A simple synthesis of highly functionalized 2,5-diaminofurans based pyrimidine derivatives from 1-(carboxymethyl)uracil via a multi-component reaction is described. The reactive 1:1 intermediate produced from the r...A simple synthesis of highly functionalized 2,5-diaminofurans based pyrimidine derivatives from 1-(carboxymethyl)uracil via a multi-component reaction is described. The reactive 1:1 intermediate produced from the reaction of tert-butyl isocyanide and dialkyl acetylenedicarboxylates was trapped at room temperature by 1-(carboxymethyl)uracil derivatives to yield polyfunctio- nalized furan rings in fairly good yields.展开更多
An improved method is proposed for the extraction of the symmetry energy coefficient relative to the temperature,a_(sym)/T,in the heavy-ion reactions near the Fermi energy region,based on the modified Fisher Model.Thi...An improved method is proposed for the extraction of the symmetry energy coefficient relative to the temperature,a_(sym)/T,in the heavy-ion reactions near the Fermi energy region,based on the modified Fisher Model.This method is applied to the primary fragments of antisymmetrized molecular dynamics(AMD)simulations for ^(46)Fe+^(46)Fe,^(40)Ca+^(40)Ca and ^(48)Ca+^(48)Ca at 35 MeV/nucleon,in order to make direct comparison to the results from the K(N,Z)method of Ono et al.In our improved method,the extracted values of a_(sym)/T increase as the size of isotopes increases whereas,in the K(N,Z)method,the results show rather constant behavior.This increase in our result is attributed to the surface contribution of the symmetry energy in finite nuclei.In order to evaluate the surface contribution,the relation a_(sym)/T=[a_(sym)^((V))(1-k_(S/V) A^(-1/3))]/T is applied and k_(S/V)=1.20~1.25 was extracted.This value is smaller than those extracted from the mass table,reflecting the weakened surface contribution at higher temperature regime.Δμ/T,the difference of the neutron-proton chemical potentials relative to the temperature,is also extracted in this method at the same time.The average values of the extractedΔμ/T,Δμ/T show a linear dependence on the proton-neutron a_(sym)metry parameter of the system,δ_(sys),andΔμ/T=(15.1±0.2)δ_(sys)-(0.5±0.1)is obtained.展开更多
α-Trifluoromethyl ketones are a class of useful compounds with versatile applications.Their synthetic application via the transformation of the C—F bonds is of particular interest by allowing the synthesis of organi...α-Trifluoromethyl ketones are a class of useful compounds with versatile applications.Their synthetic application via the transformation of the C—F bonds is of particular interest by allowing the synthesis of organic compounds with diverse structures.Herein,the advances in the research areas ofα-trifluoromethyl ketone synthesis and their defluorination reactions are reviewed.Discussion on the mechanisms of the typical reactions has also been provided,in hope of affording some guides to the chemistry ofα-trifluoromethyl ketones in the synthetic methods toward themselves and their derivatives.展开更多
A convenient photocatalytic multi-component reaction of alkenes,quinoxalin-2(1H)-ones,and diazo compounds has been developed in the presence of water.A number of ester-containing quinoxalin-2(1H)-ones could be efficie...A convenient photocatalytic multi-component reaction of alkenes,quinoxalin-2(1H)-ones,and diazo compounds has been developed in the presence of water.A number of ester-containing quinoxalin-2(1H)-ones could be efficiently obtained in moderate to good yields at room temperature.This metal-free visiblelight-driven tandem reaction was conducted through proton-coupled electron transfer(PCET)process using water as the hydrogen donor and 1,2,3,5-tetrakis(carbazol-9-yl)-4,6-dicyanobenzene(4CzIPN)as the photocatalyst.展开更多
Three efficient methods for the synthesis of a series of Cu(Ⅱ) and Cu(Ⅰ) complexes based on imidazo[1,5-a]pyridine derivatives were developed.These methods include the following:(ⅰ)Cu(Ⅱ) salts were used as metal s...Three efficient methods for the synthesis of a series of Cu(Ⅱ) and Cu(Ⅰ) complexes based on imidazo[1,5-a]pyridine derivatives were developed.These methods include the following:(ⅰ)Cu(Ⅱ) salts were used as metal sources and N,N-dimethylformamide was employed as a solvent as well as a reductant to produce Cu(Ⅰ) complexes.(ⅱ) An iodide-containing compound was utilized as a ligand and iodide source to prepare complexes.An in situ metalligand reaction occurred and an iodide-bridged copper complex was generated.(ⅲ) A series of aldehydes were added to the reaction systems to induce in situ metal-ligand reactions between the aldehydes and the imidazo[1,5-a]pyridine derivatives,producing polydentate ligand scaffolds.Eight complexes were prepared and characterized.The catalytic activities of these complexes toward the ketalization of ketones by ethylene glycol were investigated.With the exception of complex4,the remaining seven complexes all showed high catalytic activity.The lower activity of 4 may be due to the larger radius of bridging iodide ions and the shorter Cu(Ⅰ)…Cu(Ⅰ) distance.CCDC:2357696,1·2CH_(2)Cl_(2);2357697,2;2018292,3;2092192,4;2092190,5;2155557,6;2406155,7;2406156,8·EtOH.展开更多
Chiral carbonyl compounds frequently occur in natural products and pharmaceuticals. Additionally, they serve as important intermediates in organic synthesis. Transition metal-catalyzed asymmetric carbonylative cross-c...Chiral carbonyl compounds frequently occur in natural products and pharmaceuticals. Additionally, they serve as important intermediates in organic synthesis. Transition metal-catalyzed asymmetric carbonylative cross-coupling reactions are among the most straightforward and effective methods for synthesizing chiral carbonyl compounds, including esters, amides, and ketones. The advances in asymmetric carbonylative cross-coupling reactions using various O-, N-, C-, and S-containing nucleophiles or electrophiles over the past decade are summarized.展开更多
Paclitaxel is one of the commonly used drugs in postoperative chemotherapy for ovarian cancer patients. However, affected by drug dosage and individual differences in the course of medication, patients will have diffe...Paclitaxel is one of the commonly used drugs in postoperative chemotherapy for ovarian cancer patients. However, affected by drug dosage and individual differences in the course of medication, patients will have different degrees of adverse reactions, which will cause damage to the patient’s body once they occur. This paper retrospectively analyzed the clinical data of patients with severe allergic reactions such as fecal incontinence and numbness of hands and feet caused by the use of paclitaxel liposome during postoperative chemotherapy in a case of ovarian cancer admitted to our hospital. The causes and corresponding treatment measures were analyzed, in order to provide the reference for medical staff to take effective countermeasures in advance in the future.展开更多
