subduction zone is separated into two parts by the Louisvlle Ridge Seamount Chain(LRSC),i.e.,the Tanga subduction zone and the Kermadec subduction zone.Known for...Situated in the southwestern Pacific,the Tonga-Kermadec subduction zone is separated into two parts by the Louisvlle Ridge Seamount Chain(LRSC),i.e.,the Tanga subduction zone and the Kermadec subduction zone.Known for its vigorous volcanic activity,frequent large earthquakes,rapid plate subduction,and distinctive subducting plate morphology,this subduction zone provides valuable insights into its structures,dynamics,and associated geohazards.This study compiles geological and geophysical datasets in this region,including seismicity,focal mechanisms,seismic reflection and refraction profiles,and seismic tomography,to understand the relationship between lithospheric structures of the subduction system and associated seismicity-volcanic activities.Our analysis suggests that variations in overlying sediment thickness,subduction rate,and subduction angle significantly influence the lithospheric deformation processes within the Tonga-Kermadec subduction system.Furthermore,these factors contribute to the notable differences in seismicity and volcanism observed between the Tonga subduction zone and the Kermadec subduction zone.This study enhances our understanding of plate tectonics by providing insights into the interplay between subduction dynamics and lithospheric deformation,which are crucial for analyzing geological and geophysical behaviors in similar subduction environments.展开更多
The Reliability-Based Design Optimization(RBDO)of complex engineering structures considering uncertainties has problems of being high-dimensional,highly nonlinear,and timeconsuming,which requires a significant amount ...The Reliability-Based Design Optimization(RBDO)of complex engineering structures considering uncertainties has problems of being high-dimensional,highly nonlinear,and timeconsuming,which requires a significant amount of sampling simulation computation.In this paper,a basis-adaptive Polynomial Chaos(PC)-Kriging surrogate model is proposed,in order to relieve the computational burden and enhance the predictive accuracy of a metamodel.The active learning basis-adaptive PC-Kriging model is combined with a quantile-based RBDO framework.Finally,five engineering cases have been implemented,including a benchmark RBDO problem,three high-dimensional explicit problems,and a high-dimensional implicit problem.Compared with Support Vector Regression(SVR),Kriging,and polynomial chaos expansion models,results show that the proposed basis-adaptive PC-Kriging model is more accurate and efficient for RBDO problems of complex engineering structures.展开更多
Polycyclic polyprenylated acylphloroglucinols(PPAPs)represent a distinct subclass of specialized metabolites predominantly found in the plant kingdom,particularly within the Guttiferae(Clusiaceae)family.These compound...Polycyclic polyprenylated acylphloroglucinols(PPAPs)represent a distinct subclass of specialized metabolites predominantly found in the plant kingdom,particularly within the Guttiferae(Clusiaceae)family.These compounds exhibit remarkable structural diversity and a wide range of biological activities.Seco-and nor-PPAPs,two unique variants of PPAPs with diverse skeletal structures,have been extensively investigated.As of June 2023,200 compounds have been isolated from four genera,with Hypericum being the primary source.Notably,115 of these compounds were identified in the past four years,indicating a significant increase in research activity.Seco-and nor-PPAPs can be categorized into six main subgroups based on the original PPAP scaffolds.Biological studies have revealed their potential in various therapeutic applications,including anti-cancer,anti-inflammatory,hepatoprotective,anti-Alzheimer’s disease(anti-AD),multidrug resistance(MDR)reversal,anti-depressant,neuroprotective,and immunosuppressive effects.This review provides a comprehensive overview of the occurrence,structures,and bioactivities of natural seco-and nor-PPAPs,offering valuable insights for the further development of PPAPs.展开更多
Plant-based fermentations provide an untapped source for novel biotechnological applications.In this study,a probiotic named Lactobacillus fermentum 21828 was introduced to ferment Lentinus edodes.Polysaccharides were...Plant-based fermentations provide an untapped source for novel biotechnological applications.In this study,a probiotic named Lactobacillus fermentum 21828 was introduced to ferment Lentinus edodes.Polysaccharides were extracted from fermented and non-fermented L.edodes and purified via DEAE-52 and Sephadex G-100.The components designated F-LEP-2a and NF-LEP-2a were analyzed by FT-IR,HPGPC,HPAEC,SEM,GC-MS and NMR.The results revealed that probiotic fermentation increased the molecular weight from 1.16×10^(4) Da to 1.87×10^(4) Da and altered the proportions of glucose,galactose and mannose,in which glucose increased from 45.94%to 48.16%.Methylation analysis and NMR spectra indicated that F-LEP-2a and NF-LEP-2a had similar linkage patterns.Furthermore,their immunomodulatory activities were evaluated with immunosuppressive mice.NF-LEP and F-LEP improved immune organ indices,immunoglobulin(Ig G and Ig M)and cytokines concentrations;restored the antioxidation capacity of liver;and maintained the balance of gut microbiota.F-LEP displayed better moderating effects on the spleen index,immunoglobulin,cytokines and the diversity of gut microbiota than NF-LEP(200,400 mg/kg).Our study provides an efficient and environment-friendly way for the structural modification of polysaccharides,which helps to enhance their biological activity and promote their wide application in food,medicine and other fields.展开更多
