Redox-active organic compounds have received much attention as high-capacity electrodes for rechargeable batteries.However,the high solubility in organic electrolytes during charge and discharge processes hinders the ...Redox-active organic compounds have received much attention as high-capacity electrodes for rechargeable batteries.However,the high solubility in organic electrolytes during charge and discharge processes hinders the practical exploitation of organic compounds.This study presents a cobalt-based metal–organic coordination compound with bifunctional coordinated water(Co-MOC-H_(2)O)for sodium-ion storage.The coordinated water enhances interactions between sodium ions and nitrogen atoms in organic ligands through chelation,activating the inert sodium-ion storage sites(C=N).Moreover,the stable hydrogen bonded framework formed by the coordinated water molecules prevents the active organic compounds from dissolving into the electrolyte,thereby enhancing cycling stability.With the bifunctional coordinated water molecules,the Co-MOC-H_(2)O electrode delivers a high capacity of 403 mAh g^(-1)at 0.2 A g^(-1)over 600 cycles and exhibits a capacity retention of 77.9%at 2 A g^(-1)after 1100 cycles.This work highlights the crucial role of the coordinated water molecules in constructing high capacity and long-life sodium-ion storage materials.展开更多
AIM:To investigate the genetic basis of Weill-Marchesani syndrome(WMS)in a Chinese family and clarify the pathogenic mechanism of novel ADAMTS17 mutations.METHODS:Comprehensive clinical assessments and genetic analyse...AIM:To investigate the genetic basis of Weill-Marchesani syndrome(WMS)in a Chinese family and clarify the pathogenic mechanism of novel ADAMTS17 mutations.METHODS:Comprehensive clinical assessments and genetic analyses were performed on a Chinese family with two affected siblings.Whole-exome sequencing(WES)was conducted for the proband and other family members.Bioinformatics tools were used to evaluate the conservation,predicted pathogenicity,and structural effects of the identified ADAMTS17 variants.In addition,protein structure modeling was applied to assess the functional impacts of the mutations.RESULTS:The proband(a 32-year-old male)and his elder sister(42y)presented typical clinical features of WMS,including short stature,brachydactyly,high myopia,ectopia lentis,and secondary glaucoma.WES identified a novel compound heterozygous mutation in ADAMTS17:a splicing mutation(c.451-2A>G)inherited from the father and a missense mutation(c.1043G>A;p.C348Y)inherited from the mother.The splicing mutation disrupted normal mRNA splicing and processing,leading to premature translation termination.The missense mutation,which is located in the metalloprotease catalytic domain,was predicted to abolish a critical disulfide bond,thereby impairing protein stability.Both mutations exhibited high evolutionary conservation and were predicted to be pathogenic by multiple bioinformatics algorithms.CONCLUSION:A novel compound heterozygous mutation in ADAMTS17 is identified in this WMS-affected Chinese family,and its pathogenicity is verified via bioinformatics analysis and protein structural modeling.These findings are expected to facilitate the genetic diagnosis of WMS and deepen the understanding of its molecular pathogenesis.展开更多
Prussian blue analogs(PBAs)are considered one of the excellent cathode materials for sodium-ion batteries due to their low cost and high theoretical specific capacity,especially sodium-rich iron-based PBAs(FeHCF)can p...Prussian blue analogs(PBAs)are considered one of the excellent cathode materials for sodium-ion batteries due to their low cost and high theoretical specific capacity,especially sodium-rich iron-based PBAs(FeHCF)can provide higher energy density.FeHCF has a poor charge/discharge platform stability at high voltages(FeC_(6)moiety),which is mainly affected by its coordination environment.In this research,Cu^(+)(six-coordinated),which is close to the ionic radius of Fe^(2+),was used for substitution,the FeC_(6)vacancies of FeHCF were reduced,and the coordination environment was optimized.The low Cu^(+)-substituted FeHCF(Cu^(+)0.625)has an optimal electrochemical performance at 8.5 mA/g with a reversible specific capacity of 142 mA h/g and FeC_(6)moiety contribution of more than 68 mA h/g,which is superior to that of unmodified and other Cu^(2+)-substituted FeHCFs.In situ tests demonstrate the reversible structural stability of the Cu^(+)0.625,supporting the stability of their high-voltage platform capacity.This Cu^(+)substitution strategy further enriches the approach to optimize the coordination environment of sodium-rich FeHCF.展开更多
Temperature has a substantial impact on the emission of biogenic volatile organic compounds(BVOCs).Moder-ate warm temperatures,e.g.,30–40°C,could boost plant metabolism,increasing BVOC emissions.Against the back...Temperature has a substantial impact on the emission of biogenic volatile organic compounds(BVOCs).Moder-ate warm temperatures,e.g.,30–40°C,could boost plant metabolism,increasing BVOC emissions.Against the backdrop of global warming,plants emit more BVOCs to cope with thermal stress,leading to elevated concen-trations of tropospheric ozone(O_(3))and secondary organic aerosols(SOA).In recent years,a considerable body of research has explored the interaction between tree species and BVOCs under the influence of various environ-mental factors.Although many studies have examined explored the temperature dependence of BVOC emissions in the past,few studies have conducted a comprehensive and in-depth investigation into the impacts of tempera-ture.This review summarizes the relevant studies on BVOCs in the past decade,including the main biosynthetic pathways,emission observation techniques and emission inventories,as well as how temperature affects isoprene and monoterpene emission rates and the formation of O_(3) and SOA.Our work offers a theoretical foundation and guidance for future efforts to advance the comprehension of BVOC emission characteristics and develop strategies to mitigate secondary pollution.展开更多
Traffic at urban intersections frequently encounters unexpected obstructions,resulting in congestion due to uncooperative and priority-based driving behavior.This paper presents an optimal right-turn coordination syst...Traffic at urban intersections frequently encounters unexpected obstructions,resulting in congestion due to uncooperative and priority-based driving behavior.This paper presents an optimal right-turn coordination system for Connected and Automated Vehicles(CAVs)at single-lane intersections,particularly in the context of left-hand side driving on roads.The goal is to facilitate smooth right turns for certain vehicles without creating bottlenecks.We consider that all approaching vehicles share relevant information through vehicular communications.The Intersection Coordination Unit(ICU)processes this information and communicates the optimal crossing or turning times to the vehicles.The primary objective of this coordination is to minimize overall traffic delays,which also helps improve the fuel consumption of vehicles.By considering information from upcoming vehicles at the intersection,the coordination system solves an optimization problem to determine the best timing for executing right turns,ultimately minimizing the total delay for all vehicles.The proposed coordination system is evaluated at a typical urban intersection,and its performance is compared to traditional traffic systems.Numerical simulation results indicate that the proposed coordination system significantly enhances the average traffic speed and fuel consumption compared to the traditional traffic system in various scenarios.展开更多
Acceptorless dehydrogenative coupling of pyridinemethanol with ketones is one of the most reliable methodologies to access functionalized 1,8-naphthyridine derivatives.However,it is challenging to develop environmenta...Acceptorless dehydrogenative coupling of pyridinemethanol with ketones is one of the most reliable methodologies to access functionalized 1,8-naphthyridine derivatives.However,it is challenging to develop environmentally friendly catalytic systems,especially in constructing efficient and recyclable catalysts under water or solvent-free conditions.Here,we designed two novel coordination polymers Cd-CPs and Fe-CPs to investigate their catalytic performance in water.Gratifyingly,it was observed that Cd-CPs as a multifunctional catalyst was successfully applied to establish a universal pathway for direct fabrication of 1,8-naphthyridine derivatives under water conditions,while it was effective for the synthesis of1,3,5-triazines through acceptorless dehydrogenative coupling strategies.The features of broad substrate,high atom efficiency,and good catalyst reusability highlight the feasibility of this transformation.In additional,we demonstrated the spindle-like structures Fe-P,derived from the Fe-CPs via phosphorylation,which can be used as an efficient electrocatalyst for oxygen evolution reaction with good stability.This work provides two highly efficient non-noble metal catalysts for functionalized 1,8-naphthyridine derivatives production and oxygen evolution reaction,and opens a new avenue to further fabricate diverse metal catalysts with high catalytic performance in water.展开更多