The investigation of reaction kinetics is the key to understanding the nature of reaction processes.However,monitoring fast photochemical reactions by mass spectrometry remains challenging.Herein,we developed an optic...The investigation of reaction kinetics is the key to understanding the nature of reaction processes.However,monitoring fast photochemical reactions by mass spectrometry remains challenging.Herein,we developed an optical focusing inductive electrospray(OF-iESI)mass spectrometry platform for real-time and in-situ photoreaction monitoring.Coaxial irradiation from back of nanoelectrospray emitter with a taper section was utilized,so the emitter could act as optical lens to help achieving much larger optical power density at emitter tip compared to other sections,which allowed for in-situ reaction monitoring of photoreactions.Through theoretical calculations,the highest optical power density region volume was ca.45 nL.We also integrated a controller for the laser source(450 nm),enabling the modulation of pulse duration(>1 ms).This facilitates the study of photochemical reaction kinetics.The in-situ capability of this device was proved by capturing the short-lived photogenerated intermediates during the dehydrogenation of tetrahydroquinoline.This device was further used to investigate the kinetics of triplet energy transfer based Paternò-Büchi reaction.The reaction order has hitherto remained undetermined while the result of OF-iESI suggested it followed pseudo-second-order reaction kinetics.The short-lived donor-acceptor collision complex intermediate was also successfully identified by tandem mass spectrometry.展开更多
In the realm of nonlinear integrable systems,the presence of decompositions facilitates the establishment of linear superposition solutions and the derivation of novel coupled systems exhibiting nonlinear integrabilit...In the realm of nonlinear integrable systems,the presence of decompositions facilitates the establishment of linear superposition solutions and the derivation of novel coupled systems exhibiting nonlinear integrability.By focusing on single-component decompositions within the potential BKP hierarchy,it has been observed that specific linear superpositions of decomposition solutions remain consistent with the underlying equations.Moreover,through the implementation of multi-component decompositions within the potential BKP hierarchy,successful endeavors have been undertaken to formulate linear superposition solutions and novel coupled Kd V-type systems that resist decoupling via alterations in dependent variables.展开更多
Multi-component transition group metal borides(MMB_(2))have become a research hotspot due to their new composition design concepts and superior properties compared with conventional ceramics.Most of the current method...Multi-component transition group metal borides(MMB_(2))have become a research hotspot due to their new composition design concepts and superior properties compared with conventional ceramics.Most of the current methods,however,are complicated and time-consuming,the mass production remains a chal-lenge.Herein,we proposed a new high-efficiency strategy for synthesis of MMB_(2)using molten aluminum as the medium for the first time.The prepared Al-containing multi-component borides(TiZrHfNbTa)B_(2)microcrystals had a homogeneous composition with a hexagonal AlB_(2)structure and ultra-high hardness value of∼35.3 GPa,which was much higher than data reported in the literature and the rule of mix-ture estimations.Furthermore,combined with the First-principles calculation results,we found that the Poisson’s ratio(v)values exhibit a clearly ascending trend from 0.17 at VEC=3.5 to 0.18 at VEC=3.4,then to 0.201 at VEC=3.2 with the increasing of Al content.This indicates that the intrinsic toughness of multi-component boride microcrystals is obviously enhanced by the trace-doped Al elements.Besides,the fabricated Al-containing multi-component boride microcrystals have superior oxidation activation en-ergy and structural stability.The enhanced oxidation resistance is mainly attributed to the formation of a protective Al2 O3 oxide layer and the lattice distortion,both of which lead to sluggish diffusion of O_(2).These findings propose a new unexplored avenue for the fabrication of MMB_(2)materials with supe-rior comprehensive performance including ultra-hardness and intrinsically improved thermo-mechanical properties.展开更多
Designing highly active electrocatalysts for the hydrogen evolution reaction(HER)and oxygen evolution and reduction reactions(OER and ORR)is pivotal to renewable energy technology.Herein,based on density functional th...Designing highly active electrocatalysts for the hydrogen evolution reaction(HER)and oxygen evolution and reduction reactions(OER and ORR)is pivotal to renewable energy technology.Herein,based on density functional theory(DFT)calculations,we systematically investigate the catalytic activity of iron-nitrogen-carbon based covalent organic frameworks(COF)monolayers with axially coordinated ligands(denotes as Fe N_(4)-X@COF,X refers to axial ligand,X=-SCN,-I,-H,-SH,-NO_(2),-Br,-ClO,-Cl,-HCO_(3),-NO,-ClO_(2),-OH,-CN and-F).The calculated results demonstrate that all the catalysts possess good thermodynamic and electrochemical stabilities.The different ligands axially ligated to the Fe active center could induce changes in the charge of the Fe center,which further regulates the interaction strength between intermediates and catalysts that governs the catalytic activity.Importantly,FeN_(4)-SH@COF and Fe N_(4)-OH@COF are efficient bifunctional catalysts for HER and OER,FeN_(4)-OH@COF and FeN_(4)-I@COF are promising bifunctional catalysts for OER and ORR.These findings not only reveal promising bifunctional HER/OER and OER/ORR catalysts but also provide theoretical guidance for designing optimum ironnitrogen-carbon based catalysts.展开更多
This paper, an addendum to “Dialectical Thermodynamics’ solution to the conceptual imbroglio that is the reversible path”, this journal, 10, 775-799, was written in response to the requests of several readers to pr...This paper, an addendum to “Dialectical Thermodynamics’ solution to the conceptual imbroglio that is the reversible path”, this journal, 10, 775-799, was written in response to the requests of several readers to provide further evidence of the said “imbroglio”. The evidence here presented relates to the incompatibility existing between the total-entropy and the Gibbs energy prescriptions for the reversible path. The previously published proof of the negentropic nature of the transformation of heat into work is here included to validate out conclusions about the Gibbs energy perspective.展开更多
