An efficient and novel procedure for the preparation of pyrazolo[3,4-b]pyridine derivatives through multi-component reaction of aldehyde, 5-amino-3-methyl-1-phenylpyrazole and malononitrile or cyanoacetate in [bmim][B...An efficient and novel procedure for the preparation of pyrazolo[3,4-b]pyridine derivatives through multi-component reaction of aldehyde, 5-amino-3-methyl-1-phenylpyrazole and malononitrile or cyanoacetate in [bmim][BF4] is described in this paper. Advantages of the method presented here include mild conditions, high yields together with a green nature and ease of recovery and reuse of the reaction medium.展开更多
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
Oxonium ylide intermediates generated from α-diazocarbonyl compounds and water were trapped by Zn（Ⅱ）-activated α- dicarbonyl compounds. The reaction gave α,β-dihydroxyl acid derivatives in moderate yield.
An expedient,synthetic method to fused polycyclic derivatives of isoquinoline is described via tandem reaction of isoquinoline,dialkyl acetylenedicarboxylates and dialkyl chloromalonate.
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
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
A mild and efficient photochemical multi-component tandem reaction of quinoxalin-2(1H)-ones, alkenes and sulfinic acids is reported. This tandem reaction could be conveniently carried out at room temperature by employ...A mild and efficient photochemical multi-component tandem reaction of quinoxalin-2(1H)-ones, alkenes and sulfinic acids is reported. This tandem reaction could be conveniently carried out at room temperature by employing 4Cz IPN as the metal-free photocatalyst and dioxygen(air) as the environmentally benign oxidant. A number of sulfonated quinoxalin-2(1H)-ones were obtained in satisfactory yields with favorable functional group tolerance. Radical trapping experiment and fluorescence quenching experiments were performed to elucidate this visible-light mediated radical reaction process.展开更多
A thermally-induced multi-component reaction of CF_(3)-substituted imidoyl sulfoxonium ylides(TFISYs),amines and(triphenylphosphonio)difluoroacetate(PDFA)has been developed,allowing a facile access to 2-trifluoromethy...A thermally-induced multi-component reaction of CF_(3)-substituted imidoyl sulfoxonium ylides(TFISYs),amines and(triphenylphosphonio)difluoroacetate(PDFA)has been developed,allowing a facile access to 2-trifluoromethyl-4-aminoquinolines in high yields.The reaction proceeds smoothly with or without the addition of sulfur and utilizes difluorocarbene as a C1 synthon under simply heating conditions.Mechanistic study reveals that in-situ generated thiocarbonyl fluoride,isothiocyanate or gem-difluoroalkene might act as the key reaction intermediates.展开更多
Paclitaxel(Taxol^(@))as a cornerstone of chemotherapy remains in high demand.The semi-synthesis of paclitaxel via coupling of Taxus leaf-produced baccatin III and manually synthesized isoserine(C-13 side chain)is one ...Paclitaxel(Taxol^(@))as a cornerstone of chemotherapy remains in high demand.The semi-synthesis of paclitaxel via coupling of Taxus leaf-produced baccatin III and manually synthesized isoserine(C-13 side chain)is one of the solutions to avoid environmental damage caused by the sacrifice of the whole Taxus brevifolia.A green synthesis of the C-13 side chain is pivotal to the green production of paclitaxel.We herein report a green synthesis of isoserine derivatives and the semi-synthesis of paclitaxel via a straightforward assembly of isoserines based on an Rh2(TPA)3(OAc)/CPA1 co-catalyzed asymmetric multi-component reaction of ethyl diazoacetate,triethyl silanol and N-(anthrancen-9-ylmethyl)benzaldimine.The method is featured by improved atom economy,effective mass yield,and environmental factors compared to our previous racemic method and BMS company's semi-synthesis method.And the method allows for rapid access to paclitaxel derivatives with varied C-13 side chains.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