Single-atom catalysts are promising for H_(2)O_(2) photosynthesis from O_(2) and H_(2)O,but their efficiency is still limited by the ill-defined electronic structure.In this study,Co single-atoms with unique four plan...Single-atom catalysts are promising for H_(2)O_(2) photosynthesis from O_(2) and H_(2)O,but their efficiency is still limited by the ill-defined electronic structure.In this study,Co single-atoms with unique four planar N-coordination and one axial P-coordination(Co-N_(4)P_(1))are decorated on the lateral edges of nanorod-like crystalline g-C_(3)N_(4)(CCN)photocatalysts.Significantly,the electronic structures of central Co as active sites for O_(2) reduction reaction(ORR)and planar N-coordinator as active sites for H_(2)O oxidation reaction(WOR)in Co-N_(4)P_(1) can be well regulated by the synergetic effects of introducing axial P-coordinator,in contrast to the decorated Co single-atoms with only four planar N-coordination(Co-N_(4)).Specifically,directional photoelectron accumulation at central Co active sites,induced by an introduced midgap level in Co-N_(4)P_(1),mediates the ORR active sites from 4e–-ORR-selective terminal–NH_(2) sites to 2e–-ORR-selective Co sites,moreover,an elevated d-band center of Co 3d orbital strengthens ORR intermediate*OOH adsorption,thus jointly facilitating a highly selective and active 2e^(–)-ORR pathway to H_(2)O_(2) photosynthesis.Simultaneously,a downshifted p-band center of N_(2)p orbital in Co-N_(4)P_(1) weakens WOR intermediate*OH adsorption,thus enabling a preferable 2e^(–)-WOR pathway toward H_(2)O_(2) photosynthesis.Subsequently,Co-N_(4)P_(1) exhibits exceptional H_(2)O_(2) photosynthesis efficiency,reaching 295.6μmol g^(-1) h^(-1) with a remarkable solar-to-chemical conversion efficiency of 0.32%,which is 15 times that of Co-N_(4)(19.2μmol g^(-1) h^(-1))and 10 times higher than CCN(27.6μmol g^(-1) h^(-1)).This electronic structure modulation on single-atom catalysts offers a promising strategy for boosting the activity and selectivity of H_(2)O_(2) photosynthesis.展开更多
Cyclocarya paliurus(Batalin)Iljinskaja,as a unique and rare monocotyledonous plant in Southern China,is a promising and economical Chinese herbal medicine and functional food.People have conducted a number of research...Cyclocarya paliurus(Batalin)Iljinskaja,as a unique and rare monocotyledonous plant in Southern China,is a promising and economical Chinese herbal medicine and functional food.People have conducted a number of research on C.paliurus because of its rich triterpenoids.However,no comprehensive review has illustrated the composition and pharmacological activity of triterpenoids from C.paliurus.This review summarizes 177 triterpenoids from different parts of C.paliurus.The structures of compounds were elucidated,and their biosynthesis was inferred.The biological activities of compounds and triterpenoid-rich extracts,including anti-diabetes,antihyperlipidemia,anti-inflammatory,anticancer or cytotoxicity,antioxidation,etc.,were discussed.C.paliurus can be an important and valuable supplement to the food market.This review provides a reference for the further research and application of C.paliurus triterpenoids in the fields of foods and pharmaceuticals.展开更多
文摘To expand the study on the structures and biological activities of the anthracyclines anticancer drugs and reduce their toxic side effects,the new anthraquinone derivatives,9‑pyridylanthrahydrazone(9‑PAH)and 9,10‑bispyridylanthrahydrazone(9,10‑PAH)were designed and synthesized.Utilizing 9‑PAH and 9,10‑PAH as promising anticancer ligands,their respective copper complexes,namely[Cu(L1)Cl_(2)]Cl(1)and{[Cu_(4)(μ_(2)‑Cl)_(3)Cl_(4)(9,10‑PAH)_(2)(DMSO)_(2)]Cl_(2)}_(n)(2),were subsequently synthesized,where the new ligand L1 is formed by coupling two 9‑PAH ligands in the coordination reaction.The chemical and crystal structures of 1 and 2 were elucidated by IR,MS,elemental analysis,and single‑crystal X‑ray diffraction.Complex 1 forms a mononuclear structure.L1 coordinates with Cu through its three N atoms,together with two Cl atoms,to form a five‑coordinated square pyramidal geometry.Complex 2 constitutes a polymeric structure,wherein each structural unit centrosymmetrically encompasses two five‑coordinated binuclear copper complexes(Cu1,Cu2)of 9,10‑PAH,with similar square pyramidal geometry.A chlorine atom(Cl_(2)),located at the symmetry center,bridges Cu1 and Cu1A to connect the two binuclear copper structures.Meanwhile,the two five‑coordinated Cu2 atoms symmetrically bridge the adjacent structural units via one coordinated Cl atom,respectively,thus forming a 1D chain‑like polymeric structure.In vitro anticancer activity assessments revealed that 1 and 2 showed significant cytotoxicity even higher than cisplatin.Specifically,the IC_(50)values of 2 against HeLa‑229 and SK‑OV‑3 cancer cell lines were determined to be(5.92±0.32)μmol·L^(-1)and(6.48±0.39)μmol·L^(-1),respectively.2 could also block the proliferation of HeLa‑229 cells in S phase and significantly induce cell apoptosis.In addition,fluorescence quenching competition experiments suggested that 2 might interact with DNA by an intercalative binding mode,offering insights into its underlying anticancer mechanism.CCDC:2388918,1;2388919,2.
