We present some convergence and boundedness theorems with respect to filter convergence for lattice group-valued measures. We give a direct proof, based on the sliding hump argument. Furthermore we pose some open prob...We present some convergence and boundedness theorems with respect to filter convergence for lattice group-valued measures. We give a direct proof, based on the sliding hump argument. Furthermore we pose some open problems.展开更多
Let {Si}li=l be an iterated function system (IFS) on Rd with an attractor K. Let (S,cr) denote the one-sided full shift over the finite alphabet {1,2,...,l}, and let π:∑ -K be the coding map. Given an asymptot...Let {Si}li=l be an iterated function system (IFS) on Rd with an attractor K. Let (S,cr) denote the one-sided full shift over the finite alphabet {1,2,...,l}, and let π:∑ -K be the coding map. Given an asymptotically (sub)-additive sequence of continuous functions{Si}n≥1, we define the asymptotically additive projection pressure Pπ and show the variational principle for Pπunder certain affine IFS. We also obtain variational principle for the asymptotically sub-additive projection pressure if the IFS satisfies asymptotically weak separation condition (AWSC). Furthermore, when the IFS satisfies AWSC, we investigate the zero temperature limits of the asymptotically sub-additive projection pressure Pπ(β) with positive parameter β.展开更多
A facile catalytic enantioselective 1,2-addition of diynes to trifluoromethyl ketones was developed. By a com- bination of Me2Zn, Ti(OPr-i)4, BaF2 and quinine, the reaction of a series of terminal diynes with triflu...A facile catalytic enantioselective 1,2-addition of diynes to trifluoromethyl ketones was developed. By a com- bination of Me2Zn, Ti(OPr-i)4, BaF2 and quinine, the reaction of a series of terminal diynes with trifluoromethyl ke- tones proceeded to afford trifluoromethylated chrial tertiary alcohols with the diyne moiety in good to high yields with moderate to high enantioselectivities. Furthermore, this catalytic asymmetric diyne addition to trifluoro- methylketone was applied in the synthesis of the Efavirenz analogue.展开更多
A photoinduced reaction of potassium alkyltrifluoroborates,sulfur dioxide,and para-quinone methides under visible light irradiation at room temperature is developed,giving rise to diarylmethyl alkylsulfones in moderat...A photoinduced reaction of potassium alkyltrifluoroborates,sulfur dioxide,and para-quinone methides under visible light irradiation at room temperature is developed,giving rise to diarylmethyl alkylsulfones in moderate to good yields.This reaction works well under photocatalysis with a broad substrate scope by using DABCO·(SO_(2))_(2)as the source of sulfur dioxide.Mechanistic study shows that this transformation is initiated by alkyl radicals generated in situ from potassium alkyltrifluoroborates in the presence of photocatalyst.The subsequent insertion of sulfur dioxide and radical 1,6-addition of para-quinone methides with alkylsulfonyl radical intermediates afford the corresponding diarylmethyl alkylsulfones.展开更多
Alkenes and alkynes are typical substrates used in atom transfer radical addition(ATRA)reactions,resulting in the formation of vicinal disubstituted products.In this report,vinyldiazoacetates were first developed as t...Alkenes and alkynes are typical substrates used in atom transfer radical addition(ATRA)reactions,resulting in the formation of vicinal disubstituted products.In this report,vinyldiazoacetates were first developed as the radical acceptors in an ATRA reaction of RfI,leading to 1,3-difunctional adducts.The reaction is driven by visible light,without the need for external photocatalysts and additives.A series of control experiments and density functional theory(DFT)calculations indicate the 1,3-addition proceeds via a radical-chain process and the initial Rf radical was generated by homolytic dissociation of a radical pair complex of triplet free vinylcarbene and perfluoroalkyl iodide.After postreaction isomerization,various 1-iodo-3-perfluoroalkyl-alkenes were obtained in good yields with high Z selectivity.The synthetic utility of the ATRA 1,3-adduct was demonstrated by cross-coupling reactions and defluorination of perfluoroalkyl groups.展开更多