Chili fermentation is one of the most important processes in the production of Pixian Douban(PXDB),which determines the flavor and product quality of PXDB.However,the maturity of fermented chili mainly depends on empi...Chili fermentation is one of the most important processes in the production of Pixian Douban(PXDB),which determines the flavor and product quality of PXDB.However,the maturity of fermented chili mainly depends on empirical judgment,which can not satisfy the need for standardized production of PXDB.Therefore,this study aimed to investigate volatile and non-volatile substances during the maturation process and to find markers related to the maturity of fermented chili.Two-dimensional gas chromatography-mass spectrometry(GC×GC-MS)combined with multivariate statistical analysis and relative odor activity values(ROAV)analysis revealed that 2-methoxy-3-isobutyl pyrazine,linalool,3-(methylthio)propionaldehyde,myrcene,and decanal(ROAV≥1,VIP>1,P<0.05)were regarded as potentially active aromatic markers for differentiating fermentation time.Additionally,ultra-high performance liquid chromatography coupled with quadrupole time-of-flight mass spectrometry(UPLCQTOF-MS)combined with multivariate statistical analysis revealed that 25 compounds could serve as differentiated non-volatile compounds.The correlation of maturity-related physicochemical indicators with volatile and nonvolatile compounds revealed that four volatile compounds(2-methoxy-3-isobutylpyrazine,linalool,myrcene,and decanal)along with seven non-volatile compounds could serve as markers for evaluating the maturity of fermented chili.This study is expected to establish a standard for the determination of the maturity the fermented chili and lay the foundation for intelligent production of PXDB.展开更多
The emergence of precision electronic devices and wearable electronic products urgently requires high-performance multifunctional electromagnetic wave(EMW)absorbers to meet the applicability and versatility in various...The emergence of precision electronic devices and wearable electronic products urgently requires high-performance multifunctional electromagnetic wave(EMW)absorbers to meet the applicability and versatility in various applications.Herein,a dual-network(DN)gel was successfully prepared using acrylamide and sodium lignosulphonate as the basic units by simple chemical cross-linking and physical cross-linking methods.Specifically,the hydrogel forms two types of cross-linking networks through metal coordination and hydrogen bonding.Benefiting from the combined effects of dipole polarization and conductivity loss,the gel achieves an effective absorption bandwidth(EAB)of 6.74 GHz at a thickness of only 1.89 mm,demonstrating excellent EMW absorption performance.In addition,this unique structural configuration endows the EMW absorber with multifunctional features,such as remarkable tensile strength,good environmental compatibility,ultraviolet(UV)resistance,and excellent adhesion.Integrating multiple functional features into the EMW gels displays a broad application prospect in a variety of application scenarios.This research reveals the significance of DN structure design in the electromagnetic wave absorption(EWA)performance of gel-based materials,providing a substantial foundation for the multifunctional design of gel-based absorbers.展开更多
A trace analytical method based on solid-phase extraction gas chromatography-tandem mass spectrometry(SPE–GC–MS/MS)was developed for the rapid detection of 256 semi-volatile organic compounds(SVOCs),including 25 pol...A trace analytical method based on solid-phase extraction gas chromatography-tandem mass spectrometry(SPE–GC–MS/MS)was developed for the rapid detection of 256 semi-volatile organic compounds(SVOCs),including 25 polycyclic aromatic hydrocarbons(PAHs),70 polychlorinated biphenyls(PCBs),123 pesticides,20 phthalate esters(PAEs),4 organophosphate esters(OPEs),9 synthetic musks(SMs),and 5 UV filters(UVs)in water.No-tably,this method provided a decent linearity of calibration standards(R^(2)>0.999),excellent method limits of quantification(MLOQs)(0.12–11.41 ng/L),satisfactory matrix spiking recovery rates(60.4%–126%),and high precision(intra-day relative standard deviations(RSDs):1.0%–10.0%,inter-day RSDs:3.0%–15.0%,and inter-week RSDs:3.4%–15.7%),making it suitable for trace-level studies.Statistical analysis revealed that SVOCs with higher volatility exhibited enhanced recovery rates.Validation of the methodology involved analyzing SVOCs in real spring water and river water samples.Twenty-seven SVOCs were detected in spring water and 58 in river water,with an average concentration of 631.73 and 16,095 ng/L,respectively.Among the detected SVOCs,PAEs constituted the predominant proportion.This study underscored the presence of SVOCs contamination specifi-cally within the spring water,although SVOCs concentrations in river water were significantly greater than those found in spring water.In summary,this sensitive method based on SPE–GC–MS/MS was successfully developed and validated for the rapid analysis of a diverse array of 256 SVOCs at trace levels in water,including not only the traditional highly valued PAHs,PCBs,pesticides,and PAEs,but also the emerging OPEs,UVs,and SMs.展开更多
BACKGROUND:Breast hyperplasia is a common benign breast disease mainly caused by endocrine disorders,manifested as abnormal hyperplasia of breast tissue.In recent years,traditional Chinese medicine compounds and probi...BACKGROUND:Breast hyperplasia is a common benign breast disease mainly caused by endocrine disorders,manifested as abnormal hyperplasia of breast tissue.In recent years,traditional Chinese medicine compounds and probiotics have shown good potential in regulating the endocrine system and improving the intestinal microecology,providing new ideas for the treatment of breast hyperplasia.OBJECTIVE:To explore the effects and mechanisms of traditional Chinese medicine compounds and fermented probiotic compounds on breast hyperplasia in mice,providing new theoretical and experimental bases for the clinical treatment and prevention of breast hyperplasia.METHODS:(1)Network pharmacology tools were used to predict the anti-breast-hyperplasia activity of Herba Gueldenstaedtiae(Euphorbia humifusa),as well as its potential targets and signaling pathways.The databases included:TCMSP,OMIM,GeneCards database,UniProt website,Venny2.1.0 website,Metascape,HERB website,and STRING database,all of which are open-access databases.Network pharmacology can predict and screen key information such as the targets corresponding to the active ingredients of traditional Chinese medicine,disease targets,and action pathways through network analysis and computer-system analysis.Therefore,it has been increasingly widely used in the research of traditional Chinese medicine.(2)A breast hyperplasia model was induced in mice by injecting estrogen and progesterone.Mice in the normal blank group were injected intraperitoneally with normal saline every day.Mice in the model group and drugadministration groups were injected intraperitoneally with estradiol benzoate injection at a concentration of 0.5 mg/kg every day for 25 days.From the 26th day,the injection of estradiol benzoate injection was stopped.Mice in the normal blank group were injected intramuscularly with normal saline every day,and mice in the model group and drug-administration groups were injected intramuscularly with progesterone injection at a concentration of 5 mg/kg for 5 days.After the model was established,each group was given drugs respectively.The normal blank group and the model group were gavaged with 0.2 mL/d of normal saline;the positive blank group(Xiaozheng Pill group)was gavaged with an aqueous solution of Xiaozheng Pill at 0.9 mg/g;the low-,medium-and high-dose groups of Compound Herba Gueldenstaedtiae were gavaged with an aqueous solution of the compound medicine at 0.75,1.5,and 3.0 mg/(g·d)respectively;the low-,medium-and high-dose groups of traditional Chinese medicine-bacteria fermentation were gavaged with an aqueous solution of the compound medicine at 0.75,1.5,and 3.0 mg/(g·d)respectively.The administration was continuous for 30 days.RESULTS AND CONCLUSION:(1)The results of network pharmacology research showed that the Compound Herba Gueldenstaedtiae(Euphorbia humifusa)contained 46 active ingredients,which were related to 1213 potential targets.After comparison with 588 known breast-hyperplasia targets,it was speculated that 50 of these targets might be related to the direct effect of the compound on breast hyperplasia.