文摘Two Gd_(2)complexes,namely[Gd_(2)(dbm)_(2)(HL_(1))_(2)(CH_(3)OH)_(2)]·4CH_(3)OH(1)and[Gd_(2)(dbm)_(2)(L_(2))_(2)(CH_(3)OH)_(2)]·2CH_(3)OH(2),where H_(3)L_(1)=(Z)-N'-[4-(diethylamino)-2-hydroxybenzylidene]-2-hydroxyacetohydrazide,H_(2)L_(2)=(E)-N'-(5-bromo-2-hydroxy-3-methoxybenzylidene)nicotinohydrazide,Hdbm=dibenzoylmethane,have been constructed by adopting the solvothermal method.Structural characterization unveils that both complexes 1 and 2 are constituted by two Gd^(3+)ions,two dbm-ions,two CH_(3)OH molecules,and two polydentate Schiff-base ligands(HL_(1)^(2-)or L_(2)^(2-)).In addition,complex 1 contains four free methanol molecules,whereas complex 2 harbors two free methanol molecules.By investigating the interactions between complexes 1 and 2 and four types of bacteria(Bacillus subtilis,Escherichia coli,Staphylococcus aureus,Candida albicans),it was found that both complexes 1 and 2 exhibited potent antibacte-rial activities.The interaction mechanisms between the ligands H_(3)L_(1),H_(2)L_(2),complexes 1 and 2,and calf thymus DNA(CT-DNA)were studied using ultraviolet-visible spectroscopy,fluorescence titration,and cyclic voltammetry.The results demonstrated that both complexes 1 and 2 can intercalate into CT-DNA molecules,thereby inhibiting bacterial proliferation to achieve the antibacterial effects.CCDC:2401116,1;2401117,2.
基金support from the National Natural Science Foundation of China(No:52061040)China Postdoctoral Science Foundation(No:2021M692512)+1 种基金Opening Project of Material Corrosion and Protection Key Laboratory of Sichuan Province(No:2023CL01)Open Projects of Key Laboratory of Advanced Technologies of Materials,Ministry of Education China,Southwest Jiaotong University(No:KLATM202003).
文摘Integrating a heterogeneous structure can significantly enhance the strength-ductility synergy of composites.However,the relationship between hetero-deformation induced(HDI)strain hardening and dislocation activity caused by heterogeneous structures in the magnesium matrix composite remains unclear.In this study,a dual-heterogeneous TiC/AZ61 composite exhibits significantly improved plastic elongation(PEL)by nearly one time compared to uniform FG composite,meanwhile maintaining a high strength(UTS:417 MPa).This is because more severe deformation inhomogeneity in heterogeneous structure leads to more geometrically necessary dislocations(GNDs)accumulation and stronger HDI stress,resulting in higher HDI hardening compared to FG and CG composites.During the early stage of plastic deformation,the pile-up types of GND in the FG zone and CG zone are significantly different.GNDs tend to form substructures in the FG zone instead of the CG zone.They only accumulate at grain boundaries of the CG region,thereby leading to obviously increased back stress in the CG region.In the late deformation stage,the elevated HDI stress activates the new〈c+a〉dislocations in the CG region,resulting in dislocation entanglements and even the formation of substructures,further driving the high hardening in the heterogeneous composite.However,For CG composite,〈c+a〉dislocations are not activated even under large plastic strains,and only〈a〉dislocations pile up at grain boundaries and twin boundaries.Our work provides an in-depth understanding of dislocation variation and HDI hardening in heterogeneous magnesium-based composites.
基金supported by National Natural Science Foundation of China(No.523B2070,No.52225606).
文摘Polymeric perylene diimide(PDI)has been evidenced as a good candidate for photocatalytic water oxidation,yet the origin of the photocatalytic oxygen evolution activity remains unclear and needs further exploration.Herein,with crystal and atomic structures of the self-assembled PDI revealed from the X-ray diffraction pattern,the electronic structure is theoretically illustrated by the first-principles density functional theory calculations,suggesting the suitable band structure and the direct electronic transition for efficient photocatalytic oxygen evolution over PDI.It is confirmed that the carbonyl O atoms on the conjugation structure serve as the active sites for oxygen evolution reaction by the crystal orbital Hamiltonian group analysis.The calculations of reaction free energy changes indicate that the oxygen evolution reaction should follow the reaction pathway of H_(2)O→^(*)OH→^(*)O→^(*)OOH→^(*)O_(2)with an overpotential of 0.81 V.Through an in-depth theoretical computational analysis in the atomic and electronic structures,the origin of photocatalytic oxygen evolution activity for PDI is well illustrated,which would help the rational design and modification of polymeric photocatalysts for efficient oxygen evolution.