Although there is a growing interest in developing asymmetric 1,6-addition reactions of carbon nucleo-philes to Michael acceptors,the corresponding 1,6-addition of homoenolates remains an unsolved problem.Currently,th...Although there is a growing interest in developing asymmetric 1,6-addition reactions of carbon nucleo-philes to Michael acceptors,the corresponding 1,6-addition of homoenolates remains an unsolved problem.Currently,the N-heterocyclic carbene(NHC)-catalyzed cycloadditions of homoenolate equivalent intermediates have achieved widespread success.However,considerable limitations still exist for the linear reactions with electron-deficient alkenes,which are limited to 1,4-Michael acceptors.This report presents the first NHC-catalyzed asym-metric homoenolate addition of enals to 1,6-Michael acceptors.The strategy leads to the challenging nonspirocyclic 3,3-disubstituted oxindoles with two adjacent stereocenters,a quaternary and a trisubsti-tuted one,in good yields and high stereoselectivities with a wide variety of substrates.展开更多
Simple and readily available chiral N-(sulfinyl)allylamines have been developed as efficient novel ligands for the rhodium-catalyzed enantioselective 1,2-addition of arylboronic acids to challenging aliphatic a-keto...Simple and readily available chiral N-(sulfinyl)allylamines have been developed as efficient novel ligands for the rhodium-catalyzed enantioselective 1,2-addition of arylboronic acids to challenging aliphatic a-ketoesters. By employing the linear or branched sulfinamide-olefin ligands, interesting enantioselectivity as well as regioselectiw ity reversal in the related asymmetric additions were observed.展开更多
A series of homoallyl β', γ'-unsaturated amines were synthesized via1,2-addition of α,β-unsaturated imines with allylsamarium bromide in excellent yields under mildand neutral conditions.
Stereoselective approach for preparation ofα-difluoromethylα-propargylamines has been developed.1,2-Addition of lithium acetylides to diverse chiral difluoromethylated(S)-N-tert-butanesulfinyl ketimines by using T...Stereoselective approach for preparation ofα-difluoromethylα-propargylamines has been developed.1,2-Addition of lithium acetylides to diverse chiral difluoromethylated(S)-N-tert-butanesulfinyl ketimines by using Ti(O^iPr)_4 as catalyst and THF as solvent afforded N-tert-butanesulfinamides in good to excellent yields(51-93%) and good diastereoselectivities(dr.85:15 to 93:7).The N-tert -butanesulfinyl group can be readily cleaved under mild acidic condition(4 mol/L HCl in dioxane) to provide the correspondingα-difiuoromethylα-propargylamine in excellent yields(90-95%).展开更多
Herein,we report a highly efficient versatile synthetic route to Chiraphos derivatives through Rh/Ph-bod catalyzed asymmetric addition of aryl boronic acids to phosphinyl dienes.Various substituted phosphinyl dienes,b...Herein,we report a highly efficient versatile synthetic route to Chiraphos derivatives through Rh/Ph-bod catalyzed asymmetric addition of aryl boronic acids to phosphinyl dienes.Various substituted phosphinyl dienes,both on the parent skeleton and the phosphine atoms,were well tolerated with this method and provided chiral phosphine oxides in satisfied yield and up to 95%ee.The corresponding Chiraphos derivative displayed an advantage over Chiraphos in the representative Pd-catalyzed asymmetric 1,4-addition reaction.展开更多
The addition of methanol to C60 in the presence of acetylglycine (AG) was carried out under irradiation.The novel compound,1,4-dimethoxyl-l,4-dihydrofullerene (1),was isolated and characterized by FTIR,UV-vis,1H and 1...The addition of methanol to C60 in the presence of acetylglycine (AG) was carried out under irradiation.The novel compound,1,4-dimethoxyl-l,4-dihydrofullerene (1),was isolated and characterized by FTIR,UV-vis,1H and 13C NMR,and FDMS.展开更多
文摘We present some convergence and boundedness theorems with respect to filter convergence for lattice group-valued measures. We give a direct proof, based on the sliding hump argument. Furthermore we pose some open problems.