(2)After drug intervention,there was no significant change in the high-dose group of Compound Herba Gueldenstaedtiae compared with the normal blank group.The liver indicators of the other intervention groups all significantly decreased(P<0.05).(3)In terms of kidney and uterine indicators,the medium-dose group of Compound Herba Gueldenstaedtiae decreased significantly compared with the normal blank group(P<0.05).In terms of the uterine index,the model group increased significantly compared with the normal blank group(P<0.01).(4)After 1-month drug treatment,the number of lobules and acini in the breast tissue of the Xiaozheng Pill group,the low,medium,and high-dose group of Compound Herba Gueldenstaedtiae,the low,medium,and highdose groups of traditional Chinese medicine-bacteria fermentation decreased,and the duct openings narrowed.With the increase of drug dose,diffuse hyperplasia of breast tissue was significantly improved.(5)The ELISA results showed that compared with the model group,the estrogen level was lower in the medium-dose group of traditional Chinese medicine-bacteria fermentation after the intervention(P<0.05).In addition,the follicle-stimulating hormone level in the low-dose group of Compound Herba Gueldenstaedtiae was lower than that of the model group(P<0.05).(6)The intervention in the mouse model led to changes in the abundance of short chain fatty acids and intestinal flora in all groups.To conclude,the Compound Herba Gueldenstaedtiae and its probiotic fermentation products significantly improved mammary gland hyperplasia in mice by regulating hormone levels,improving the structure of the gut microbiota,and increasing the content of shortchain fatty acids,providing new ideas and potential sources of drugs for the treatment of breast hyperplasia.展开更多
In high-intensity electromagnetic warfare,radar systems are persistently subjected to multi-jammer attacks,including potentially novel unknown jamming types that may emerge exclusively under wartime conditions.These j...In high-intensity electromagnetic warfare,radar systems are persistently subjected to multi-jammer attacks,including potentially novel unknown jamming types that may emerge exclusively under wartime conditions.These jamming signals severely degrade radar detection performance.Precise recognition of these unknown and compound jamming signals is critical to enhancing the anti-jamming capabilities and overall reliability of radar systems.To address this challenge,this article proposes a novel open-set compound jamming cognition(OSCJC)method.The proposed method employs a detection-classification dual-network architecture,which not only overcomes the false alarm and misdetection issues of traditional closed-set recognition methods when dealing with unknown jamming but also effectively addresses the performance bottleneck of existing open-set recognition techniques focusing on single jamming scenarios in compound jamming environments.To achieve unknown jamming detection,we first employ a consistency labeling strategy to train the detection network using diverse known jamming samples.This strategy enables the network to acquire highly generalizable jamming features,thereby accurately localizing candidate regions for individual jamming components within compound jamming.Subsequently,we introduce contrastive learning to optimize the classification network,significantly enhancing both intra-class clustering and inter-class separability in the jamming feature space.This method not only improves the recognition accuracy of the classification network for known jamming types but also enhances its sensitivity to unknown jamming types.Simulations and experimental data are used to verify the effectiveness of the proposed OSCJC method.Compared with the state-of-the-art open-set recognition methods,the proposed method demonstrates superior recognition accuracy and enhanced environmental adaptability.展开更多
Endogenous hydrogen systems,consisting of metal–organic coordination catalysts and alcohols,have been widely applied for the transfer hydrogenation(TH)of biomass-derived carbonyl compounds in recent years.Metal-organ...Endogenous hydrogen systems,consisting of metal–organic coordination catalysts and alcohols,have been widely applied for the transfer hydrogenation(TH)of biomass-derived carbonyl compounds in recent years.Metal-organic coordination catalysts showed satisfactory ability of TH in the secondary alcohols,but most of them could not effectively employ the cheaper primary alcohols as hydrogen donors.Furthermore,they commonly contained high metal contents,which also led to low catalytic efficiency in significant measure.In this work,we constructed a novel magnesium single-atom catalyst(Mg-NC)with merely 0.37 wt%Mg by means of a combined self-assembly and pyrolysis strategy.The characterization results indicated that Mg was atomically dispersed and it was coordinated with four pyridinic-N in Mg-NC.Due to the obvious electron transfer from Mg to its coordinated pyridinic-N,Mg–N_(4)active centers displayed high Lewis acid-base strength with abundant content,which brought remarkable catalytic activity.When Mg-NC was used for the TH of 5-hydroxymethylfurfural(HMF)in ethanol(EtOH),2,5-bis(hydroxymethyl)furan(BHMF)yield was up to 96.3%with high productivity of 19.85 molBHMF mol_(Mg)^(−1)h^(−1)at 150°C for 5 h.More interestingly,the process of TH over Mg-NC in EtOH was proved to proceed via the hydrogen radical mechanism.Additionally,Mg-NC exhibited powerful catalytic universality;it could not only utilize other primary alcohols(such as n-propanol and n-butanol)as hydrogen donors,but also catalyze the TH of other carbonyl compounds(such as furfural,5-methylfurfural,benzaldehyde,cyclohexanone,and levulinic acid).Overall,this work offered some important clues and references to reinforce the hydrogen-supplying ability of primary alcohols in the TH of various biomass-derived carbonyl compounds to high-value fine chemicals.展开更多
Oxygen vacancy(Vo)engineering has been recognized as one of the most effective strategies for enhancing the photocatalytic CO_(2) conversion performance of metal oxides,as it can simultaneously facilitate photogenerat...Oxygen vacancy(Vo)engineering has been recognized as one of the most effective strategies for enhancing the photocatalytic CO_(2) conversion performance of metal oxides,as it can simultaneously facilitate photogenerated charge carrier separation efficiency and provide additional surface reaction sites.However,the wide application of Vo engineering in photocatalysis are limited by its poor stability,owing to the easy recovery of these vacancy defects by atmospheric oxygen.Herein,we develop an indium(In)doping strategy to regulate the coordination environment in CeO_(2) with abundant Vo(CeO_(2-x)),thereby enhance its stability during photocatalytic CO_(2) conversion.Confirmed by positron annihilation lifetime spectroscopy(PALS),In dopants combine with Vo by substituting for part of Ce^(4+),forming In^(3+)-Vo complexes that effectively inhibit the formation of unstable va-cancy clusters.Such In^(3+)-Vo complexes can also reduce the energy required for formation of the CO products.Therefore,the optimized In-doped CeO_(2-x) exhibits excellent photocatalytic CO_(2) conversion performance,with a CO yield of 301.6μmol⋅g^(-1) after 5 h of light irradiation,and maintain high activity after four cycles of experiments.Comprehensive experimental and theoretical studies indicate that the introduction of In doping not only significantly improves the stability of Vo in CeO_(2-x),but also reconstruct the reaction kinetics of the CO_(2) conversion by forming In^(3+)-Vo complexes thus facilitating the overall reaction.展开更多