文摘2-substituted-1-amino-o-carboranes 2-R-1-NH_(2)-o-C_(2)B_(10)H_(10)(R=CH_(3),1a;R=Ph,1b)were synthesized and the reactions of these compounds with the yttrium dialkyl complex[Y(L)(CH_(2)SiMe3)_(2)](L=[2-(2,5-Me_(2)C_(4)H_(2)N)C_(6)H4NC(Ph)=NDipp]-,Dipp=2,6-iPr_(2)C_(6)H_(3))were investigated.The 1H NMR spectroscopy indicate that the reaction of ytrrium dialkyl complex with one equivalent of 2-R-1-NH_(2)-o-C_(2)B_(10)H_(10) produce the mixture of ytrrium alkyl-amido complex[Y(L)(2-R-1-NH-o-C_(2)B_(10)H_(10))(CH_(2)SiMe3)](R=CH_(3),2a;R=Ph,2b)and bis(amido)complex[Y(L)(2-R-1-NH-o-C_(2)B_(10)H_(10))_(2)](R=CH_(3),3a;R=Ph,3b).The yttrium bridging imido complex[Y(L)(2-CH_(3)-1-N-o-C_(2)B_(10)H_(10))]_(2)(4a)was obtained by heating the mixture at 55℃for 12 h.Complex 3a was isolated and characterized by treating the yttrium dialkyl complex with two equivalents of 1a.The structures of complexes 3a and 4a were verified by single-crystal Xray diffraction.CCDC:2424136,3a;2424137,4a.
文摘A novel 3D metal-organic framework(MOF)[Pr_(2)(L)_(3)(H_(2)O)5·H_(2)O]n(Pr-1),(H_(2)L=4,4'-oxybis(benzoic acid))with a rare structure of broken layer net,was constructed under the condition of solvothermal synthesis.The struc-ture and crystal net were analyzed and characterized.This rod net of Pr-1 is new to both RCSR and ToposPro data-bases,and is named as rn-12 as suggested.Due to the luminescent properties of H_(2)L and Pr(Ⅲ),the solid-state fluo-rescence property and sensing performance(solvents and metal ions)of Pr-1 were investigated.The sensing experi-ments indicated that Pr-1 could act as a fluorescence sensor to detect Cd^(2+)ions with good sensitivity.In addition,antibacterial activities show that Pr-1 exhibited stronger antibacterial activity against Escherichia coli(E.coli),Staphylococcus aureus(S.aureus),and Bacillus subtilis(B.subtilis)compared to synthetic materials.
基金funded by the National Natural Science Foundation of China(No.42174104,No.42204089)the Hubei Provincial Natural Science Foundation of China(2022CFB350)+1 种基金the Basic Research Fund of Institute of Seismology,China Earthquake Administration(IS202326341)Open Fund ofWuhan,Gravitation and Solid Earth Tides,National Observation and Research Station(WHYWZ202108,WHYWZ202301)。
文摘Controlled by the squeezing collision between the Yangtze block and the North China block and the left movement of the Tanlu fault, the Xu-Su region developed into an arc-shaped nappe structure, and many destructive earthquakes occurred in its periphery. The geological structure of this area is complex, and there is the possibility of moderate and strong earthquakes. To further explore the crust density structure and identify the main faults and deep structural features in the Xu-Su region, based on the observed seismic data and gravity/GNSS co-site observation data, combined with the EGM2008 global gravity field model, we obtained the density of three-dimensional structure using cross gradient method joint inversion. Based on this, a geological model of the Xu-Su region was established. The results show that the crustal density anomaly amplitude within 0-25 km of the Xu-Su region ranges from-280 to 490 kg/m3, showing a zonal distribution in east-west direction and a segmented north-south direction. There are several density anomalies in the shallow(0-4 km) region at Tongshan, Huaibei, Xiayi, Woyang, etc. The density anomalies are significantly correlated with the distribution of regional faults. The density structure is divided into two large regions by Subei fault, which can be further divided along the eastwest Kouziji-Nanzhao fault and Guzhen-Huaiyuan fault. The earthquakes are obviously related to the regional fault activity and the spatial distribution of abnormal bodies. The earthquake-prone areas(5-15 km) correspond to the abnormal density mutation zone, upper uplift zone, and transformation zone near Xiaoxian, Tongshan, and Xushuanglou faults. The comprehensive results show three weak seismic activity areas in the whole region, which are located near the Huaibei, Xiaoxian, and Wohe faults. The results provide theoretical support for seismic risk analysis in this area, and these three areas should be emphasized in future seismic hazard analysis.
基金the Fundamental Research Funds for the Central Universities(KYCYXT2022011,KJYQ2024014)the National Key Research and Development Program of China(2021YFD1700102)for the generous financial support for our programs.
