Ga(ClO4)3-catalyzed reaction of 1,2-aryldiamines and α-bromoketones to afford 2-substituted quinoxalines in good yields is described.The reaction proceeded via grinding process with 10%(molar fraction) catalyst u...Ga(ClO4)3-catalyzed reaction of 1,2-aryldiamines and α-bromoketones to afford 2-substituted quinoxalines in good yields is described.The reaction proceeded via grinding process with 10%(molar fraction) catalyst under solvent-free conditions at room temperature.For unsymmetrical o-phenylenediamines bearing electron-withdrawing groups,regio-selective quinoxalines were obtained.展开更多
A facile one-pot synthesis of 3,4,5-substituted furan-2(5H)-one derivatives from a three-component reaction of aniline derivatives, dialkylacetylenedicarboxylates and aromatic aldehydes under mild conditions using t...A facile one-pot synthesis of 3,4,5-substituted furan-2(5H)-one derivatives from a three-component reaction of aniline derivatives, dialkylacetylenedicarboxylates and aromatic aldehydes under mild conditions using tetra-n-butylammonium bisulfate as a catalyst has been developed.展开更多
In this work,six novel axially unfixed biaryl-based water-compatible bifunctional organocatalysts were de-signed and synthesized for the organocatalytic access to a variety of 3-alkyl-3-hydroxy-2-oxindole derivatives ...In this work,six novel axially unfixed biaryl-based water-compatible bifunctional organocatalysts were de-signed and synthesized for the organocatalytic access to a variety of 3-alkyl-3-hydroxy-2-oxindole derivatives via aldol reactions in water.Organocatalyzed by 5a,the direct aldol reactions of isatins with enolisable ketones under-went readily in water,furnishing the structurally diverse 3-alkyl-3-hydroxy-2-oxindoles in various stereoselectivi-ties(up to>99%dr and>99%ee).Moreover,a plausible transition state of the conducted aldol reactions was hy-pothesized to shed light on the observed stereoselectivities of the obtained 3-alkyl-3-hydroxy-2-oxindoles.展开更多
1-Substituted 1,2,3-triazoles represents‘privileged’structural scaffolds of many clinical pharmaceuticals.However,the traditional methods for their preparation mainly rely on thermal[3+2]cycloaddition of potentially...1-Substituted 1,2,3-triazoles represents‘privileged’structural scaffolds of many clinical pharmaceuticals.However,the traditional methods for their preparation mainly rely on thermal[3+2]cycloaddition of potentially dangerous acetylene and azides.Here we report a base-mediated[4+1]annulation of azoalkenes generated in situ from readily available difluoroacetaldehyde N-tosylhydrazones(DFHZ-Ts)with amines under relatively mild conditions.This azide-and acetylene-free strategy provides facile access to diverse 1-substituted 1,2,3-triazole derivatives in high yield in a regiospecific manner.This transformation has great functional group tolerance and can suit a broad substrate scope.Furthermore,the application of this novel methodology in the gram-scale synthesis of an antibiotic drug PH-027 and in the late-stage derivatization of several bioactive small molecules and clinical drugs demonstrated its generality,practicability and applicability.展开更多
A method of C(sp^3)-H bond functionalization of methyl azaarenes catalyzed by alumina-supported heteropoly acid and addition to isatins was developed. This transformation could be used for the synthesis of biologica...A method of C(sp^3)-H bond functionalization of methyl azaarenes catalyzed by alumina-supported heteropoly acid and addition to isatins was developed. This transformation could be used for the synthesis of biologically important 3-hydroxy-2-oxindole derivatives in good to excellent yields and the catalyst could be reused for six times without significant decrease in activity.展开更多
Cyclopropanedicarboxylic acid anhydride can be converted to 4-substituted 3-oxabicyclo- [3.1.0]hexan-2-one by reaction with Grignard reagents in ether or tetrahydrofuran solution.