Carbonyl compounds play a pivotal role in the formation of secondary pollutants such as O_(3) and SOA,signifi-cantly impacting air quality and human health.This study extended the observation period compared to previo...Carbonyl compounds play a pivotal role in the formation of secondary pollutants such as O_(3) and SOA,signifi-cantly impacting air quality and human health.This study extended the observation period compared to previous research,providing a long-term perspective on carbonyl compound variations and their environmental implica-tions.Atmospheric observations were conducted at Beijing(BJ)and Xianghe(XH)during the summer and winter months of 2018,2019,and 2023 to study the sources and impacts of carbonyl compounds in typical urban areas and peri‑urban areas.Notably,concentrations in the summer of 2023 increased compared to 2018 and 2019.The predominant carbonyl compounds—formaldehyde,acetaldehyde,and acetone—accounted for over 60%of the total.The mean values of OFP in BJ ranged from 18.55 to 58.61μg/m3,lower than those in XH(29.82 to 65.48μg/m3),with formaldehyde and acetaldehyde contributing over 80%of the total.SOAP exhibited a similar pattern,with values in XH(69.21 to 508.55μg/m3)significantly exceeding those in BJ(34.47 to 159.78μg/m3).The PMF model highlighted vehicle exhaust,secondary pollution,and biomass combustion as major sources of carbonyl compounds,emphasizing differences in source contributions between the two regions.This study’s com-parative analysis over different years and locations provides new insights into the dynamic changes in carbonyl compounds and their environmental importance.These results not only reinforce the importance of carbonyl compounds regulation but also offer a valuable reference for evaluating and refining emission control strategies during this period.展开更多
The precise tuning of magnetic nanoparticle size and magnetic domains,thereby shaping magnetic properties.However,the dynamic evolution mechanisms of magnetic domain configurations in relation to electromagnetic(EM)at...The precise tuning of magnetic nanoparticle size and magnetic domains,thereby shaping magnetic properties.However,the dynamic evolution mechanisms of magnetic domain configurations in relation to electromagnetic(EM)attenuation behavior remain poorly understood.To address this gap,a thermodynamically controlled periodic coordination strategy is proposed to achieve precise modulation of magnetic nanoparticle spacing.This approach unveils the evolution of magnetic domain configurations,progressing from individual to coupled and ultimately to crosslinked domain configurations.A unique magnetic coupling phenomenon surpasses the Snoek limit in low-frequency range,which is observed through micromagnetic simulation.The crosslinked magnetic configuration achieves effective low-frequency EM wave absorption at 3.68 GHz,encompassing nearly the entire C-band.This exceptional magnetic interaction significantly enhances radar camouflage and thermal insulation properties.Additionally,a robust gradient metamaterial design extends coverage across the full band(2–40 GHz),effectively mitigating the impact of EM pollution on human health and environment.This comprehensive study elucidates the evolution mechanisms of magnetic domain configurations,addresses gaps in dynamic magnetic modulation,and provides novel insights for the development of high-performance,low-frequency EM wave absorption materials.展开更多
Two novel energetic coordination compounds Zn2（DAT）5（H2O）3（TNR）2 and Co2（DAT）5（H2O）3（TNR）2 were synthesized and their structures were characterized by elemental analysis and FT-IR spectroscopy.The crystal ...Two novel energetic coordination compounds Zn2（DAT）5（H2O）3（TNR）2 and Co2（DAT）5（H2O）3（TNR）2 were synthesized and their structures were characterized by elemental analysis and FT-IR spectroscopy.The crystal structures were determined by single-crystal X-ray diffraction.The results reveal that the compounds have similar molecular structures and the crystals belong to the triclinic system,space group P with a = 11.491（3）,b = 13.564（3）,c = 15.496（3） ,V = 2180.4（8） 3,C17H28 Zn2N36O19,Mr = 1203.02 g·mol-1,Dc = 1.832 g·cm-3,μ（MoKα） = 1.221 mm-1,F（000） = 1223,Z = 2,R = 0.0596 and wR = 0.1514 for 11289 observed reflections（I 〉 2σ（I）） for Zn2（DAT）5（H2O）3（TNR）2 and a = 11.5291（13）,b = 13.4894（15）,c = 15.4852（17） ,V = 2164.8（4） 3,C17H28Co2N36O19,Mr = 1190.14 g·mol-1,Dc = 1.826 g·cm-3,μ（MoKα） = 0.888 mm-1,F（000） = 1211,Z = 2,R = 0.0576 and wR = 0.1431 for 11218 observed reflections（I 〉 2σ（I）） for Co2（DAT）5（H2O）3（TNR）2,respectively.The thermal decomposition characteristics of the com-pounds were investigated using differential scanning calorimetry and thermal gravimetry-diffediffer-rential thermal gravimetry.The results of thermal decomposition processes were similar for the two compounds.Both undergo four-step decomposition after the loss of coordinated H2O molecules.The final solid residues for the two DAT complexes were the corresponding metal oxides.The kinetic parameter of the first exothermic process of the compounds was studied by applying the Kissinger and Ozawa-Doyle methods.The thermodynamic parameters of the activation could be calculated.Sensitivity tests revealed that Co2（DAT）5（H2O）3（TNR）2 was more sensitive than Zn2（DAT）5（H2O）3（TNR）2.展开更多
The binding of Co (phen)2dppz3+ to calf thymus DNA,as investigated using absorption spectroscopy. viscosity and electrophoresis measurements,here dppz is dipyrido[3, 2-a: 2'3'-c]phenazine. The compound shows a...The binding of Co (phen)2dppz3+ to calf thymus DNA,as investigated using absorption spectroscopy. viscosity and electrophoresis measurements,here dppz is dipyrido[3, 2-a: 2'3'-c]phenazine. The compound shows absorption hypochromicity and the specific viscosity increased upon binding to calf thymus DNA The complex is also shown to be more efficient photosensitisers for single strand breaks in plasmid DNA展开更多
A novel luminescent coordination compound Eu（TTA）3（DEDAF）（1, TTA = 1,1,1-trifluoro-3-（2-thenoyl）acetone, DEDAF = 9,9-diethyl-4,5-diazafluoren） has been synthesized and fully characterized by infrared spectrum,...A novel luminescent coordination compound Eu（TTA）3（DEDAF）（1, TTA = 1,1,1-trifluoro-3-（2-thenoyl）acetone, DEDAF = 9,9-diethyl-4,5-diazafluoren） has been synthesized and fully characterized by infrared spectrum, elemental analysis, UV-vis spectrum, etc. X-ray single-crystal diffraction analysis reveals that compound 1 shows a mononuclear structure with the europium atom in coordinating to one DAF and three TTA ligands. The mononuclear structure units are assembled into a 3-D polymer by hydrogen bonds and π-π interactions. Photoluminescent property of 1 was investigated in detail at room temperature. Complex 1 emits strong red luminescence. However, it could be quenched even by small amount of water. The fluorescence intensity at 614 nm decreases linearly with the water content increasing（vol% in acetonitrile） in the range of 0.025~0.2% under 278 nm excitation. Thermogravimetric analysis has also been studied, which demonstrates good thermal stability of 1.展开更多
The mixed ligand coordination compound of copper with norfloxacin (NFLX) and 1, 10-phen has been synthesized and characterized by means of X-ray single crystal diffraction. The structure features of the coordination ...The mixed ligand coordination compound of copper with norfloxacin (NFLX) and 1, 10-phen has been synthesized and characterized by means of X-ray single crystal diffraction. The structure features of the coordination compound are described. Antibacterial activities of the coordination compound have been tested against different microorganisms. The antitumor activities of the coordination compound on leukemia HL-60 cell line and liver cancer BEL-7402 cell line have been measured, respectively. The results indicated that the coordination compound has strong inhibitory effect on HL-60 and BEL-7402 cell lines.展开更多
Two coordination compounds, namely [Ce（3,5-Br2BC）3（3,5-HBrzBC）]n （1） and [Zn（3,5-Br2BC）2（phen）] （2, 3,5-HBr2BC = 3,5-dibromobenzoic acid, phen = 1,10-phenanthroline）, were assembled. Single-crystal X-ray d...Two coordination compounds, namely [Ce（3,5-Br2BC）3（3,5-HBrzBC）]n （1） and [Zn（3,5-Br2BC）2（phen）] （2, 3,5-HBr2BC = 3,5-dibromobenzoic acid, phen = 1,10-phenanthroline）, were assembled. Single-crystal X-ray diffraction studies show that compound 1 possesses a ID chain coordination network, which is further extended into a 3D supramolecular architecture via Br..＇Br and Br＇＂O halogen bonding. Compound 2 consists of a mononuclear molecule, which is assembled to a 3D supramolecular framework through C-H..-O hydrogen bond, π-π stacking interactions and Br..π halogen bonding. Luminescent and magnetic properties of both compounds have also been studied.展开更多
基金supported by the National Natural Science Foundation of China(22121005,92372203,92372001,52072186,and 52301278)the National Key Research and Development Program of China(2022YFB2402200)+3 种基金the Science and Technology Plans of Tianjin(23JCYBJC00170)the Fundamental Research Funds for the Central Universities,Nankai University(63241206 and 9242000710)Shanghai Jiao Tong University Shaoxing Research Institute of Renewable Energy and Molecular Engineering(JDSX2023003)the Natural Science Foundation of Jiangsu Province(BK20230937).