Continuous-flow upgrading of pentaerythritol synthesis technology via base-catalyzed aldol and Cannizzaro reactions of formaldehyde and acetaldehyde faces the challenge of effectively controlling the critical side rea...Continuous-flow upgrading of pentaerythritol synthesis technology via base-catalyzed aldol and Cannizzaro reactions of formaldehyde and acetaldehyde faces the challenge of effectively controlling the critical side reaction of hydroxymethyl acetaldehyde(HA)to the acrolein intermediate.Here,we first identified the forms of industrial formaldehyde as methane diol that easily converts to the alkaline formaldehyde under alkaline(NaOH)environment.The carbonyl group of alkaline formaldehyde induces deprotonation of acetaldehyde instead of the recognized base-hydroxyl group-induced deprotonation,and it needs to overcome only 18.31 kcal·mol^(-1)(1 kcal=4.186 kJ)energy barrier to form key intermediates of HA.The sodium solvation cage formed by NaOH hexa-coordinated formaldehyde effectively inhibits the alkalinity,thus contributing to a high energy barrier(46.21 kcal·mol^(-1))to unwanted acrolein formation.In addition,the solvation cage gradually opens to increase the alkalinity with the consumption of formaldehyde,thus facilitating the subsequent Cannizzaro reaction(to overcome 11.77 kcal·mol^(-1)).In comparison,strong alkalinity promotes the formation of acrolein(36.65 kcal·mol^(-1))to initiate the acetal side reaction,while weak alkalinity reduces the possibility of the Cannizzaro reaction(to overcome 20.44 kcal·mol^(-1)).This theoretically reveals the importance of the segmented feeding of weak and strong bases to successively control the aldol reaction and Cannizzaro reaction,and the combination of Na_(2)CO_(3) or HCOONa with NaOH improves the pentaerythritol yield by 7%to 13%compared to that of NaOH alone(70%yield)within 1 min at a throughput of 155.7 ml·min^(-1).展开更多
Efficient catalysis of the oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)is essential for the rechargeable zinc-air batteries(R-ZABs).However,challenges remain due to the scarcity of effective bifunc...Efficient catalysis of the oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)is essential for the rechargeable zinc-air batteries(R-ZABs).However,challenges remain due to the scarcity of effective bifunctional electrocatalysts and limited understanding of the structure-activity relationships.Pyrrole-type single-atom catalysts(SACs)with unique electronic structures have emerged as promising electrocatalysts.In this work,we combine density functional theory(DFT)calculations and experimental studies to systematically explore the structure-activity relationships and potential of pyrrole-type transition metal-N_(3)(TM-po-N_(3))as bifunctional catalysts.DFT calculations reveal that differences in the dependence of ORR and OER activities on the free energy of adsorption of reaction intermediates significantly affect the TM-po-N_(3)bifunctional activity and identify magnetic Cu-po-N_(3)as the best candidate.The bifunctional activity of Cu-po-N_(3)originates from interactions between spin-polarized out-of-plane Cu_3d and O_2s+2p orbitals.Theoretical predictions are validated experimentally,showing that the synthesized Cu-SAC/NC exhibits excellent bifunctional performance with a small potential gap of 0.666 V.Additionally,the assembled R-ZABs display a high-power density of 170 mW cm^(-2)and long-term stability,with the charge-discharge voltage gap increasing by only 0.01 V over 240 h.This work provides new insights into the design of efficient bifunctional catalysts.展开更多
Unsaturated alcohols are a class of Biogenic volatile organic compounds(BVOCs)emitted in large quantities by plants when damaged or under adverse environmental conditions,and studies on their atmospheric degradation a...Unsaturated alcohols are a class of Biogenic volatile organic compounds(BVOCs)emitted in large quantities by plants when damaged or under adverse environmental conditions,and studies on their atmospheric degradation at night are still lacking.We used chamber experiments to study the gas-phase reactions of three unsaturated alcohols,E-2-penten-1-ol,Z-2-hexen-1-ol and Z-3-hepten-1-ol,with NO_(3)radicals(NO_(3)•)during the night.The rate constants of these reactions were(11.7±1.76)×10^(−13),(8.55±1.33)×10^(−13)and(6.08±0.47)×10^(−13)cm^(3)/(molecule·s)at 298K and 760 Torr,respectively.In contrast,the reaction rate of similar substances with ozone was about 10^(−18)cm^(3)/(molecule·s),which indicates that the reaction with NO_(3)•is themain oxidation pathway for unsaturated alcohols at night.Small molecule aldehydes and ketones were the main gas-phase organic products of the reaction of three aldehydes and ketones with NO_(3)•,and the total small molecule aldehydes and ketones yields can reach between 45%-60%.They mainly originate from the breakage of alkoxy radicals,and different breakage sites determine different product distributions.In addition,the SOA yields of the three unsaturated alcohols with NO_(3)•were 7.1%±1.0%,12.5%±1.9%and 30.0%±4.5%,respectively,whichweremuch higher than those of similarly structured substances with O_(3)or OH radicals(•OH).The results of high-resolution mass spectrometry shows that the main components of Secondary organic aerosol(SOA)of the three unsaturated alcohols are dimeric compounds containing several nitrate groups,which are formed through the polymerization of oxyalkyl radicals.展开更多
The Glauber/eikonal model is a widely used tool for studying intermediate-and high-energy nuclear reactions.When calculating the Glauber/eikonal model phase shift functions,the optical limit approximation(OLA)is often...The Glauber/eikonal model is a widely used tool for studying intermediate-and high-energy nuclear reactions.When calculating the Glauber/eikonal model phase shift functions,the optical limit approximation(OLA)is often used.The OLA neglects the multiple scattering of the constituent nucleons in the projectile and target nuclei.However,the nucleon-target version of the Glauber model(the NTG model)proposed by Abu-Ibrahim and Suzuki includes multiple scattering effects between the projectile nucleons and target nuclei.The NTG model was found to improve the description of the elastic scattering angular distributions and total reaction cross sections of some light heavy-ion systems with respect to the OLA.In this work,we study the single-nucleon removal reactions(SNRRs)induced by carbon isotopes on ^(12)C and ^(9)Be targets using both the NTG model and the OLA.Reduction factors(RFs)of the single-nucleon spectroscopic factors were obtained by comparing the experimental and theoretical SNRR cross sections.On average,the RFs obtained with the NTG model were smaller than those obtained using the OLA by 7.8%,in which the average difference in one-neutron removal was 10.6% and that in one-proton removal was 4.2%.However,the RFs were still strongly dependent on the neutron-proton asymmetryΔS of the projectile nuclei,even when the NTG model was used.展开更多