The spiral-wound heat exchanger(SWHE) is the primary low-temperature heat exchanger for large-scale LNG plants due to its high-pressure resistance, compact structure, and high heat exchange efficiency. This paper stud...The spiral-wound heat exchanger(SWHE) is the primary low-temperature heat exchanger for large-scale LNG plants due to its high-pressure resistance, compact structure, and high heat exchange efficiency. This paper studied the shell-side heat and mass transfer characteristics of vapor-liquid two-phase mixed refrigerants in an SWHE by combining a multi-component model in FLUENT software with a customized multicomponent mass transfer model. Besides, the mathematical model under the sloshing condition was obtained through mathematical derivation, and the corresponding UDF code was loaded into FLUENT as the momentum source term. The results under the sloshing conditions were compared with the relevant parameters under the steady-state condition. The shell-side heat and mass transfer characteristics of the SWHE were investigated by adjusting the component ratio and other working conditions. It was found that the sloshing conditions enhance the heat transfer performance and sometimes have insignificant effects. The sloshing condition is beneficial to reduce the flow resistance. The comprehensive performance of multi-component refrigerants has been improved and the improvement is more significant under sloshing conditions, considering both the heat transfer and pressure drop.These results will provide theoretical support for the research and design of multi-component heat and mass transfer enhancement of LNG SWHE under ocean sloshing conditions.展开更多
Wearable,flexible devices have garnered widespread attention in the realm of human motion and life activity detection.Currently,the development of simple,green,and easily scalable methods for fabricating strain sensor...Wearable,flexible devices have garnered widespread attention in the realm of human motion and life activity detection.Currently,the development of simple,green,and easily scalable methods for fabricating strain sensors still presents significant challenges.In this study,we successfully modified the surface of reduced graphene oxide(rGO)with SnCuNiIn multi-component alloy nanoparticles(MCA NPs),with an average size of 13.29 nm,utilizing a green and facile microwave heating approach.Leveraging the SnCuNiIn MCA NPs/rGO powder,we formulated a conductive ink based on water and ethylene glycol,which,when screen-printed,yielded conductive patterns with a minimum resistivity of 4.366 mΩ·cm.Strain sensors produced using this ink demonstrate exceptional performance,demonstrating favorable resistance change rates during a single bending process that meets practical application requirements,and enduring 5000 bending cycles with a resistance change of less than 5%.These sensors exhibited a high gauge factor(GF_(max)=52.7)and outstanding cycling stability.Lastly,strain sensors are employed to monitor human normal life activities and motion states,showcasing significant potential for application in wearable electronic products.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
Sulfur-doped iron-cobalt tannate nanorods(S-FeCoTA)derived from metal-organic frameworks(MOFs)as electrocatalysts were synthesized via a one-step hydrothermal method.The optimized S-FeCoTA was interlaced by loose nano...Sulfur-doped iron-cobalt tannate nanorods(S-FeCoTA)derived from metal-organic frameworks(MOFs)as electrocatalysts were synthesized via a one-step hydrothermal method.The optimized S-FeCoTA was interlaced by loose nanorods,which had many voids.The S-FeCoTA catalysts exhibited excellent electrochemical oxygen evolution reaction(OER)performance with a low overpotential of 273 mV at 10 mA·cm^(-2)and a small Tafel slope of 36 mV·dec^(-1)in 1 mol·L^(-1)KOH.The potential remained at 1.48 V(vs RHE)at 10 mA·cm^(-2)under continuous testing for 15 h,implying that S-FeCoTA had good stability.The Faraday efficiency of S-FeCoTA was 94%.The outstanding OER activity of S-FeCoTA is attributed to the synergistic effects among S,Fe,and Co,thus promoting electron transfer,reducing the reaction kinetic barrier,and enhancing the OER performance.展开更多