文摘Redox-active organic compounds have received much attention as high-capacity electrodes for rechargeable batteries.However,the high solubility in organic electrolytes during charge and discharge processes hinders the practical exploitation of organic compounds.This study presents a cobalt-based metal–organic coordination compound with bifunctional coordinated water(Co-MOC-H_(2)O)for sodium-ion storage.The coordinated water enhances interactions between sodium ions and nitrogen atoms in organic ligands through chelation,activating the inert sodium-ion storage sites(C=N).Moreover,the stable hydrogen bonded framework formed by the coordinated water molecules prevents the active organic compounds from dissolving into the electrolyte,thereby enhancing cycling stability.With the bifunctional coordinated water molecules,the Co-MOC-H_(2)O electrode delivers a high capacity of 403 mAh g^(-1)at 0.2 A g^(-1)over 600 cycles and exhibits a capacity retention of 77.9%at 2 A g^(-1)after 1100 cycles.This work highlights the crucial role of the coordinated water molecules in constructing high capacity and long-life sodium-ion storage materials.
文摘AIM:To investigate the genetic basis of Weill-Marchesani syndrome(WMS)in a Chinese family and clarify the pathogenic mechanism of novel ADAMTS17 mutations.METHODS:Comprehensive clinical assessments and genetic analyses were performed on a Chinese family with two affected siblings.Whole-exome sequencing(WES)was conducted for the proband and other family members.Bioinformatics tools were used to evaluate the conservation,predicted pathogenicity,and structural effects of the identified ADAMTS17 variants.In addition,protein structure modeling was applied to assess the functional impacts of the mutations.RESULTS:The proband(a 32-year-old male)and his elder sister(42y)presented typical clinical features of WMS,including short stature,brachydactyly,high myopia,ectopia lentis,and secondary glaucoma.WES identified a novel compound heterozygous mutation in ADAMTS17:a splicing mutation(c.451-2A>G)inherited from the father and a missense mutation(c.1043G>A;p.C348Y)inherited from the mother.The splicing mutation disrupted normal mRNA splicing and processing,leading to premature translation termination.The missense mutation,which is located in the metalloprotease catalytic domain,was predicted to abolish a critical disulfide bond,thereby impairing protein stability.Both mutations exhibited high evolutionary conservation and were predicted to be pathogenic by multiple bioinformatics algorithms.CONCLUSION:A novel compound heterozygous mutation in ADAMTS17 is identified in this WMS-affected Chinese family,and its pathogenicity is verified via bioinformatics analysis and protein structural modeling.These findings are expected to facilitate the genetic diagnosis of WMS and deepen the understanding of its molecular pathogenesis.
基金supported by the Key Talent Project of Gansu Province(2025RCXM017)the National Natural Science Foundation of China(52261040)+2 种基金the Postgraduate Innovation Star Program of Gansu Province(2025CXZX-476)the Major Science and Technology Project of Gansu Province(22ZD6GA008)the Innovation Driven Assistance Engineering Project of Gansu Association for Science and Technology(GXH20250325-5).
文摘Prussian blue analogs(PBAs)are considered one of the excellent cathode materials for sodium-ion batteries due to their low cost and high theoretical specific capacity,especially sodium-rich iron-based PBAs(FeHCF)can provide higher energy density.FeHCF has a poor charge/discharge platform stability at high voltages(FeC_(6)moiety),which is mainly affected by its coordination environment.In this research,Cu^(+)(six-coordinated),which is close to the ionic radius of Fe^(2+),was used for substitution,the FeC_(6)vacancies of FeHCF were reduced,and the coordination environment was optimized.The low Cu^(+)-substituted FeHCF(Cu^(+)0.625)has an optimal electrochemical performance at 8.5 mA/g with a reversible specific capacity of 142 mA h/g and FeC_(6)moiety contribution of more than 68 mA h/g,which is superior to that of unmodified and other Cu^(2+)-substituted FeHCFs.In situ tests demonstrate the reversible structural stability of the Cu^(+)0.625,supporting the stability of their high-voltage platform capacity.This Cu^(+)substitution strategy further enriches the approach to optimize the coordination environment of sodium-rich FeHCF.
基金supported by the National Key R&D Program of China(No.2024YFC3714200)Guangxi Key Research and Development Program,China(No.Guike AB24010074)+2 种基金the National Natural Science Foundation of China(Nos.22276099,U24A20515 and 22361162668)the Natural Science Foundation of Jiangsu Province(No.BK20240036)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(No.KYCX24_1529).
文摘Temperature has a substantial impact on the emission of biogenic volatile organic compounds(BVOCs).Moder-ate warm temperatures,e.g.,30–40°C,could boost plant metabolism,increasing BVOC emissions.Against the backdrop of global warming,plants emit more BVOCs to cope with thermal stress,leading to elevated concen-trations of tropospheric ozone(O_(3))and secondary organic aerosols(SOA).In recent years,a considerable body of research has explored the interaction between tree species and BVOCs under the influence of various environ-mental factors.Although many studies have examined explored the temperature dependence of BVOC emissions in the past,few studies have conducted a comprehensive and in-depth investigation into the impacts of tempera-ture.This review summarizes the relevant studies on BVOCs in the past decade,including the main biosynthetic pathways,emission observation techniques and emission inventories,as well as how temperature affects isoprene and monoterpene emission rates and the formation of O_(3) and SOA.Our work offers a theoretical foundation and guidance for future efforts to advance the comprehension of BVOC emission characteristics and develop strategies to mitigate secondary pollution.
基金supported by the Japan Society for the Promotion of Science(JSPS)Grants-in-Aid for Scientific Research(C)23K03898.
文摘Traffic at urban intersections frequently encounters unexpected obstructions,resulting in congestion due to uncooperative and priority-based driving behavior.This paper presents an optimal right-turn coordination system for Connected and Automated Vehicles(CAVs)at single-lane intersections,particularly in the context of left-hand side driving on roads.The goal is to facilitate smooth right turns for certain vehicles without creating bottlenecks.We consider that all approaching vehicles share relevant information through vehicular communications.The Intersection Coordination Unit(ICU)processes this information and communicates the optimal crossing or turning times to the vehicles.The primary objective of this coordination is to minimize overall traffic delays,which also helps improve the fuel consumption of vehicles.By considering information from upcoming vehicles at the intersection,the coordination system solves an optimization problem to determine the best timing for executing right turns,ultimately minimizing the total delay for all vehicles.The proposed coordination system is evaluated at a typical urban intersection,and its performance is compared to traditional traffic systems.Numerical simulation results indicate that the proposed coordination system significantly enhances the average traffic speed and fuel consumption compared to the traditional traffic system in various scenarios.