文摘To develop new environmentally friendly fungicides,we designed and synthesized a novel series of D/Lconfigured camphor oxime ester derivatives based on the natural product camphor as a lead compound.We investigated the in vitro antifungal activity of these compounds against six common plant pathogenic fungi.Among them,compounds B1-6,B1-17 and B2-6 displayed great in vitro activity against Rhizoctonia solani with EC50 values of 7.28,4.64,and 7.62μg/mL.The HOMO and LUMO calculations indicated that strong electronwithdrawing halogen elements exhibit better activity compared to electron-donating alkyl groups.Preliminary mechanistic studies,using SEM and TEM,indicated that compound B1-17 induced disordered entanglement of hyphae,shrinkage of hyphal surfaces,and vacuole swelling and rupture,which disrupted normal hyphal growth.Additionally,compound B1-17 induced the production and accumulation of ROS,disrupted MMP,and effectively inhibited the germination and formation of sclerotia in Rhizoctonia solani.These compounds hold potential as new antifungal agents for further research.
文摘Hydrocracking technology represents a crucial position in the conversion of heavy oil and the transformation development from oil refining to the chemical industry.The properties of catalysts are one of the key factors in the hydrocracking process.As the main acidic component of hydrocracking catalyst,the influence of zeolite properties on the reaction performance has been the focus of research.In this study,a series of NiMo/Al_(2)O_(3)-Y catalysts were prepared using different Y zeolites as acidic components,and their performances in the hydrocracking of n-C_(10)were also evaluated.The structure-activity relationship between Y zeolite and the cracking performance of n-C_(10)was investigated with machine learning.First,a database of the physical and chemical properties of Y zeolite and their performance was established,and the correlation analysis was also conducted.Parameters such as the cell constant,acid content,acid strength,B/L ratio,mesopore volume,micropore volume of Y zeolite,and the reaction temperature were selected as independent variables.The conversion of n-C_(10)and the ratios of products C_(3)/C_(7)and i-C_(4)/n-C_(4)were selected as dependent variables.A model was established by the random forest algorithm and a new zeolite was predicted based on it.The results of model prediction were in good agreement with the experimental results.The R^(2)of the n-C_(10)conversion,C_(3)/C_(7)ratio,and i-C_(4)/n-C_(4)ratio were 0.9866,0.9845,and 0.9922,and the minimum root mean square error values were 0.0163,0.101,and 0.0211,respectively.These results can provide reference for the development of high performance hydrocracking catalyst and technology.
基金supported by the National Natural Science Foundation of China(Nos.82273782 and U2004123)Training Program for Young Key Teachers of Colleges and Universities in Henan Province(No.2023GGJS008)。
文摘In this work,we employed a ring-opening strategy to develop a series of novel N-benzyl arylamide derivatives as tubulin polymerization inhibitors.Notably,13n(MY-1388)exhibited remarkable antiproliferative potency on fifteen human cancer cell lines,with half maximal inhibitory concentration(IC_(50))values ranging from 8 nmol/L to 48 nmol/L.Furthermore,13n effectively suppressed tubulin polymerization by targeting the colchicine-binding site(IC_(50)=0.62μmol/L).13n also exhibited significant inhibition of cell colony formation,as well as displayed potent effects on inducing G2/M phase cell cycle arrest and promoting apoptosis.Importantly,13n exhibited enhanced and adequate liver microsomal stability in human and rat liver microsomes,and also exhibited a moderate half-life(T_(1/2)=0.938 h)in vivo.Meanwhile,13n demonstrated effective antitumor effects in vivo in suppressing tumor growth in the MGC-803xenograft model(tumor growth inhibition(TGI)value was 76.4%at the dosage of 30 mg kg^(-1)day^(-1))with a good safety profile.Collectively,these results revealed that 13n represents a promising tubulin polymerization inhibitor that deserves further investigation for its efficacy in treating gastric cancers.
基金support of the National Biodiversity Future Center (NBFC) to the University of Padova,the Research Centre for Plant ProtectionCertification (CREA),and the National Research Council (CNR),funded under the National Recovery and Resilience Plan (NRRP)+2 种基金Mission 4 Component 2 Investment 1.4-Call for tender No.3138 of 16 December 2021,rectified by Decree n.3175 of 18 December 2021 of Italian Ministry of University and Research funded by the European Union–NextGenerationEUProject code CN_00000033,Concession Decree No.1034 of 17 June 2022adopted by the Italian Ministry of University and Research,CUP:C93C22002810006,CUP:B83D21014060006,CUP:B83C22002930006,Project title“National Biodiversity Future CenterNBFC”support by Beaver Trust,grant number:1185451
文摘The Eurasian beaver(Castor fiber Linnaeus,1758)can be considered a hydrological ecosystem engineer as it shapes environmental characteristics through its building activities and feeding behaviour.Even if several studies have so far reported beaver impact on multi-taxon biodiversity and forest regeneration,there is a lack of research on forest stand structure evolution following beaver direct activity on trees.This represents a pivotal topic for predicting restoration outcomes and reccommending sound silvicultural and management practices to maintain specific forest conditions.Specifically,the study aims at investigating forest stand structure and tree species diversity changes considering river variability,distance from the riverbank and beaver's gnawing activity intensity.The Eurasian beaver is only recently recolonising the three analysed Mediterranean rivers,but stand structure seems to be already significantly impacted by the species.The number of trees was reduced,increasing mean diameter at breast height at stand level,as most of the youngest and/or smaller trees are entirely cut down.Strongest structural variations can be detected in intensively impacted stands and in the forest portions closer to the riverbank.The absence of a significant effect on most of the diversity indices is likely due to the initially homogeneous composition of the tree layer in each stand and to the limited variety of beaver's diet within the sites.Future resprouting of secondary tree shoots,as well as beaver gnawing activity changes in intensity over time and space,can further produce variations in structural parameters and woody species diversity in the medium-and long-term period.Therefore,it will be crucial to further monitor the long-term effects,as structural shifts can produce significant effects on riparian ecosystem functions.