An efficient,convenient and environmentally benign procedure for the synthesis of novel 3-oxo-3Hbenzo[a]pyrano[2.3-c]phenazine-l-carboxylate and 3-（5-hydroxybenzo[a]phenazin-6-yl） acrylate derivatives has been devel...An efficient,convenient and environmentally benign procedure for the synthesis of novel 3-oxo-3Hbenzo[a]pyrano[2.3-c]phenazine-l-carboxylate and 3-（5-hydroxybenzo[a]phenazin-6-yl） acrylate derivatives has been developed by domino three-component condensation reaction between 2-hydroxynaphthalene-1,4-dione,benzene-1,2-diamines and acetylenic esters in the presence of a catalytic amount of DABCO as an expedient,eco-friendly and reusable base catalyst in water.This green process produces biologically and pharmacologically significant heterocycles in a one-pot single operation and offers considerable advantages such as：operational simplicity,short reaction time,high yields,reusability of catalyst,absence of any tedious workup or purification and avoids hazardous reagents/solvents.展开更多
Nitrogen-doping of carbon support(N-C)for platinum(Pt)nanoparticles to form Pt/N-C catalyst represents an effective strategy to promote the electrocatalysis of cathodic oxygen reduction reaction(ORR)in proton exchange...Nitrogen-doping of carbon support(N-C)for platinum(Pt)nanoparticles to form Pt/N-C catalyst represents an effective strategy to promote the electrocatalysis of cathodic oxygen reduction reaction(ORR)in proton exchange membrane fuel cells.For fundamental understanding,clearly identifying the metalsupport effect on enhancement mechanisms of ORR electrocatalysis is definitely needed.In this work,the impact of Pt-support interaction via interfacial Pt-N coordination on electrocatalytic ORR activity and stability in Pt/N-C catalyst is deeply studied through structural/compositional characterizations,electrochemical measurements and theoretical DFT-calculations/AIMD-simulations.The resulting Pt/N-C catalyst exhibits a superior electrocatalytic performance compared to the commercial Pt/C catalyst in both half-cell and H_(2)-O_(2)fuel cell.Experimental and theoretical results reveal that the interfacial Pt-N coordination enables electron transfer from N-C support to Pt nanoparticles,which can weaken the adsorption strength of oxygen intermediates on Pt surface to improve ORR activity and induce the strong Pt-support interaction to enhance electrochemical stability.展开更多
The development of an e fficacious and easily prepared no nprecious metal electrocatalyst is crucial for the oxygen reduction reaction(ORR).This work used a dual template method to prepare the amorphous rare earth-bas...The development of an e fficacious and easily prepared no nprecious metal electrocatalyst is crucial for the oxygen reduction reaction(ORR).This work used a dual template method to prepare the amorphous rare earth-based catalyst PrO_(x)-NC,and optimized the calcination temperature and proportion.The PrO_(x)-NC-900 catalyst has high durability and activity and exhibits superior ORR performance in alkaline electrolytes with an onset potential(E_(0))of 0.96 V and a half-wave potential(E_(1/2))of 0.85 V.The research results indicate that the ORR performance of rare earth oxide composite carbon catalysts can be improved by adjusting oxygen vacancies(Ov).In addition,high specific surface area,N rich defect carbon.increased oxygen vacancies,and the synergistic effect of oxygen vacancies and N-doped carbon interfacial layer play a significant part in the enhancement of ORR.The performance of the zinc air battery assembled with PrO_(x)-NC-900 is significantly improved,and rare earth oxides and carbon frameworks originating from metal organic frameworks(MOFs)contribute to the oxygen electrocatalyst and electron transfer rate of the zinc air battery.This catalyst provides promising information for the development of rare earth metal oxide nanostructures as potential candidate materials for ORR in alkaline media.展开更多
Pt-based nanocatalysts offer excellent prospects for various industries.However,the low loading of Pt with excellent performance for efficient and stable nanocatalysts still presents a considerable challenge.In this s...Pt-based nanocatalysts offer excellent prospects for various industries.However,the low loading of Pt with excellent performance for efficient and stable nanocatalysts still presents a considerable challenge.In this study,nanocatalysts with ultralow Pt content,excellent performance,and carbon black as support were prepared through in-situ synthesis.These~2-nm particles uniformly and stably dispersed on carbon black because of the strong s-p-d orbital hybridizations between carbon black and Pt,which suppressed the agglomeration of Pt ions.This unique structure is beneficial for the hydrogen evolution reaction.The catalysts exhibited remarkable catalytic activity for hydrogen evolution reaction,exhibiting a potential of 100 mV at 100 mA·cm^(-2),which is comparable to those of commercial Pt/C catalysts.Mass activity(1.61 A/mg)was four times that of a commercial Pt/C catalyst(0.37 A/mg).The ultralow Pt loading(6.84wt%)paves the way for the development of next-generation electrocatalysts.展开更多