Lithium rich layered oxide(LRLO) has been considered as one of the promising cathodes for lithium-ion batteries(LIBs). The high voltage and large capacity of LRLO depend on Li2MnO_(3)phase. To ameliorate the electroch...Lithium rich layered oxide(LRLO) has been considered as one of the promising cathodes for lithium-ion batteries(LIBs). The high voltage and large capacity of LRLO depend on Li2MnO_(3)phase. To ameliorate the electrochemical performance of Li2MnO_(3), also written as Li(Li1/3Mn2/3)O_(2), we propose a strategy to substitute Mn4+and Li+in Mn/Li transition metal layer with Ti4+, which can stabilize the structure of Li2MnO_(3)by inhibiting the excessive oxidation of O_(2)-above 4.5 V. More significantly, the unequal-valent substitution brings about the emergence of interlayer Li vacancies, which can promote the Li-ion diffusion based on the enlarged interlayer and increase the capacity by activating the Mn3+/4+redox. We designed Li0.7[Li1/3Mn2/3]0.7Ti0.3O_(2)with high interlayer Li vacancies, which presents a high capacity(290 m Ah/g at 10 m A/g) and stable cycling performance(84% over 60 cycles at 50 m A/g). We predict that this strategy will be helpful to further improve the electrochemical performance of LRLOs.展开更多
We have developed simple,cost effective and environmentally benign protocol for the synthesis of 5-substituted 1H-tetrazoles via[2,3]cycloaddition reaction from organic nitriles and sodium azide in glycerol under cata...We have developed simple,cost effective and environmentally benign protocol for the synthesis of 5-substituted 1H-tetrazoles via[2,3]cycloaddition reaction from organic nitriles and sodium azide in glycerol under catalyst free condition.The corresponding 5-substituted 1H-tetrazoles were obtained with good to excellent yields(68-95%).展开更多
Using factor analysis (principle component) and multiple linear regression methods,4 solute-related structure parameters were selected from 10 structure parameters and the relationships between the retention propertie...Using factor analysis (principle component) and multiple linear regression methods,4 solute-related structure parameters were selected from 10 structure parameters and the relationships between the retention properties (logk’) of 25 2-cyano-3-methylthio-3-substituted amino-acrylates and the 4 parameters were established.There is a good agreement between the observed k’ values and the predicted fe’ values.展开更多
基金Supported by the National Natural Science Foundation of China(Nos.20772088,21172163)the Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions,China(No.JSSYSXK2010007)
文摘Ga(ClO4)3-catalyzed reaction of 1,2-aryldiamines and α-bromoketones to afford 2-substituted quinoxalines in good yields is described.The reaction proceeded via grinding process with 10%(molar fraction) catalyst under solvent-free conditions at room temperature.For unsymmetrical o-phenylenediamines bearing electron-withdrawing groups,regio-selective quinoxalines were obtained.
基金fnancial support from the Research Council of the University of Sistan and Baluchestan
文摘A facile one-pot synthesis of 3,4,5-substituted furan-2(5H)-one derivatives from a three-component reaction of aniline derivatives, dialkylacetylenedicarboxylates and aromatic aldehydes under mild conditions using tetra-n-butylammonium bisulfate as a catalyst has been developed.
基金We thank the Beijing Municipal Commission of Education(No.JC015001200902)the Beijing Municipal Natural Science Foundation(Nos.710201,2122008)+1 种基金the Basic Research Foundation of Beijing University of Technology(No.X4015001201101)the Funding Project for Academic Human Resources Development in Institutions of Higher Learning under the Jurisdiction of Beijing Municipality(No.PHR201008025)and the Doctoral Scientific Research Start-up Foundation of Beijing University of Technology(No.52015001200701)for financial supports.
文摘In this work,six novel axially unfixed biaryl-based water-compatible bifunctional organocatalysts were de-signed and synthesized for the organocatalytic access to a variety of 3-alkyl-3-hydroxy-2-oxindole derivatives via aldol reactions in water.Organocatalyzed by 5a,the direct aldol reactions of isatins with enolisable ketones under-went readily in water,furnishing the structurally diverse 3-alkyl-3-hydroxy-2-oxindoles in various stereoselectivi-ties(up to>99%dr and>99%ee).Moreover,a plausible transition state of the conducted aldol reactions was hy-pothesized to shed light on the observed stereoselectivities of the obtained 3-alkyl-3-hydroxy-2-oxindoles.