基金financial support of this work by the National Natural Science Foundation of China(No.21861039)Postgraduate Research&Practice Innovation Program of Jiangsu Province(No.KYCX24_2530)the Fundamental Research Funds for the Central Universities。
文摘Acceptorless dehydrogenative coupling of pyridinemethanol with ketones is one of the most reliable methodologies to access functionalized 1,8-naphthyridine derivatives.However,it is challenging to develop environmentally friendly catalytic systems,especially in constructing efficient and recyclable catalysts under water or solvent-free conditions.Here,we designed two novel coordination polymers Cd-CPs and Fe-CPs to investigate their catalytic performance in water.Gratifyingly,it was observed that Cd-CPs as a multifunctional catalyst was successfully applied to establish a universal pathway for direct fabrication of 1,8-naphthyridine derivatives under water conditions,while it was effective for the synthesis of1,3,5-triazines through acceptorless dehydrogenative coupling strategies.The features of broad substrate,high atom efficiency,and good catalyst reusability highlight the feasibility of this transformation.In additional,we demonstrated the spindle-like structures Fe-P,derived from the Fe-CPs via phosphorylation,which can be used as an efficient electrocatalyst for oxygen evolution reaction with good stability.This work provides two highly efficient non-noble metal catalysts for functionalized 1,8-naphthyridine derivatives production and oxygen evolution reaction,and opens a new avenue to further fabricate diverse metal catalysts with high catalytic performance in water.
基金supported by the Sichuan Provincial Department of Science and Technology(2024ZHCG0086)the Chongqing Science and Technology Commission(cstc2021jscx-cylhX0014).
文摘Chili fermentation is one of the most important processes in the production of Pixian Douban(PXDB),which determines the flavor and product quality of PXDB.However,the maturity of fermented chili mainly depends on empirical judgment,which can not satisfy the need for standardized production of PXDB.Therefore,this study aimed to investigate volatile and non-volatile substances during the maturation process and to find markers related to the maturity of fermented chili.Two-dimensional gas chromatography-mass spectrometry(GC×GC-MS)combined with multivariate statistical analysis and relative odor activity values(ROAV)analysis revealed that 2-methoxy-3-isobutyl pyrazine,linalool,3-(methylthio)propionaldehyde,myrcene,and decanal(ROAV≥1,VIP>1,P<0.05)were regarded as potentially active aromatic markers for differentiating fermentation time.Additionally,ultra-high performance liquid chromatography coupled with quadrupole time-of-flight mass spectrometry(UPLCQTOF-MS)combined with multivariate statistical analysis revealed that 25 compounds could serve as differentiated non-volatile compounds.The correlation of maturity-related physicochemical indicators with volatile and nonvolatile compounds revealed that four volatile compounds(2-methoxy-3-isobutylpyrazine,linalool,myrcene,and decanal)along with seven non-volatile compounds could serve as markers for evaluating the maturity of fermented chili.This study is expected to establish a standard for the determination of the maturity the fermented chili and lay the foundation for intelligent production of PXDB.
基金supported by the National Natural Science Foundation of China(Nos.52231007,51872238,52074227,and 21806129)the Fundamental Research Funds for the Central Universities(Nos.3102018zy045,3102019AX11,and 5000220455)the Natural Science Basic Research Plan in Shaanxi Province of China(Nos.2017JQ5116 and 2020JM-118).
文摘The emergence of precision electronic devices and wearable electronic products urgently requires high-performance multifunctional electromagnetic wave(EMW)absorbers to meet the applicability and versatility in various applications.Herein,a dual-network(DN)gel was successfully prepared using acrylamide and sodium lignosulphonate as the basic units by simple chemical cross-linking and physical cross-linking methods.Specifically,the hydrogel forms two types of cross-linking networks through metal coordination and hydrogen bonding.Benefiting from the combined effects of dipole polarization and conductivity loss,the gel achieves an effective absorption bandwidth(EAB)of 6.74 GHz at a thickness of only 1.89 mm,demonstrating excellent EMW absorption performance.In addition,this unique structural configuration endows the EMW absorber with multifunctional features,such as remarkable tensile strength,good environmental compatibility,ultraviolet(UV)resistance,and excellent adhesion.Integrating multiple functional features into the EMW gels displays a broad application prospect in a variety of application scenarios.This research reveals the significance of DN structure design in the electromagnetic wave absorption(EWA)performance of gel-based materials,providing a substantial foundation for the multifunctional design of gel-based absorbers.
基金supported by the National Natural Science Foundation of China(No.51939009)Shenzhen Science and Technology Program(Nos.JCYJ20241202125905008 and GXWD20201231165807007-20200810165349001).
文摘A trace analytical method based on solid-phase extraction gas chromatography-tandem mass spectrometry(SPE–GC–MS/MS)was developed for the rapid detection of 256 semi-volatile organic compounds(SVOCs),including 25 polycyclic aromatic hydrocarbons(PAHs),70 polychlorinated biphenyls(PCBs),123 pesticides,20 phthalate esters(PAEs),4 organophosphate esters(OPEs),9 synthetic musks(SMs),and 5 UV filters(UVs)in water.No-tably,this method provided a decent linearity of calibration standards(R^(2)>0.999),excellent method limits of quantification(MLOQs)(0.12–11.41 ng/L),satisfactory matrix spiking recovery rates(60.4%–126%),and high precision(intra-day relative standard deviations(RSDs):1.0%–10.0%,inter-day RSDs:3.0%–15.0%,and inter-week RSDs:3.4%–15.7%),making it suitable for trace-level studies.Statistical analysis revealed that SVOCs with higher volatility exhibited enhanced recovery rates.Validation of the methodology involved analyzing SVOCs in real spring water and river water samples.Twenty-seven SVOCs were detected in spring water and 58 in river water,with an average concentration of 631.73 and 16,095 ng/L,respectively.Among the detected SVOCs,PAEs constituted the predominant proportion.This study underscored the presence of SVOCs contamination specifi-cally within the spring water,although SVOCs concentrations in river water were significantly greater than those found in spring water.In summary,this sensitive method based on SPE–GC–MS/MS was successfully developed and validated for the rapid analysis of a diverse array of 256 SVOCs at trace levels in water,including not only the traditional highly valued PAHs,PCBs,pesticides,and PAEs,but also the emerging OPEs,UVs,and SMs.