Mg batteries have high energy density,economic safety,and environmental friendliness.They show great potential as an ideal energy storage technology.This review summarizes the limitations of Mg batteries and explores ...Mg batteries have high energy density,economic safety,and environmental friendliness.They show great potential as an ideal energy storage technology.This review summarizes the limitations of Mg batteries and explores the complex reactions at the Mg anode/electrolyte interface.It focuses on critical issues such as the dissolution of Mg anodes,the evolution of hydrogen gas,the formation of a passivation layer that hinders Mg^(2+)migration,and dendrite growth.To address these interface problems,the review discusses strategies to improve interface reactions.These include the structural design of Mg anodes,suitable substitute materials for the anode,and artificial solid electrolyte interphase films.Finally,it outlines the future research directions for the ideal Mg anode interfaces.The goal is to develop more efficient interface design schemes and optimization strategies to advance Mg battery technology further.展开更多
Driving of the nuclear fusion reaction p+^(11)B3α+8.7 MeV under laboratory conditions by interaction between high-power laser pulses and matter has become a popular field of research,owing to its numerous potential a...Driving of the nuclear fusion reaction p+^(11)B3α+8.7 MeV under laboratory conditions by interaction between high-power laser pulses and matter has become a popular field of research,owing to its numerous potential applications:as an alternative to deuterium-tritium for fusion energy production,astrophysics studies,and alpha-particle generation for medical treatment.One possible scheme for laser-driven p-^(11)B reactions is to direct a beam of laser-accelerated protons onto a boron(B)sample(the so-called“pitcher-catcher”scheme).This technique has been successfully implemented on large high-energy lasers,yielding hundreds of joules per shot at low repetition.We present here a complementary approach,exploiting the high repetition rate of the VEGA III petawatt laser at CLPU(Spain),aiming at accumulating results from many interactions at much lower energy,to provide better control of the parameters and the statistics of the measurements.Despite a moderate energy per pulse,our experiment allowed exploration of the laser-driven fusion process with tens(up to hundreds)of laser shots.The experiment provided a clear signature of the reactions involved and of the fusion products,accumulated over many shots,leading to an improved optimization of the diagnostics for experimental campaigns of this type.In this paper,we discuss the effectiveness of laser-driven p-11B fusion in the pitcher-catcher scheme,at a high repetition rate,addressing the challenges of this experimental scheme and highlighting its critical aspects.Our proposed methodology allows evaluation of the performance of this scheme for laser-driven alpha particle production and can be adapted to high-repetition-rate laser facilities with higher energy and intensity.展开更多
Objective:To explore the adverse reactions associated with antibiotics and analyze strategies for their rational use.Methods:A retrospective analysis was conducted on 60 patients who experienced adverse reactions to a...Objective:To explore the adverse reactions associated with antibiotics and analyze strategies for their rational use.Methods:A retrospective analysis was conducted on 60 patients who experienced adverse reactions to antibiotics between August 2021 and August 2023.The types of antibiotics that caused adverse reactions were analyzed,and the symptoms of adverse reactions and measures for rational use of antibiotics were summarized.Results:Among the analyzed cases of adverse reactions to antibiotics,the highest rate was observed in patients aged 61–75 years,accounting for 38.33%,followed by patients aged 51–60 years,accounting for 20.00%.In terms of the types of antibiotics that caused adverse reactions,cephalosporins were the most common,accounting for 40.00%,followed by penicillins,accounting for 18.33%.Analysis of the systems involved in adverse reactions showed that skin and appendage disorders were the most common,accounting for 36.67%,followed by the digestive system,accounting for 28.33%.Conclusion:Irrational use of antibiotics can lead to adverse drug reactions.Therefore,it is necessary to analyze strategies for the rational use of antibiotics to reduce adverse drug reactions and ensure the safety of antibiotic use.展开更多
[Objectives]To explore the methods for identifying pure honey.[Methods]Using 35 batches of Jiulongteng honey sourced from various production areas in Guangxi as the research subjects,this study investigated the chromo...[Objectives]To explore the methods for identifying pure honey.[Methods]Using 35 batches of Jiulongteng honey sourced from various production areas in Guangxi as the research subjects,this study investigated the chromogenic reactions of starch and dextrin,as well as the comparative study of thin-layer chromatography of oligosaccharides present in Jiulongteng honey.[Results]None of the 35 batches of Jiulongteng honey samples exhibited blue(indicating starch),green,or reddish-brown(indicating dextrin)coloration,suggesting that no adulterants such as artificially added starch,dextrin,or sugar were present in these samples.Furthermore,none of the 35 batches displayed additional spots below the corresponding positions of the control,indicating that the sugar composition was consistent with the oligosaccharide profile of natural honey.No components inconsistent with the oligosaccharide profile of natural honey were detected.Therefore,it can be concluded that the Jiulongteng honey samples in this experiment were pure and free from adulteration with starch,dextrin,or other sugar substances.[Conclusions]The method employed in this experiment is straightforward and quick to implement,effectively preventing adulterated honey from entering the market.It enhances the efficiency of quality control for Jiulongteng honey and promotes the healthy development of the Jiulongteng honey industry.展开更多
基金supported by the Research Council of the University of Mazandaran,Iran
文摘A simple synthesis of highly functionalized 2,5-diaminofurans based pyrimidine derivatives from 1-(carboxymethyl)uracil via a multi-component reaction is described. The reactive 1:1 intermediate produced from the reaction of tert-butyl isocyanide and dialkyl acetylenedicarboxylates was trapped at room temperature by 1-(carboxymethyl)uracil derivatives to yield polyfunctio- nalized furan rings in fairly good yields.