基金supported by the National Natural Science Foundation of China(NSFC,Nos.21871043,21961130376)Department of Science and Technology of Jilin Province(Nos.20180101185JC,20190701012GH,20200801065GH)the Fundamental Research Funds for the Central Universities(Nos.2412019ZD001,2412020ZD003)。
文摘1-Substituted 1,2,3-triazoles represents‘privileged’structural scaffolds of many clinical pharmaceuticals.However,the traditional methods for their preparation mainly rely on thermal[3+2]cycloaddition of potentially dangerous acetylene and azides.Here we report a base-mediated[4+1]annulation of azoalkenes generated in situ from readily available difluoroacetaldehyde N-tosylhydrazones(DFHZ-Ts)with amines under relatively mild conditions.This azide-and acetylene-free strategy provides facile access to diverse 1-substituted 1,2,3-triazole derivatives in high yield in a regiospecific manner.This transformation has great functional group tolerance and can suit a broad substrate scope.Furthermore,the application of this novel methodology in the gram-scale synthesis of an antibiotic drug PH-027 and in the late-stage derivatization of several bioactive small molecules and clinical drugs demonstrated its generality,practicability and applicability.
基金Financial support from the National Natural Science Foundation of China(No.21402103)the research fund of Qingdao Agricultural University's High-level Person(No.631303)the Scientific Research Foundation of Shandong Province Outstanding Young Scientist Award(No.BS2013YY024) were gratefully acknowledged
文摘A method of C(sp^3)-H bond functionalization of methyl azaarenes catalyzed by alumina-supported heteropoly acid and addition to isatins was developed. This transformation could be used for the synthesis of biologically important 3-hydroxy-2-oxindole derivatives in good to excellent yields and the catalyst could be reused for six times without significant decrease in activity.
基金the National Natural Science Foundation of China.
文摘Cyclopropanedicarboxylic acid anhydride can be converted to 4-substituted 3-oxabicyclo- [3.1.0]hexan-2-one by reaction with Grignard reagents in ether or tetrahydrofuran solution.
基金financially supported by the National Natural Science Foundation of China (Nos. 51972258 and 22109186)Open Fund by Sanya Science and Education Innovation Park of Wuhan University of Technology (No. 2021KF0021)supported by 21C Innovation Laboratory,Contemporary Amperex Technology Ltd. by Project No. 21C-OP-202002。
文摘Lithium rich layered oxide(LRLO) has been considered as one of the promising cathodes for lithium-ion batteries(LIBs). The high voltage and large capacity of LRLO depend on Li2MnO_(3)phase. To ameliorate the electrochemical performance of Li2MnO_(3), also written as Li(Li1/3Mn2/3)O_(2), we propose a strategy to substitute Mn4+and Li+in Mn/Li transition metal layer with Ti4+, which can stabilize the structure of Li2MnO_(3)by inhibiting the excessive oxidation of O_(2)-above 4.5 V. More significantly, the unequal-valent substitution brings about the emergence of interlayer Li vacancies, which can promote the Li-ion diffusion based on the enlarged interlayer and increase the capacity by activating the Mn3+/4+redox. We designed Li0.7[Li1/3Mn2/3]0.7Ti0.3O_(2)with high interlayer Li vacancies, which presents a high capacity(290 m Ah/g at 10 m A/g) and stable cycling performance(84% over 60 cycles at 50 m A/g). We predict that this strategy will be helpful to further improve the electrochemical performance of LRLOs.
基金support from Department of Atomic Energy-Board of Research in Nuclear Sciences(DAE-BRNS)(No2009/37/39/BRNS/2268)
文摘We have developed simple,cost effective and environmentally benign protocol for the synthesis of 5-substituted 1H-tetrazoles via[2,3]cycloaddition reaction from organic nitriles and sodium azide in glycerol under catalyst free condition.The corresponding 5-substituted 1H-tetrazoles were obtained with good to excellent yields(68-95%).
文摘Using factor analysis (principle component) and multiple linear regression methods,4 solute-related structure parameters were selected from 10 structure parameters and the relationships between the retention properties (logk’) of 25 2-cyano-3-methylthio-3-substituted amino-acrylates and the 4 parameters were established.There is a good agreement between the observed k’ values and the predicted fe’ values.