文摘BACKGROUND:Breast hyperplasia is a common benign breast disease mainly caused by endocrine disorders,manifested as abnormal hyperplasia of breast tissue.In recent years,traditional Chinese medicine compounds and probiotics have shown good potential in regulating the endocrine system and improving the intestinal microecology,providing new ideas for the treatment of breast hyperplasia.OBJECTIVE:To explore the effects and mechanisms of traditional Chinese medicine compounds and fermented probiotic compounds on breast hyperplasia in mice,providing new theoretical and experimental bases for the clinical treatment and prevention of breast hyperplasia.METHODS:(1)Network pharmacology tools were used to predict the anti-breast-hyperplasia activity of Herba Gueldenstaedtiae(Euphorbia humifusa),as well as its potential targets and signaling pathways.The databases included:TCMSP,OMIM,GeneCards database,UniProt website,Venny2.1.0 website,Metascape,HERB website,and STRING database,all of which are open-access databases.Network pharmacology can predict and screen key information such as the targets corresponding to the active ingredients of traditional Chinese medicine,disease targets,and action pathways through network analysis and computer-system analysis.Therefore,it has been increasingly widely used in the research of traditional Chinese medicine.(2)A breast hyperplasia model was induced in mice by injecting estrogen and progesterone.Mice in the normal blank group were injected intraperitoneally with normal saline every day.Mice in the model group and drugadministration groups were injected intraperitoneally with estradiol benzoate injection at a concentration of 0.5 mg/kg every day for 25 days.From the 26th day,the injection of estradiol benzoate injection was stopped.Mice in the normal blank group were injected intramuscularly with normal saline every day,and mice in the model group and drug-administration groups were injected intramuscularly with progesterone injection at a concentration of 5 mg/kg for 5 days.After the model was established,each group was given drugs respectively.The normal blank group and the model group were gavaged with 0.2 mL/d of normal saline;the positive blank group(Xiaozheng Pill group)was gavaged with an aqueous solution of Xiaozheng Pill at 0.9 mg/g;the low-,medium-and high-dose groups of Compound Herba Gueldenstaedtiae were gavaged with an aqueous solution of the compound medicine at 0.75,1.5,and 3.0 mg/(g·d)respectively;the low-,medium-and high-dose groups of traditional Chinese medicine-bacteria fermentation were gavaged with an aqueous solution of the compound medicine at 0.75,1.5,and 3.0 mg/(g·d)respectively.The administration was continuous for 30 days.RESULTS AND CONCLUSION:(1)The results of network pharmacology research showed that the Compound Herba Gueldenstaedtiae(Euphorbia humifusa)contained 46 active ingredients,which were related to 1213 potential targets.After comparison with 588 known breast-hyperplasia targets,it was speculated that 50 of these targets might be related to the direct effect of the compound on breast hyperplasia.(2)After drug intervention,there was no significant change in the high-dose group of Compound Herba Gueldenstaedtiae compared with the normal blank group.The liver indicators of the other intervention groups all significantly decreased(P<0.05).(3)In terms of kidney and uterine indicators,the medium-dose group of Compound Herba Gueldenstaedtiae decreased significantly compared with the normal blank group(P<0.05).In terms of the uterine index,the model group increased significantly compared with the normal blank group(P<0.01).(4)After 1-month drug treatment,the number of lobules and acini in the breast tissue of the Xiaozheng Pill group,the low,medium,and high-dose group of Compound Herba Gueldenstaedtiae,the low,medium,and highdose groups of traditional Chinese medicine-bacteria fermentation decreased,and the duct openings narrowed.With the increase of drug dose,diffuse hyperplasia of breast tissue was significantly improved.(5)The ELISA results showed that compared with the model group,the estrogen level was lower in the medium-dose group of traditional Chinese medicine-bacteria fermentation after the intervention(P<0.05).In addition,the follicle-stimulating hormone level in the low-dose group of Compound Herba Gueldenstaedtiae was lower than that of the model group(P<0.05).(6)The intervention in the mouse model led to changes in the abundance of short chain fatty acids and intestinal flora in all groups.To conclude,the Compound Herba Gueldenstaedtiae and its probiotic fermentation products significantly improved mammary gland hyperplasia in mice by regulating hormone levels,improving the structure of the gut microbiota,and increasing the content of shortchain fatty acids,providing new ideas and potential sources of drugs for the treatment of breast hyperplasia.
文摘In high-intensity electromagnetic warfare,radar systems are persistently subjected to multi-jammer attacks,including potentially novel unknown jamming types that may emerge exclusively under wartime conditions.These jamming signals severely degrade radar detection performance.Precise recognition of these unknown and compound jamming signals is critical to enhancing the anti-jamming capabilities and overall reliability of radar systems.To address this challenge,this article proposes a novel open-set compound jamming cognition(OSCJC)method.The proposed method employs a detection-classification dual-network architecture,which not only overcomes the false alarm and misdetection issues of traditional closed-set recognition methods when dealing with unknown jamming but also effectively addresses the performance bottleneck of existing open-set recognition techniques focusing on single jamming scenarios in compound jamming environments.To achieve unknown jamming detection,we first employ a consistency labeling strategy to train the detection network using diverse known jamming samples.This strategy enables the network to acquire highly generalizable jamming features,thereby accurately localizing candidate regions for individual jamming components within compound jamming.Subsequently,we introduce contrastive learning to optimize the classification network,significantly enhancing both intra-class clustering and inter-class separability in the jamming feature space.This method not only improves the recognition accuracy of the classification network for known jamming types but also enhances its sensitivity to unknown jamming types.Simulations and experimental data are used to verify the effectiveness of the proposed OSCJC method.Compared with the state-of-the-art open-set recognition methods,the proposed method demonstrates superior recognition accuracy and enhanced environmental adaptability.
基金financially supported by the National Natural Science Foundation of China(U22A20421)the Qinglan Project of Jiangsu Province,the 533 Talent Program of Huaian City,and the College Students’Innovative Entrepreneurial Training Plan Program of Jiangsu Province(X202510323027).
文摘Endogenous hydrogen systems,consisting of metal–organic coordination catalysts and alcohols,have been widely applied for the transfer hydrogenation(TH)of biomass-derived carbonyl compounds in recent years.Metal-organic coordination catalysts showed satisfactory ability of TH in the secondary alcohols,but most of them could not effectively employ the cheaper primary alcohols as hydrogen donors.Furthermore,they commonly contained high metal contents,which also led to low catalytic efficiency in significant measure.In this work,we constructed a novel magnesium single-atom catalyst(Mg-NC)with merely 0.37 wt%Mg by means of a combined self-assembly and pyrolysis strategy.The characterization results indicated that Mg was atomically dispersed and it was coordinated with four pyridinic-N in Mg-NC.Due to the obvious electron transfer from Mg to its coordinated pyridinic-N,Mg–N_(4)active centers displayed high Lewis acid-base strength with abundant content,which brought remarkable catalytic activity.When Mg-NC was used for the TH of 5-hydroxymethylfurfural(HMF)in ethanol(EtOH),2,5-bis(hydroxymethyl)furan(BHMF)yield was up to 96.3%with high productivity of 19.85 molBHMF mol_(Mg)^(−1)h^(−1)at 150°C for 5 h.More interestingly,the process of TH over Mg-NC in EtOH was proved to proceed via the hydrogen radical mechanism.Additionally,Mg-NC exhibited powerful catalytic universality;it could not only utilize other primary alcohols(such as n-propanol and n-butanol)as hydrogen donors,but also catalyze the TH of other carbonyl compounds(such as furfural,5-methylfurfural,benzaldehyde,cyclohexanone,and levulinic acid).Overall,this work offered some important clues and references to reinforce the hydrogen-supplying ability of primary alcohols in the TH of various biomass-derived carbonyl compounds to high-value fine chemicals.
基金supported by the National Natural Science Foundation of China(No.22202152)Tianjin Municipal Science and Technology Bureau(No.24JCQNJC00990)Cangzhou Institute of Tiangong University(No.TGCYY-F-0304).
文摘Oxygen vacancy(Vo)engineering has been recognized as one of the most effective strategies for enhancing the photocatalytic CO_(2) conversion performance of metal oxides,as it can simultaneously facilitate photogenerated charge carrier separation efficiency and provide additional surface reaction sites.However,the wide application of Vo engineering in photocatalysis are limited by its poor stability,owing to the easy recovery of these vacancy defects by atmospheric oxygen.Herein,we develop an indium(In)doping strategy to regulate the coordination environment in CeO_(2) with abundant Vo(CeO_(2-x)),thereby enhance its stability during photocatalytic CO_(2) conversion.Confirmed by positron annihilation lifetime spectroscopy(PALS),In dopants combine with Vo by substituting for part of Ce^(4+),forming In^(3+)-Vo complexes that effectively inhibit the formation of unstable va-cancy clusters.Such In^(3+)-Vo complexes can also reduce the energy required for formation of the CO products.Therefore,the optimized In-doped CeO_(2-x) exhibits excellent photocatalytic CO_(2) conversion performance,with a CO yield of 301.6μmol⋅g^(-1) after 5 h of light irradiation,and maintain high activity after four cycles of experiments.Comprehensive experimental and theoretical studies indicate that the introduction of In doping not only significantly improves the stability of Vo in CeO_(2-x),but also reconstruct the reaction kinetics of the CO_(2) conversion by forming In^(3+)-Vo complexes thus facilitating the overall reaction.
基金supported by the National Natural Science Foundation of China(Nos.41905108 and 42130704).