文摘An improved method is proposed for the extraction of the symmetry energy coefficient relative to the temperature,a_(sym)/T,in the heavy-ion reactions near the Fermi energy region,based on the modified Fisher Model.This method is applied to the primary fragments of antisymmetrized molecular dynamics(AMD)simulations for ^(46)Fe+^(46)Fe,^(40)Ca+^(40)Ca and ^(48)Ca+^(48)Ca at 35 MeV/nucleon,in order to make direct comparison to the results from the K(N,Z)method of Ono et al.In our improved method,the extracted values of a_(sym)/T increase as the size of isotopes increases whereas,in the K(N,Z)method,the results show rather constant behavior.This increase in our result is attributed to the surface contribution of the symmetry energy in finite nuclei.In order to evaluate the surface contribution,the relation a_(sym)/T=[a_(sym)^((V))(1-k_(S/V) A^(-1/3))]/T is applied and k_(S/V)=1.20~1.25 was extracted.This value is smaller than those extracted from the mass table,reflecting the weakened surface contribution at higher temperature regime.Δμ/T,the difference of the neutron-proton chemical potentials relative to the temperature,is also extracted in this method at the same time.The average values of the extractedΔμ/T,Δμ/T show a linear dependence on the proton-neutron a_(sym)metry parameter of the system,δ_(sys),andΔμ/T=(15.1±0.2)δ_(sys)-(0.5±0.1)is obtained.
文摘α-Trifluoromethyl ketones are a class of useful compounds with versatile applications.Their synthetic application via the transformation of the C—F bonds is of particular interest by allowing the synthesis of organic compounds with diverse structures.Herein,the advances in the research areas ofα-trifluoromethyl ketone synthesis and their defluorination reactions are reviewed.Discussion on the mechanisms of the typical reactions has also been provided,in hope of affording some guides to the chemistry ofα-trifluoromethyl ketones in the synthetic methods toward themselves and their derivatives.
基金supported by Sichuan Science and Technology Program(No.2023NSFSC0101)the 2024 Provincial platform project of Chengdu Normal University(No.GNFZ202404)+1 种基金Natural Science Foundation of Shandong Province(No.ZR2021MB065)National Natural Science Foundation of China(No.22101237)。
文摘A convenient photocatalytic multi-component reaction of alkenes,quinoxalin-2(1H)-ones,and diazo compounds has been developed in the presence of water.A number of ester-containing quinoxalin-2(1H)-ones could be efficiently obtained in moderate to good yields at room temperature.This metal-free visiblelight-driven tandem reaction was conducted through proton-coupled electron transfer(PCET)process using water as the hydrogen donor and 1,2,3,5-tetrakis(carbazol-9-yl)-4,6-dicyanobenzene(4CzIPN)as the photocatalyst.
文摘Three efficient methods for the synthesis of a series of Cu(Ⅱ) and Cu(Ⅰ) complexes based on imidazo[1,5-a]pyridine derivatives were developed.These methods include the following:(ⅰ)Cu(Ⅱ) salts were used as metal sources and N,N-dimethylformamide was employed as a solvent as well as a reductant to produce Cu(Ⅰ) complexes.(ⅱ) An iodide-containing compound was utilized as a ligand and iodide source to prepare complexes.An in situ metalligand reaction occurred and an iodide-bridged copper complex was generated.(ⅲ) A series of aldehydes were added to the reaction systems to induce in situ metal-ligand reactions between the aldehydes and the imidazo[1,5-a]pyridine derivatives,producing polydentate ligand scaffolds.Eight complexes were prepared and characterized.The catalytic activities of these complexes toward the ketalization of ketones by ethylene glycol were investigated.With the exception of complex4,the remaining seven complexes all showed high catalytic activity.The lower activity of 4 may be due to the larger radius of bridging iodide ions and the shorter Cu(Ⅰ)…Cu(Ⅰ) distance.CCDC:2357696,1·2CH_(2)Cl_(2);2357697,2;2018292,3;2092192,4;2092190,5;2155557,6;2406155,7;2406156,8·EtOH.
文摘Chiral carbonyl compounds frequently occur in natural products and pharmaceuticals. Additionally, they serve as important intermediates in organic synthesis. Transition metal-catalyzed asymmetric carbonylative cross-coupling reactions are among the most straightforward and effective methods for synthesizing chiral carbonyl compounds, including esters, amides, and ketones. The advances in asymmetric carbonylative cross-coupling reactions using various O-, N-, C-, and S-containing nucleophiles or electrophiles over the past decade are summarized.
文摘Paclitaxel is one of the commonly used drugs in postoperative chemotherapy for ovarian cancer patients. However, affected by drug dosage and individual differences in the course of medication, patients will have different degrees of adverse reactions, which will cause damage to the patient’s body once they occur. This paper retrospectively analyzed the clinical data of patients with severe allergic reactions such as fecal incontinence and numbness of hands and feet caused by the use of paclitaxel liposome during postoperative chemotherapy in a case of ovarian cancer admitted to our hospital. The causes and corresponding treatment measures were analyzed, in order to provide the reference for medical staff to take effective countermeasures in advance in the future.