基金supported by the National Natural Science Foundation of China(NSFC)(Nos.22178148 and 22278193)a Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions.
文摘As a catalyst of the air cathode in zinc-air batteries,tungstic acid ferrous(FeWO_(4)),a nanoscale transition metal tungstate,shows a broad application prospect in the oxygen reduction reaction(ORR).While FeWO_(4)possesses favorable electrochemical properties and thermodynamic stability,its intrinsic semiconductor characteristics result in a relatively slow electron transfer rate,limiting the ORR catalytic activity.In this work,the electronic structure of FeWO_(4)is significantly modulated by introducing phosphorus(P)atoms with abundant valence electrons.The P doping can adjust the electronic structure of FeWO_(4)and then optimize oxygen-containing intermediates'absorption/desorption efficiency to achieve improved ORR activity.Furthermore,the sodium chloride template is utilized to construct a porous carbon framework for anchoring phosphorus-doped iron tungstate(P-FeWO_(4)/PNC).The porous carbon skeleton provides numerous active sites for the absorption/desorption and redox reactions on the P-FeWO_(4)/PNC surface and serves as mass transport channels for reactants and intermediates.The P-FeWO_(4)/PNC demonstrates ORR performance(E1/2=0.86 V vs.RHE).Furthermore,the zinc-air batteries incorporating the P-FeWO_(4)/PNC composite demonstrate an increased peak power density(172.2 mW·cm^(-2)),high specific capacity(810.1 mAh·g^(-1)),and sustained long-term cycling stability lasting up to 240 h.This research not only contributes to the advancement of cost-effective tungsten-based non-precious metallic ORR catalysts,but also guides their utilization in zinc-air batteries.
基金the National Natural Science Foundation of China(No.21978164,22078189 and 22105120)the Outstanding Youth Science Fund of Shaanxi Province(No.2021JC-046)and the Special Support Program for high level talents of Shaanxi Province+3 种基金the Innovation Support Program of Shaanxi Province(2021JZY-001)the Key Research and Development Program of Shaanxi Province(No.2020GY-243)the Special Research Fund of Education Department of Shaanxi(No.20JK0535)the National High-end Foreign Expert Project(No.GDW20186100428).
文摘Pore structure engineering has been acknowledged as suitable approach to creating active sites and en-hancing ion transport capabilities of hard carbon anodes.However,conventional porous carbon materials exhibit high BET and surface defects.Additionally,the sodium storage mechanism predominantly occurs in the slope region.This contradicts practical application requirements because the capacity of the plateau region is crucial for determining the actual capacity of batteries.In our work,we prepared a novel“core-shell”carbon framework(CNA1200).Introducingclosedporesand carboxylgroupsinto coal-basedcarbon materials to enhance its sodium storage performance.The closed pore structure dominates in the“core”structure,which is attributed to the timely removal of sodium hydroxide(NaOH)to prevent further for-mation of active carbon structure.The presence of closed pores is beneficial for increasing sodium ion storage in the low-voltage plateau region.And the“shell”structure originates from coal tar pitch,it not only uniformly connects hard carbon particles together to improve cycling stability,but is also rich in carboxyl groups to enhance the reversible sodium storage performance in slope region.CNA1200 has ex-cellent electrochemical performance,it exhibits a specific capacity of 335.2 mAh g^(−1)at a current density of 20 mA g^(−1)with ICE=51.53%.In addition,CNA1200 has outstanding cycling stability with a capac-ity retention of 91.8%even when cycling over 200 times.When CNA1200 is used as anode paired with Na_(3)V_(2)(PO_(4))_(3)cathode,it demonstrates a capacity of 109.54 mAh g^(−1)at 0.1 C and capacity retention of 94.64%at 0.5 C.This work provides valuable methods for regulating the structure of sodium-ion battery(SIBs)anode and enhances the potential for commercialization.