Oxygen release and electrolyte decomposition under high voltage endlessly exacerbate interfacial ramifications and structu ral degradation of high energy-density Li-rich layered oxide(LLO),leading to voltage and capac...Oxygen release and electrolyte decomposition under high voltage endlessly exacerbate interfacial ramifications and structu ral degradation of high energy-density Li-rich layered oxide(LLO),leading to voltage and capacity fading.Herein,the dual-strategy of Cr,B complex coating and local gradient doping is simultaneously achieved on LLO surface by a one-step wet chemical reaction at room temperature.Density functional theory(DFT)calculations prove that stable B-O and Cr-O bonds through the local gradient doping can significantly reduce the high-energy O 2p states of interfacial lattice O,which is also effective for the near-surface lattice O,thus greatly stabilizing the LLO surface,Besides,differential electrochemical mass spectrometry(DEMS)indicates that the Cr_(x)B complex coating can adequately inhibit oxygen release and prevents the migration or dissolution of transition metal ions,including allowing speedy Li^(+)migration,The voltage and capacity fading of the modified cathode(LLO-C_(r)B)are adequately suppressed,which are benefited from the uniformly dense cathode electrolyte interface(CEI)composed of balanced organic/inorganic composition.Therefore,the specific capacity of LLO-CrB after 200 cycles at 1C is 209.3 mA h g^(-1)(with a retention rate of 95.1%).This dual-strategy through a one-step wet chemical reaction is expected to be applied in the design and development of other anionic redox cathode materials.展开更多
基金the National Natural Science Foundation of China(No.20573034).
文摘An efficient and novel procedure for the preparation of pyrazolo[3,4-b]pyridine derivatives through multi-component reaction of aldehyde, 5-amino-3-methyl-1-phenylpyrazole and malononitrile or cyanoacetate in [bmim][BF4] is described in this paper. Advantages of the method presented here include mild conditions, high yields together with a green nature and ease of recovery and reuse of the reaction medium.
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.
基金supported by National Science Foundation of China(No.20772033)China postdoctoral Science Foundation(No.20080440607)
文摘Oxonium ylide intermediates generated from α-diazocarbonyl compounds and water were trapped by Zn（Ⅱ）-activated α- dicarbonyl compounds. The reaction gave α,β-dihydroxyl acid derivatives in moderate yield.
基金Sanandaj Branch, Islamic Azad University Research Council for the fnancial support of this research
文摘An expedient,synthetic method to fused polycyclic derivatives of isoquinoline is described via tandem reaction of isoquinoline,dialkyl acetylenedicarboxylates and dialkyl chloromalonate.
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.
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 Youth Innovation and Technology Project of high School in Shandong Province (No. 2019KJC021)Natural Science Foundation of Qinghai Province of China (No. 2020-ZJ-915)。
文摘A mild and efficient photochemical multi-component tandem reaction of quinoxalin-2(1H)-ones, alkenes and sulfinic acids is reported. This tandem reaction could be conveniently carried out at room temperature by employing 4Cz IPN as the metal-free photocatalyst and dioxygen(air) as the environmentally benign oxidant. A number of sulfonated quinoxalin-2(1H)-ones were obtained in satisfactory yields with favorable functional group tolerance. Radical trapping experiment and fluorescence quenching experiments were performed to elucidate this visible-light mediated radical reaction process.
基金financial support from K.C.Wong Education Foundation(GJTD-2020-08).