基金financially supported by the National Natural Science Foundation of China(Nos.22104112 and 22374110)the Fundamental Research Funds for the Central Universities。
文摘The investigation of reaction kinetics is the key to understanding the nature of reaction processes.However,monitoring fast photochemical reactions by mass spectrometry remains challenging.Herein,we developed an optical focusing inductive electrospray(OF-iESI)mass spectrometry platform for real-time and in-situ photoreaction monitoring.Coaxial irradiation from back of nanoelectrospray emitter with a taper section was utilized,so the emitter could act as optical lens to help achieving much larger optical power density at emitter tip compared to other sections,which allowed for in-situ reaction monitoring of photoreactions.Through theoretical calculations,the highest optical power density region volume was ca.45 nL.We also integrated a controller for the laser source(450 nm),enabling the modulation of pulse duration(>1 ms).This facilitates the study of photochemical reaction kinetics.The in-situ capability of this device was proved by capturing the short-lived photogenerated intermediates during the dehydrogenation of tetrahydroquinoline.This device was further used to investigate the kinetics of triplet energy transfer based Paternò-Büchi reaction.The reaction order has hitherto remained undetermined while the result of OF-iESI suggested it followed pseudo-second-order reaction kinetics.The short-lived donor-acceptor collision complex intermediate was also successfully identified by tandem mass spectrometry.
基金sponsored by the National Natural Science Foundations of China under Grant Nos.12301315,12235007,11975131the Zhejiang Provincial Natural Science Foundation of China under Grant No.LQ20A010009。
文摘In the realm of nonlinear integrable systems,the presence of decompositions facilitates the establishment of linear superposition solutions and the derivation of novel coupled systems exhibiting nonlinear integrability.By focusing on single-component decompositions within the potential BKP hierarchy,it has been observed that specific linear superpositions of decomposition solutions remain consistent with the underlying equations.Moreover,through the implementation of multi-component decompositions within the potential BKP hierarchy,successful endeavors have been undertaken to formulate linear superposition solutions and novel coupled Kd V-type systems that resist decoupling via alterations in dependent variables.
基金financially supported by the National Natural Science Foundation of China(Nos.52271033 and 52071179)the Key program of National Natural Science Foundation of China(No.51931003)+2 种基金Natural Science Foundation of Jiangsu Province,China(No.BK20221493)Jiangsu Province Leading Edge Technology Basic Research Major Project(No.BK20222014)Foundation of“Qinglan Project”for Colleges and Universities in Jiangsu Province.
文摘Multi-component transition group metal borides(MMB_(2))have become a research hotspot due to their new composition design concepts and superior properties compared with conventional ceramics.Most of the current methods,however,are complicated and time-consuming,the mass production remains a chal-lenge.Herein,we proposed a new high-efficiency strategy for synthesis of MMB_(2)using molten aluminum as the medium for the first time.The prepared Al-containing multi-component borides(TiZrHfNbTa)B_(2)microcrystals had a homogeneous composition with a hexagonal AlB_(2)structure and ultra-high hardness value of∼35.3 GPa,which was much higher than data reported in the literature and the rule of mix-ture estimations.Furthermore,combined with the First-principles calculation results,we found that the Poisson’s ratio(v)values exhibit a clearly ascending trend from 0.17 at VEC=3.5 to 0.18 at VEC=3.4,then to 0.201 at VEC=3.2 with the increasing of Al content.This indicates that the intrinsic toughness of multi-component boride microcrystals is obviously enhanced by the trace-doped Al elements.Besides,the fabricated Al-containing multi-component boride microcrystals have superior oxidation activation en-ergy and structural stability.The enhanced oxidation resistance is mainly attributed to the formation of a protective Al2 O3 oxide layer and the lattice distortion,both of which lead to sluggish diffusion of O_(2).These findings propose a new unexplored avenue for the fabrication of MMB_(2)materials with supe-rior comprehensive performance including ultra-hardness and intrinsically improved thermo-mechanical properties.
基金supported by the National Natural Science Foundation of China(Nos.22102167 and U21A20317)。
文摘Designing highly active electrocatalysts for the hydrogen evolution reaction(HER)and oxygen evolution and reduction reactions(OER and ORR)is pivotal to renewable energy technology.Herein,based on density functional theory(DFT)calculations,we systematically investigate the catalytic activity of iron-nitrogen-carbon based covalent organic frameworks(COF)monolayers with axially coordinated ligands(denotes as Fe N_(4)-X@COF,X refers to axial ligand,X=-SCN,-I,-H,-SH,-NO_(2),-Br,-ClO,-Cl,-HCO_(3),-NO,-ClO_(2),-OH,-CN and-F).The calculated results demonstrate that all the catalysts possess good thermodynamic and electrochemical stabilities.The different ligands axially ligated to the Fe active center could induce changes in the charge of the Fe center,which further regulates the interaction strength between intermediates and catalysts that governs the catalytic activity.Importantly,FeN_(4)-SH@COF and Fe N_(4)-OH@COF are efficient bifunctional catalysts for HER and OER,FeN_(4)-OH@COF and FeN_(4)-I@COF are promising bifunctional catalysts for OER and ORR.These findings not only reveal promising bifunctional HER/OER and OER/ORR catalysts but also provide theoretical guidance for designing optimum ironnitrogen-carbon based catalysts.
文摘This paper, an addendum to “Dialectical Thermodynamics’ solution to the conceptual imbroglio that is the reversible path”, this journal, 10, 775-799, was written in response to the requests of several readers to provide further evidence of the said “imbroglio”. The evidence here presented relates to the incompatibility existing between the total-entropy and the Gibbs energy prescriptions for the reversible path. The previously published proof of the negentropic nature of the transformation of heat into work is here included to validate out conclusions about the Gibbs energy perspective.
基金funded by the National Natural Science Foundation of China(22478632)Key Scientific and Technological Project of Henan Province(242102321032).