基金financial support received from the Anhui Provincial Excellent Scientific Research and Innovation Team(2023AH010050)the Key Research and Development Plan of Anhui Province(202204c06020013,202204c06020029)+1 种基金the“Biology and Medicine”key subject of Hefei University(2023xk05)the open research project of Anhui Ecological Fermentation Engineering Research Center for Functional Fruit Beverage(FSKFKT015)。
文摘In this study,polysaccharides were extracted from blueberry fruit(BFP)and isolated to 3 components(BFP-1,BFP-2 and BFP-3).The molecular weight,monosaccharide composition,characteristic groups,microscopic morphology,and triple helical conformation of the polysaccharides were characterized using high performance permeation chromatography,high performance liquid chromatography,gas chromatographymass spectrometry,Fourier transform infrared spectrometer,scanning electron microscope and Congo red staining.Moreover,the hypolipidemic and immunological activities of the polysaccharides were also assessed.Results showed that the molecular weights of polysaccharides BFP-1,BFP-2,and BFP-3 were 5.547×10^(4),5.671×10^(4),and 3.951×10^(4)Da,respectively,the main monosaccharides were glucose(Glc),galactose(Gal)and arabinose(Ara),but BFP-3 was mainly composed of galacturonic acid(Gal A),Glc,Gal,and Ara.The backbone of BFP-1 was→4)-Glcp-(1→,which branches to Ara and xylose(Xyl)residues,while the backbone of BFP-2 was→5)-Araf-(1→,which branches to Xyl,Glc,rhamnose(Rha)and Gal residues,in particularly,BFP-3 has a more complex branching with a→3,6)-Galp-(1→)backbone,the side chain is dominated by Araf-(1→).Blueberry polysaccharides are pyran-type polysaccharides withα-glycosidic bonds,and BFP-1 has a typical triple-helical structure.The activity assay revealed that the binding of BFP-3 to sodium glycylcholate hydrate and sodium taurocholate was 79.95%and 78.50%,respectively,indicating that it had better hypolipidemic activity than the others.Immunoactivity assay showed that BFP promoted NO secretion through activating the NF-κB signalling pathway in RAW264.7 cells,which played a role in enhancing the immune function of the organism.These findings may provide a reference for the development and application of blueberry polysaccharides in functional food and medicine.
基金supported by Special Projects in Universities’Key Fields of Guangdong Province(No.2023ZDZX3017)the 2022 Tertiary Education Scientific Research Project of Guangzhou Municipal Education Bureau(No.202234607)+1 种基金the Guangdong Basic and Applied Basic Research Foundation(No.2025A1515012983)the National Natural Science Foundation of China(Nos.52371059 and 52101358).
文摘Situated in the southwestern Pacific,the Tonga-Kermadec subduction zone is separated into two parts by the Louisvlle Ridge Seamount Chain(LRSC),i.e.,the Tanga subduction zone and the Kermadec subduction zone.Known for its vigorous volcanic activity,frequent large earthquakes,rapid plate subduction,and distinctive subducting plate morphology,this subduction zone provides valuable insights into its structures,dynamics,and associated geohazards.This study compiles geological and geophysical datasets in this region,including seismicity,focal mechanisms,seismic reflection and refraction profiles,and seismic tomography,to understand the relationship between lithospheric structures of the subduction system and associated seismicity-volcanic activities.Our analysis suggests that variations in overlying sediment thickness,subduction rate,and subduction angle significantly influence the lithospheric deformation processes within the Tonga-Kermadec subduction system.Furthermore,these factors contribute to the notable differences in seismicity and volcanism observed between the Tonga subduction zone and the Kermadec subduction zone.This study enhances our understanding of plate tectonics by providing insights into the interplay between subduction dynamics and lithospheric deformation,which are crucial for analyzing geological and geophysical behaviors in similar subduction environments.
基金supported by the National Key R&D Program of China(No.2021YFB1715000)the National Natural Science Foundation of China(No.52375073)。
文摘The Reliability-Based Design Optimization(RBDO)of complex engineering structures considering uncertainties has problems of being high-dimensional,highly nonlinear,and timeconsuming,which requires a significant amount of sampling simulation computation.In this paper,a basis-adaptive Polynomial Chaos(PC)-Kriging surrogate model is proposed,in order to relieve the computational burden and enhance the predictive accuracy of a metamodel.The active learning basis-adaptive PC-Kriging model is combined with a quantile-based RBDO framework.Finally,five engineering cases have been implemented,including a benchmark RBDO problem,three high-dimensional explicit problems,and a high-dimensional implicit problem.Compared with Support Vector Regression(SVR),Kriging,and polynomial chaos expansion models,results show that the proposed basis-adaptive PC-Kriging model is more accurate and efficient for RBDO problems of complex engineering structures.
基金supported by the National Natural Science Foundation for Distinguished Young Scholars(No.81725021)the National Natural Science Foundation of China(Nos.82003633,32100321,and 32300335)+1 种基金the National Natural Science Foundation of Hubei Province(Nos.2023AFB791 and 2023AFB530)the Knowledge Innovation Project of Wuhan Science and Technology Bureau(No.2023020201020534).
文摘Polycyclic polyprenylated acylphloroglucinols(PPAPs)represent a distinct subclass of specialized metabolites predominantly found in the plant kingdom,particularly within the Guttiferae(Clusiaceae)family.These compounds exhibit remarkable structural diversity and a wide range of biological activities.Seco-and nor-PPAPs,two unique variants of PPAPs with diverse skeletal structures,have been extensively investigated.As of June 2023,200 compounds have been isolated from four genera,with Hypericum being the primary source.Notably,115 of these compounds were identified in the past four years,indicating a significant increase in research activity.Seco-and nor-PPAPs can be categorized into six main subgroups based on the original PPAP scaffolds.Biological studies have revealed their potential in various therapeutic applications,including anti-cancer,anti-inflammatory,hepatoprotective,anti-Alzheimer’s disease(anti-AD),multidrug resistance(MDR)reversal,anti-depressant,neuroprotective,and immunosuppressive effects.This review provides a comprehensive overview of the occurrence,structures,and bioactivities of natural seco-and nor-PPAPs,offering valuable insights for the further development of PPAPs.