文摘Carbonyl compounds play a pivotal role in the formation of secondary pollutants such as O_(3) and SOA,signifi-cantly impacting air quality and human health.This study extended the observation period compared to previous research,providing a long-term perspective on carbonyl compound variations and their environmental implica-tions.Atmospheric observations were conducted at Beijing(BJ)and Xianghe(XH)during the summer and winter months of 2018,2019,and 2023 to study the sources and impacts of carbonyl compounds in typical urban areas and peri‑urban areas.Notably,concentrations in the summer of 2023 increased compared to 2018 and 2019.The predominant carbonyl compounds—formaldehyde,acetaldehyde,and acetone—accounted for over 60%of the total.The mean values of OFP in BJ ranged from 18.55 to 58.61μg/m3,lower than those in XH(29.82 to 65.48μg/m3),with formaldehyde and acetaldehyde contributing over 80%of the total.SOAP exhibited a similar pattern,with values in XH(69.21 to 508.55μg/m3)significantly exceeding those in BJ(34.47 to 159.78μg/m3).The PMF model highlighted vehicle exhaust,secondary pollution,and biomass combustion as major sources of carbonyl compounds,emphasizing differences in source contributions between the two regions.This study’s com-parative analysis over different years and locations provides new insights into the dynamic changes in carbonyl compounds and their environmental importance.These results not only reinforce the importance of carbonyl compounds regulation but also offer a valuable reference for evaluating and refining emission control strategies during this period.
基金supported by the National Natural Science Foundation of China(22265021,52231007,and 12327804)the Aeronautical Science Foundation of China(2020Z056056003)Jiangxi Provincial Natural Science Foundation(20232BAB212004).
文摘The precise tuning of magnetic nanoparticle size and magnetic domains,thereby shaping magnetic properties.However,the dynamic evolution mechanisms of magnetic domain configurations in relation to electromagnetic(EM)attenuation behavior remain poorly understood.To address this gap,a thermodynamically controlled periodic coordination strategy is proposed to achieve precise modulation of magnetic nanoparticle spacing.This approach unveils the evolution of magnetic domain configurations,progressing from individual to coupled and ultimately to crosslinked domain configurations.A unique magnetic coupling phenomenon surpasses the Snoek limit in low-frequency range,which is observed through micromagnetic simulation.The crosslinked magnetic configuration achieves effective low-frequency EM wave absorption at 3.68 GHz,encompassing nearly the entire C-band.This exceptional magnetic interaction significantly enhances radar camouflage and thermal insulation properties.Additionally,a robust gradient metamaterial design extends coverage across the full band(2–40 GHz),effectively mitigating the impact of EM pollution on human health and environment.This comprehensive study elucidates the evolution mechanisms of magnetic domain configurations,addresses gaps in dynamic magnetic modulation,and provides novel insights for the development of high-performance,low-frequency EM wave absorption materials.
基金supported by the National Natural Science Foundation of China (NSAF: 10776002)the project of State Key Laboratory of Science and Technology (No. QNKT11-06, YBKY10-03)the Program for New Century Excellent Talents in University (NCET-09-0051)
文摘Two novel energetic coordination compounds Zn2（DAT）5（H2O）3（TNR）2 and Co2（DAT）5（H2O）3（TNR）2 were synthesized and their structures were characterized by elemental analysis and FT-IR spectroscopy.The crystal structures were determined by single-crystal X-ray diffraction.The results reveal that the compounds have similar molecular structures and the crystals belong to the triclinic system,space group P with a = 11.491（3）,b = 13.564（3）,c = 15.496（3） ,V = 2180.4（8） 3,C17H28 Zn2N36O19,Mr = 1203.02 g·mol-1,Dc = 1.832 g·cm-3,μ（MoKα） = 1.221 mm-1,F（000） = 1223,Z = 2,R = 0.0596 and wR = 0.1514 for 11289 observed reflections（I 〉 2σ（I）） for Zn2（DAT）5（H2O）3（TNR）2 and a = 11.5291（13）,b = 13.4894（15）,c = 15.4852（17） ,V = 2164.8（4） 3,C17H28Co2N36O19,Mr = 1190.14 g·mol-1,Dc = 1.826 g·cm-3,μ（MoKα） = 0.888 mm-1,F（000） = 1211,Z = 2,R = 0.0576 and wR = 0.1431 for 11218 observed reflections（I 〉 2σ（I）） for Co2（DAT）5（H2O）3（TNR）2,respectively.The thermal decomposition characteristics of the com-pounds were investigated using differential scanning calorimetry and thermal gravimetry-diffediffer-rential thermal gravimetry.The results of thermal decomposition processes were similar for the two compounds.Both undergo four-step decomposition after the loss of coordinated H2O molecules.The final solid residues for the two DAT complexes were the corresponding metal oxides.The kinetic parameter of the first exothermic process of the compounds was studied by applying the Kissinger and Ozawa-Doyle methods.The thermodynamic parameters of the activation could be calculated.Sensitivity tests revealed that Co2（DAT）5（H2O）3（TNR）2 was more sensitive than Zn2（DAT）5（H2O）3（TNR）2.
文摘The binding of Co (phen)2dppz3+ to calf thymus DNA,as investigated using absorption spectroscopy. viscosity and electrophoresis measurements,here dppz is dipyrido[3, 2-a: 2'3'-c]phenazine. The compound shows absorption hypochromicity and the specific viscosity increased upon binding to calf thymus DNA The complex is also shown to be more efficient photosensitisers for single strand breaks in plasmid DNA
基金supported by the Natural Science Foundation of Zhejiang Province(No.LY16B030009)National Natural Science Foundation of China(No.61205184)521 Talent Cultivation of Zhejiang Sci-Tech University(521 talent project of ZSTU)
文摘A novel luminescent coordination compound Eu（TTA）3（DEDAF）（1, TTA = 1,1,1-trifluoro-3-（2-thenoyl）acetone, DEDAF = 9,9-diethyl-4,5-diazafluoren） has been synthesized and fully characterized by infrared spectrum, elemental analysis, UV-vis spectrum, etc. X-ray single-crystal diffraction analysis reveals that compound 1 shows a mononuclear structure with the europium atom in coordinating to one DAF and three TTA ligands. The mononuclear structure units are assembled into a 3-D polymer by hydrogen bonds and π-π interactions. Photoluminescent property of 1 was investigated in detail at room temperature. Complex 1 emits strong red luminescence. However, it could be quenched even by small amount of water. The fluorescence intensity at 614 nm decreases linearly with the water content increasing（vol% in acetonitrile） in the range of 0.025~0.2% under 278 nm excitation. Thermogravimetric analysis has also been studied, which demonstrates good thermal stability of 1.
基金funded by the National Natural Science Foundation of China(No.50073019)
文摘The mixed ligand coordination compound of copper with norfloxacin (NFLX) and 1, 10-phen has been synthesized and characterized by means of X-ray single crystal diffraction. The structure features of the coordination compound are described. Antibacterial activities of the coordination compound have been tested against different microorganisms. The antitumor activities of the coordination compound on leukemia HL-60 cell line and liver cancer BEL-7402 cell line have been measured, respectively. The results indicated that the coordination compound has strong inhibitory effect on HL-60 and BEL-7402 cell lines.
基金supported by the Natural Science Foundation of Shanxi Province(No.2013011011-6)the Subject Team of Taiyuan University of Science and Technology
文摘Two coordination compounds, namely [Ce（3,5-Br2BC）3（3,5-HBrzBC）]n （1） and [Zn（3,5-Br2BC）2（phen）] （2, 3,5-HBr2BC = 3,5-dibromobenzoic acid, phen = 1,10-phenanthroline）, were assembled. Single-crystal X-ray diffraction studies show that compound 1 possesses a ID chain coordination network, which is further extended into a 3D supramolecular architecture via Br..＇Br and Br＇＂O halogen bonding. Compound 2 consists of a mononuclear molecule, which is assembled to a 3D supramolecular framework through C-H..-O hydrogen bond, π-π stacking interactions and Br..π halogen bonding. Luminescent and magnetic properties of both compounds have also been studied.