文摘Continuous-flow upgrading of pentaerythritol synthesis technology via base-catalyzed aldol and Cannizzaro reactions of formaldehyde and acetaldehyde faces the challenge of effectively controlling the critical side reaction of hydroxymethyl acetaldehyde(HA)to the acrolein intermediate.Here,we first identified the forms of industrial formaldehyde as methane diol that easily converts to the alkaline formaldehyde under alkaline(NaOH)environment.The carbonyl group of alkaline formaldehyde induces deprotonation of acetaldehyde instead of the recognized base-hydroxyl group-induced deprotonation,and it needs to overcome only 18.31 kcal·mol^(-1)(1 kcal=4.186 kJ)energy barrier to form key intermediates of HA.The sodium solvation cage formed by NaOH hexa-coordinated formaldehyde effectively inhibits the alkalinity,thus contributing to a high energy barrier(46.21 kcal·mol^(-1))to unwanted acrolein formation.In addition,the solvation cage gradually opens to increase the alkalinity with the consumption of formaldehyde,thus facilitating the subsequent Cannizzaro reaction(to overcome 11.77 kcal·mol^(-1)).In comparison,strong alkalinity promotes the formation of acrolein(36.65 kcal·mol^(-1))to initiate the acetal side reaction,while weak alkalinity reduces the possibility of the Cannizzaro reaction(to overcome 20.44 kcal·mol^(-1)).This theoretically reveals the importance of the segmented feeding of weak and strong bases to successively control the aldol reaction and Cannizzaro reaction,and the combination of Na_(2)CO_(3) or HCOONa with NaOH improves the pentaerythritol yield by 7%to 13%compared to that of NaOH alone(70%yield)within 1 min at a throughput of 155.7 ml·min^(-1).
基金supported by the Hainan Province Science and Technology Special Fund(ZDYF2020037)the National Natural Science Foundation of China(22109035,52164028,52274297,22462006)+3 种基金the Postdoctoral Science Foundation of Hainan Province(RZ2100007123)the Basic and Applied Basic Research Foundation of Guangdong Province(2019A1515110558)the Start-up Research Foundation of Hainan University(KYQD(ZR)-20008,20083,20084,21125)Hainan University(XTCX2022HYC05)。
文摘Efficient catalysis of the oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)is essential for the rechargeable zinc-air batteries(R-ZABs).However,challenges remain due to the scarcity of effective bifunctional electrocatalysts and limited understanding of the structure-activity relationships.Pyrrole-type single-atom catalysts(SACs)with unique electronic structures have emerged as promising electrocatalysts.In this work,we combine density functional theory(DFT)calculations and experimental studies to systematically explore the structure-activity relationships and potential of pyrrole-type transition metal-N_(3)(TM-po-N_(3))as bifunctional catalysts.DFT calculations reveal that differences in the dependence of ORR and OER activities on the free energy of adsorption of reaction intermediates significantly affect the TM-po-N_(3)bifunctional activity and identify magnetic Cu-po-N_(3)as the best candidate.The bifunctional activity of Cu-po-N_(3)originates from interactions between spin-polarized out-of-plane Cu_3d and O_2s+2p orbitals.Theoretical predictions are validated experimentally,showing that the synthesized Cu-SAC/NC exhibits excellent bifunctional performance with a small potential gap of 0.666 V.Additionally,the assembled R-ZABs display a high-power density of 170 mW cm^(-2)and long-term stability,with the charge-discharge voltage gap increasing by only 0.01 V over 240 h.This work provides new insights into the design of efficient bifunctional catalysts.
基金supported by the National Key Research and Development Program of China(No.2020YFA0607800)the National Natural Science Foundation of China(Nos.42022039 and 42130606)Beijing National Laboratory for Molecular Sciences(No.BNLMS-CXXM-202011),the Youth Innovation Promotion Association of Chinese Academy of Sciences(No.Y2021013).
文摘Unsaturated alcohols are a class of Biogenic volatile organic compounds(BVOCs)emitted in large quantities by plants when damaged or under adverse environmental conditions,and studies on their atmospheric degradation at night are still lacking.We used chamber experiments to study the gas-phase reactions of three unsaturated alcohols,E-2-penten-1-ol,Z-2-hexen-1-ol and Z-3-hepten-1-ol,with NO_(3)radicals(NO_(3)•)during the night.The rate constants of these reactions were(11.7±1.76)×10^(−13),(8.55±1.33)×10^(−13)and(6.08±0.47)×10^(−13)cm^(3)/(molecule·s)at 298K and 760 Torr,respectively.In contrast,the reaction rate of similar substances with ozone was about 10^(−18)cm^(3)/(molecule·s),which indicates that the reaction with NO_(3)•is themain oxidation pathway for unsaturated alcohols at night.Small molecule aldehydes and ketones were the main gas-phase organic products of the reaction of three aldehydes and ketones with NO_(3)•,and the total small molecule aldehydes and ketones yields can reach between 45%-60%.They mainly originate from the breakage of alkoxy radicals,and different breakage sites determine different product distributions.In addition,the SOA yields of the three unsaturated alcohols with NO_(3)•were 7.1%±1.0%,12.5%±1.9%and 30.0%±4.5%,respectively,whichweremuch higher than those of similarly structured substances with O_(3)or OH radicals(•OH).The results of high-resolution mass spectrometry shows that the main components of Secondary organic aerosol(SOA)of the three unsaturated alcohols are dimeric compounds containing several nitrate groups,which are formed through the polymerization of oxyalkyl radicals.
基金financially supported by the National Key R&D Program of China(No.2023YFA1606702)the National Natural Science Foundation of China(Nos.U2067205 and 12205098).
文摘The Glauber/eikonal model is a widely used tool for studying intermediate-and high-energy nuclear reactions.When calculating the Glauber/eikonal model phase shift functions,the optical limit approximation(OLA)is often used.The OLA neglects the multiple scattering of the constituent nucleons in the projectile and target nuclei.However,the nucleon-target version of the Glauber model(the NTG model)proposed by Abu-Ibrahim and Suzuki includes multiple scattering effects between the projectile nucleons and target nuclei.The NTG model was found to improve the description of the elastic scattering angular distributions and total reaction cross sections of some light heavy-ion systems with respect to the OLA.In this work,we study the single-nucleon removal reactions(SNRRs)induced by carbon isotopes on ^(12)C and ^(9)Be targets using both the NTG model and the OLA.Reduction factors(RFs)of the single-nucleon spectroscopic factors were obtained by comparing the experimental and theoretical SNRR cross sections.On average,the RFs obtained with the NTG model were smaller than those obtained using the OLA by 7.8%,in which the average difference in one-neutron removal was 10.6% and that in one-proton removal was 4.2%.However,the RFs were still strongly dependent on the neutron-proton asymmetryΔS of the projectile nuclei,even when the NTG model was used.