文摘A thermally-induced multi-component reaction of CF_(3)-substituted imidoyl sulfoxonium ylides(TFISYs),amines and(triphenylphosphonio)difluoroacetate(PDFA)has been developed,allowing a facile access to 2-trifluoromethyl-4-aminoquinolines in high yields.The reaction proceeds smoothly with or without the addition of sulfur and utilizes difluorocarbene as a C1 synthon under simply heating conditions.Mechanistic study reveals that in-situ generated thiocarbonyl fluoride,isothiocyanate or gem-difluoroalkene might act as the key reaction intermediates.
基金Support for this research from the National Natural Science Foundation of China(Nos.92056201 and 82003592)Guangdong Provincial Key Laboratory of Chiral Molecule and Drug Discovery(No.2019B030301005)The Program for Guangdong Introducing Innovative and Entrepreneurial Teams(No.2016ZT06Y337)and Zhujiang Talent Program Postdoctoral Funding Project is greatly acknowledged。
文摘Paclitaxel(Taxol^(@))as a cornerstone of chemotherapy remains in high demand.The semi-synthesis of paclitaxel via coupling of Taxus leaf-produced baccatin III and manually synthesized isoserine(C-13 side chain)is one of the solutions to avoid environmental damage caused by the sacrifice of the whole Taxus brevifolia.A green synthesis of the C-13 side chain is pivotal to the green production of paclitaxel.We herein report a green synthesis of isoserine derivatives and the semi-synthesis of paclitaxel via a straightforward assembly of isoserines based on an Rh2(TPA)3(OAc)/CPA1 co-catalyzed asymmetric multi-component reaction of ethyl diazoacetate,triethyl silanol and N-(anthrancen-9-ylmethyl)benzaldimine.The method is featured by improved atom economy,effective mass yield,and environmental factors compared to our previous racemic method and BMS company's semi-synthesis method.And the method allows for rapid access to paclitaxel derivatives with varied C-13 side chains.
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.
基金funded by the National Natural Science Foundation of China(No.51806236,No.51806239)the Fundamental Research Funds for the Central Universities(No.2015XKMS059)+1 种基金Shaanxi Postdoctoral Fund Project(No.2018BSHEDZZ56)Foundation of Key Laboratory of Thermo-Fluid Science and Engineering(Xi'an Jiaotong University),Ministry of Education(No.KLTFSE2017KF01)。
文摘The spiral-wound heat exchanger(SWHE) is the primary low-temperature heat exchanger for large-scale LNG plants due to its high-pressure resistance, compact structure, and high heat exchange efficiency. This paper studied the shell-side heat and mass transfer characteristics of vapor-liquid two-phase mixed refrigerants in an SWHE by combining a multi-component model in FLUENT software with a customized multicomponent mass transfer model. Besides, the mathematical model under the sloshing condition was obtained through mathematical derivation, and the corresponding UDF code was loaded into FLUENT as the momentum source term. The results under the sloshing conditions were compared with the relevant parameters under the steady-state condition. The shell-side heat and mass transfer characteristics of the SWHE were investigated by adjusting the component ratio and other working conditions. It was found that the sloshing conditions enhance the heat transfer performance and sometimes have insignificant effects. The sloshing condition is beneficial to reduce the flow resistance. The comprehensive performance of multi-component refrigerants has been improved and the improvement is more significant under sloshing conditions, considering both the heat transfer and pressure drop.These results will provide theoretical support for the research and design of multi-component heat and mass transfer enhancement of LNG SWHE under ocean sloshing conditions.
基金financially supported by Heilongjiang Provincial Natural Science Foundation of China(No.YQ2022E024)the National Natural Science Foundation of China(No.52375327)。
文摘Wearable,flexible devices have garnered widespread attention in the realm of human motion and life activity detection.Currently,the development of simple,green,and easily scalable methods for fabricating strain sensors still presents significant challenges.In this study,we successfully modified the surface of reduced graphene oxide(rGO)with SnCuNiIn multi-component alloy nanoparticles(MCA NPs),with an average size of 13.29 nm,utilizing a green and facile microwave heating approach.Leveraging the SnCuNiIn MCA NPs/rGO powder,we formulated a conductive ink based on water and ethylene glycol,which,when screen-printed,yielded conductive patterns with a minimum resistivity of 4.366 mΩ·cm.Strain sensors produced using this ink demonstrate exceptional performance,demonstrating favorable resistance change rates during a single bending process that meets practical application requirements,and enduring 5000 bending cycles with a resistance change of less than 5%.These sensors exhibited a high gauge factor(GF_(max)=52.7)and outstanding cycling stability.Lastly,strain sensors are employed to monitor human normal life activities and motion states,showcasing significant potential for application in wearable electronic products.