基金supported by grants from the National Key R&D Program of China(2019YFC1606701)。
文摘Plant-based fermentations provide an untapped source for novel biotechnological applications.In this study,a probiotic named Lactobacillus fermentum 21828 was introduced to ferment Lentinus edodes.Polysaccharides were extracted from fermented and non-fermented L.edodes and purified via DEAE-52 and Sephadex G-100.The components designated F-LEP-2a and NF-LEP-2a were analyzed by FT-IR,HPGPC,HPAEC,SEM,GC-MS and NMR.The results revealed that probiotic fermentation increased the molecular weight from 1.16×10^(4) Da to 1.87×10^(4) Da and altered the proportions of glucose,galactose and mannose,in which glucose increased from 45.94%to 48.16%.Methylation analysis and NMR spectra indicated that F-LEP-2a and NF-LEP-2a had similar linkage patterns.Furthermore,their immunomodulatory activities were evaluated with immunosuppressive mice.NF-LEP and F-LEP improved immune organ indices,immunoglobulin(Ig G and Ig M)and cytokines concentrations;restored the antioxidation capacity of liver;and maintained the balance of gut microbiota.F-LEP displayed better moderating effects on the spleen index,immunoglobulin,cytokines and the diversity of gut microbiota than NF-LEP(200,400 mg/kg).Our study provides an efficient and environment-friendly way for the structural modification of polysaccharides,which helps to enhance their biological activity and promote their wide application in food,medicine and other fields.
文摘Single-atom catalysts are promising for H_(2)O_(2) photosynthesis from O_(2) and H_(2)O,but their efficiency is still limited by the ill-defined electronic structure.In this study,Co single-atoms with unique four planar N-coordination and one axial P-coordination(Co-N_(4)P_(1))are decorated on the lateral edges of nanorod-like crystalline g-C_(3)N_(4)(CCN)photocatalysts.Significantly,the electronic structures of central Co as active sites for O_(2) reduction reaction(ORR)and planar N-coordinator as active sites for H_(2)O oxidation reaction(WOR)in Co-N_(4)P_(1) can be well regulated by the synergetic effects of introducing axial P-coordinator,in contrast to the decorated Co single-atoms with only four planar N-coordination(Co-N_(4)).Specifically,directional photoelectron accumulation at central Co active sites,induced by an introduced midgap level in Co-N_(4)P_(1),mediates the ORR active sites from 4e–-ORR-selective terminal–NH_(2) sites to 2e–-ORR-selective Co sites,moreover,an elevated d-band center of Co 3d orbital strengthens ORR intermediate*OOH adsorption,thus jointly facilitating a highly selective and active 2e^(–)-ORR pathway to H_(2)O_(2) photosynthesis.Simultaneously,a downshifted p-band center of N_(2)p orbital in Co-N_(4)P_(1) weakens WOR intermediate*OH adsorption,thus enabling a preferable 2e^(–)-WOR pathway toward H_(2)O_(2) photosynthesis.Subsequently,Co-N_(4)P_(1) exhibits exceptional H_(2)O_(2) photosynthesis efficiency,reaching 295.6μmol g^(-1) h^(-1) with a remarkable solar-to-chemical conversion efficiency of 0.32%,which is 15 times that of Co-N_(4)(19.2μmol g^(-1) h^(-1))and 10 times higher than CCN(27.6μmol g^(-1) h^(-1)).This electronic structure modulation on single-atom catalysts offers a promising strategy for boosting the activity and selectivity of H_(2)O_(2) photosynthesis.
基金financially supported by the National Natural Science Foundation of China(31960090,32160562)the Natural Science Foundation of Jiangxi Province(20224BAB215046)the Project Program of State Key Laboratory of Food Science and Resources,Nanchang University(SKLF-ZZB-202129,SKLF-ZZB-202324,SKLF-KF-202216)。
文摘Cyclocarya paliurus(Batalin)Iljinskaja,as a unique and rare monocotyledonous plant in Southern China,is a promising and economical Chinese herbal medicine and functional food.People have conducted a number of research on C.paliurus because of its rich triterpenoids.However,no comprehensive review has illustrated the composition and pharmacological activity of triterpenoids from C.paliurus.This review summarizes 177 triterpenoids from different parts of C.paliurus.The structures of compounds were elucidated,and their biosynthesis was inferred.The biological activities of compounds and triterpenoid-rich extracts,including anti-diabetes,antihyperlipidemia,anti-inflammatory,anticancer or cytotoxicity,antioxidation,etc.,were discussed.C.paliurus can be an important and valuable supplement to the food market.This review provides a reference for the further research and application of C.paliurus triterpenoids in the fields of foods and pharmaceuticals.