基金supported by National Natural Science Foundation of China(52371095)Innovation Research Group of Universities in Chongqing(CXQT21030)+2 种基金Chongqing Overseas Chinese Entrepreneurship and Innovation Support Program(cx2023117)Chongqing Natural Science Foundation(CSTB2022NSCQ-LZX0054,CSTB2024TIADCYKJCXX0001)Chongqing Youth Expert Studio。
文摘Mg batteries have high energy density,economic safety,and environmental friendliness.They show great potential as an ideal energy storage technology.This review summarizes the limitations of Mg batteries and explores the complex reactions at the Mg anode/electrolyte interface.It focuses on critical issues such as the dissolution of Mg anodes,the evolution of hydrogen gas,the formation of a passivation layer that hinders Mg^(2+)migration,and dendrite growth.To address these interface problems,the review discusses strategies to improve interface reactions.These include the structural design of Mg anodes,suitable substitute materials for the anode,and artificial solid electrolyte interphase films.Finally,it outlines the future research directions for the ideal Mg anode interfaces.The goal is to develop more efficient interface design schemes and optimization strategies to advance Mg battery technology further.
基金funded by the European Union via the Euratom Research and Training Program(Grant Agreement No.101052200-EUROfusion)funding from LASERLAB-EUROPE(Grant Agreement No.871124,European Union’s Horizon 2020 Research and Innovation Program)+5 种基金supported in part by the United States Department of Energy under Grant No.DE-FG02-93ER40773We also acknowledge support from Grant No.PID2021-125389OA-I00 funded by MCIN/AEI/10.13039/501100011033/FEDER,UEby“ERDF A Way of Making Europe”by the European Union and Unidad de Investigación Consolidada of Junta de Castilla y León UIC 167supported in part by the National Natural Science Foundation of China under Grant No.12375125the Fundamental Research Funds for the Central Universitiesthe support of the Czech Science Foundation through Grant No.GACR24-11398S.
文摘Driving of the nuclear fusion reaction p+^(11)B3α+8.7 MeV under laboratory conditions by interaction between high-power laser pulses and matter has become a popular field of research,owing to its numerous potential applications:as an alternative to deuterium-tritium for fusion energy production,astrophysics studies,and alpha-particle generation for medical treatment.One possible scheme for laser-driven p-^(11)B reactions is to direct a beam of laser-accelerated protons onto a boron(B)sample(the so-called“pitcher-catcher”scheme).This technique has been successfully implemented on large high-energy lasers,yielding hundreds of joules per shot at low repetition.We present here a complementary approach,exploiting the high repetition rate of the VEGA III petawatt laser at CLPU(Spain),aiming at accumulating results from many interactions at much lower energy,to provide better control of the parameters and the statistics of the measurements.Despite a moderate energy per pulse,our experiment allowed exploration of the laser-driven fusion process with tens(up to hundreds)of laser shots.The experiment provided a clear signature of the reactions involved and of the fusion products,accumulated over many shots,leading to an improved optimization of the diagnostics for experimental campaigns of this type.In this paper,we discuss the effectiveness of laser-driven p-11B fusion in the pitcher-catcher scheme,at a high repetition rate,addressing the challenges of this experimental scheme and highlighting its critical aspects.Our proposed methodology allows evaluation of the performance of this scheme for laser-driven alpha particle production and can be adapted to high-repetition-rate laser facilities with higher energy and intensity.
文摘Objective:To explore the adverse reactions associated with antibiotics and analyze strategies for their rational use.Methods:A retrospective analysis was conducted on 60 patients who experienced adverse reactions to antibiotics between August 2021 and August 2023.The types of antibiotics that caused adverse reactions were analyzed,and the symptoms of adverse reactions and measures for rational use of antibiotics were summarized.Results:Among the analyzed cases of adverse reactions to antibiotics,the highest rate was observed in patients aged 61–75 years,accounting for 38.33%,followed by patients aged 51–60 years,accounting for 20.00%.In terms of the types of antibiotics that caused adverse reactions,cephalosporins were the most common,accounting for 40.00%,followed by penicillins,accounting for 18.33%.Analysis of the systems involved in adverse reactions showed that skin and appendage disorders were the most common,accounting for 36.67%,followed by the digestive system,accounting for 28.33%.Conclusion:Irrational use of antibiotics can lead to adverse drug reactions.Therefore,it is necessary to analyze strategies for the rational use of antibiotics to reduce adverse drug reactions and ensure the safety of antibiotic use.
基金Supported by Enhancement Project of Basic Scientific Research Ability of Young and Middle-aged Teachers in Guangxi Universities(2020KY07040)School-level Scientific Research Project of Guangxi University of Chinese Medicine(2024QN022)Self-financed Scientific Research Project of Guangxi Zhuang Autonomous Region Administration of Traditional Chinese Medicine(GXZYL20240818).
文摘[Objectives]To explore the methods for identifying pure honey.[Methods]Using 35 batches of Jiulongteng honey sourced from various production areas in Guangxi as the research subjects,this study investigated the chromogenic reactions of starch and dextrin,as well as the comparative study of thin-layer chromatography of oligosaccharides present in Jiulongteng honey.[Results]None of the 35 batches of Jiulongteng honey samples exhibited blue(indicating starch),green,or reddish-brown(indicating dextrin)coloration,suggesting that no adulterants such as artificially added starch,dextrin,or sugar were present in these samples.Furthermore,none of the 35 batches displayed additional spots below the corresponding positions of the control,indicating that the sugar composition was consistent with the oligosaccharide profile of natural honey.No components inconsistent with the oligosaccharide profile of natural honey were detected.Therefore,it can be concluded that the Jiulongteng honey samples in this experiment were pure and free from adulteration with starch,dextrin,or other sugar substances.[Conclusions]The method employed in this experiment is straightforward and quick to implement,effectively preventing adulterated honey from entering the market.It enhances the efficiency of quality control for Jiulongteng honey and promotes the healthy development of the Jiulongteng honey industry.