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.
文摘Sulfur-doped iron-cobalt tannate nanorods(S-FeCoTA)derived from metal-organic frameworks(MOFs)as electrocatalysts were synthesized via a one-step hydrothermal method.The optimized S-FeCoTA was interlaced by loose nanorods,which had many voids.The S-FeCoTA catalysts exhibited excellent electrochemical oxygen evolution reaction(OER)performance with a low overpotential of 273 mV at 10 mA·cm^(-2)and a small Tafel slope of 36 mV·dec^(-1)in 1 mol·L^(-1)KOH.The potential remained at 1.48 V(vs RHE)at 10 mA·cm^(-2)under continuous testing for 15 h,implying that S-FeCoTA had good stability.The Faraday efficiency of S-FeCoTA was 94%.The outstanding OER activity of S-FeCoTA is attributed to the synergistic effects among S,Fe,and Co,thus promoting electron transfer,reducing the reaction kinetic barrier,and enhancing the OER performance.
基金financial support from the Research Council of Young ResearchersElite Club of the Islamic Azad University of YazdUniversity of Sistan and Baluchestan
文摘An efficient,convenient and environmentally benign procedure for the synthesis of novel 3-oxo-3Hbenzo[a]pyrano[2.3-c]phenazine-l-carboxylate and 3-（5-hydroxybenzo[a]phenazin-6-yl） acrylate derivatives has been developed by domino three-component condensation reaction between 2-hydroxynaphthalene-1,4-dione,benzene-1,2-diamines and acetylenic esters in the presence of a catalytic amount of DABCO as an expedient,eco-friendly and reusable base catalyst in water.This green process produces biologically and pharmacologically significant heterocycles in a one-pot single operation and offers considerable advantages such as：operational simplicity,short reaction time,high yields,reusability of catalyst,absence of any tedious workup or purification and avoids hazardous reagents/solvents.
基金supported by the National Natural Science Foundation of China(Nos.22272105 and 22002110)Natural Science Foundation of Shanghai(No.23ZR1423900)。
文摘Nitrogen-doping of carbon support(N-C)for platinum(Pt)nanoparticles to form Pt/N-C catalyst represents an effective strategy to promote the electrocatalysis of cathodic oxygen reduction reaction(ORR)in proton exchange membrane fuel cells.For fundamental understanding,clearly identifying the metalsupport effect on enhancement mechanisms of ORR electrocatalysis is definitely needed.In this work,the impact of Pt-support interaction via interfacial Pt-N coordination on electrocatalytic ORR activity and stability in Pt/N-C catalyst is deeply studied through structural/compositional characterizations,electrochemical measurements and theoretical DFT-calculations/AIMD-simulations.The resulting Pt/N-C catalyst exhibits a superior electrocatalytic performance compared to the commercial Pt/C catalyst in both half-cell and H_(2)-O_(2)fuel cell.Experimental and theoretical results reveal that the interfacial Pt-N coordination enables electron transfer from N-C support to Pt nanoparticles,which can weaken the adsorption strength of oxygen intermediates on Pt surface to improve ORR activity and induce the strong Pt-support interaction to enhance electrochemical stability.
基金Project supported by the National Natural Science Foundation of China(22062019)the Natural Science Foundation of Inner Mongolia of China(2022QN02002)Science and Technology Program of Inner Mongolia Autonomous Region,China(2020PT0003)。
文摘The development of an e fficacious and easily prepared no nprecious metal electrocatalyst is crucial for the oxygen reduction reaction(ORR).This work used a dual template method to prepare the amorphous rare earth-based catalyst PrO_(x)-NC,and optimized the calcination temperature and proportion.The PrO_(x)-NC-900 catalyst has high durability and activity and exhibits superior ORR performance in alkaline electrolytes with an onset potential(E_(0))of 0.96 V and a half-wave potential(E_(1/2))of 0.85 V.The research results indicate that the ORR performance of rare earth oxide composite carbon catalysts can be improved by adjusting oxygen vacancies(Ov).In addition,high specific surface area,N rich defect carbon.increased oxygen vacancies,and the synergistic effect of oxygen vacancies and N-doped carbon interfacial layer play a significant part in the enhancement of ORR.The performance of the zinc air battery assembled with PrO_(x)-NC-900 is significantly improved,and rare earth oxides and carbon frameworks originating from metal organic frameworks(MOFs)contribute to the oxygen electrocatalyst and electron transfer rate of the zinc air battery.This catalyst provides promising information for the development of rare earth metal oxide nanostructures as potential candidate materials for ORR in alkaline media.
基金financially supported by the National Natural Science Foundation of China(No.5217042069)the Young Elite Scientist Sponsorship Program by China Association for Science and Technology(CAST)(No.YESS20200103)the Fundamental Research Funds for the Central Universities(No.265QZ2022004)。
文摘Pt-based nanocatalysts offer excellent prospects for various industries.However,the low loading of Pt with excellent performance for efficient and stable nanocatalysts still presents a considerable challenge.In this study,nanocatalysts with ultralow Pt content,excellent performance,and carbon black as support were prepared through in-situ synthesis.These~2-nm particles uniformly and stably dispersed on carbon black because of the strong s-p-d orbital hybridizations between carbon black and Pt,which suppressed the agglomeration of Pt ions.This unique structure is beneficial for the hydrogen evolution reaction.The catalysts exhibited remarkable catalytic activity for hydrogen evolution reaction,exhibiting a potential of 100 mV at 100 mA·cm^(-2),which is comparable to those of commercial Pt/C catalysts.Mass activity(1.61 A/mg)was four times that of a commercial Pt/C catalyst(0.37 A/mg).The ultralow Pt loading(6.84wt%)paves the way for the development of next-generation electrocatalysts.
基金financially supported by the National Natural Science Foundation of China(No.12304077)the Natural Science Foundation of Science and Technology Department of Sichuan Province(No.23NSFSC6224)+3 种基金Sichuan Science and Technology Program(No.2024NSFSC0989)the Key Laboratory of Computational Physics of Sichuan Province(No.YBUJSWL-YB-2022-03)the Material Corrosion and Protection Key Laboratory of Sichuan Province(No.2023CL14 and No.2023CL01)the National Innovation Practice Project(No.202411079005S).
文摘Oxygen release and electrolyte decomposition under high voltage endlessly exacerbate interfacial ramifications and structu ral degradation of high energy-density Li-rich layered oxide(LLO),leading to voltage and capacity fading.Herein,the dual-strategy of Cr,B complex coating and local gradient doping is simultaneously achieved on LLO surface by a one-step wet chemical reaction at room temperature.Density functional theory(DFT)calculations prove that stable B-O and Cr-O bonds through the local gradient doping can significantly reduce the high-energy O 2p states of interfacial lattice O,which is also effective for the near-surface lattice O,thus greatly stabilizing the LLO surface,Besides,differential electrochemical mass spectrometry(DEMS)indicates that the Cr_(x)B complex coating can adequately inhibit oxygen release and prevents the migration or dissolution of transition metal ions,including allowing speedy Li^(+)migration,The voltage and capacity fading of the modified cathode(LLO-C_(r)B)are adequately suppressed,which are benefited from the uniformly dense cathode electrolyte interface(CEI)composed of balanced organic/inorganic composition.Therefore,the specific capacity of LLO-CrB after 200 cycles at 1C is 209.3 mA h g^(-1)(with a retention rate of 95.1%).This dual-strategy through a one-step wet chemical reaction is expected to be applied in the design and development of other anionic redox cathode materials.