文摘Let {Si}li=l be an iterated function system (IFS) on Rd with an attractor K. Let (S,cr) denote the one-sided full shift over the finite alphabet {1,2,...,l}, and let π:∑ -K be the coding map. Given an asymptotically (sub)-additive sequence of continuous functions{Si}n≥1, we define the asymptotically additive projection pressure Pπ and show the variational principle for Pπunder certain affine IFS. We also obtain variational principle for the asymptotically sub-additive projection pressure if the IFS satisfies asymptotically weak separation condition (AWSC). Furthermore, when the IFS satisfies AWSC, we investigate the zero temperature limits of the asymptotically sub-additive projection pressure Pπ(β) with positive parameter β.
文摘A facile catalytic enantioselective 1,2-addition of diynes to trifluoromethyl ketones was developed. By a com- bination of Me2Zn, Ti(OPr-i)4, BaF2 and quinine, the reaction of a series of terminal diynes with trifluoromethyl ke- tones proceeded to afford trifluoromethylated chrial tertiary alcohols with the diyne moiety in good to high yields with moderate to high enantioselectivities. Furthermore, this catalytic asymmetric diyne addition to trifluoro- methylketone was applied in the synthesis of the Efavirenz analogue.
基金Financial support from the National Natural Science Foundation of China(Nos.22007017 and 21871053)the Talents'Startup Fund of Gannan Medical University(No.QD201831)+3 种基金the Education Bureau of Jiangxi Province(No.GJJ190799)the Research Fund of Gannan Medical University(No.ZD201905)the Leading Innovative and Entrepreneur Team Introduction Program of Zhejiang(No.2019R01005)the Open Research Fund of School of Chemistry and Chemical Engineering,Henan Normal University(No.2020ZD04)。
文摘A photoinduced reaction of potassium alkyltrifluoroborates,sulfur dioxide,and para-quinone methides under visible light irradiation at room temperature is developed,giving rise to diarylmethyl alkylsulfones in moderate to good yields.This reaction works well under photocatalysis with a broad substrate scope by using DABCO·(SO_(2))_(2)as the source of sulfur dioxide.Mechanistic study shows that this transformation is initiated by alkyl radicals generated in situ from potassium alkyltrifluoroborates in the presence of photocatalyst.The subsequent insertion of sulfur dioxide and radical 1,6-addition of para-quinone methides with alkylsulfonyl radical intermediates afford the corresponding diarylmethyl alkylsulfones.
基金the National Basic Research Program of China(no.2016YFA0602900)the National Natural Science Foundation of China(nos.21871300,21673301,and 21973113)the NSF of Guangdong Province for Distinguished Young Scholar(nos.2016A030306029 and 20153100042090537).
文摘Alkenes and alkynes are typical substrates used in atom transfer radical addition(ATRA)reactions,resulting in the formation of vicinal disubstituted products.In this report,vinyldiazoacetates were first developed as the radical acceptors in an ATRA reaction of RfI,leading to 1,3-difunctional adducts.The reaction is driven by visible light,without the need for external photocatalysts and additives.A series of control experiments and density functional theory(DFT)calculations indicate the 1,3-addition proceeds via a radical-chain process and the initial Rf radical was generated by homolytic dissociation of a radical pair complex of triplet free vinylcarbene and perfluoroalkyl iodide.After postreaction isomerization,various 1-iodo-3-perfluoroalkyl-alkenes were obtained in good yields with high Z selectivity.The synthetic utility of the ATRA 1,3-adduct was demonstrated by cross-coupling reactions and defluorination of perfluoroalkyl groups.
文摘Although there is a growing interest in developing asymmetric 1,6-addition reactions of carbon nucleo-philes to Michael acceptors,the corresponding 1,6-addition of homoenolates remains an unsolved problem.Currently,the N-heterocyclic carbene(NHC)-catalyzed cycloadditions of homoenolate equivalent intermediates have achieved widespread success.However,considerable limitations still exist for the linear reactions with electron-deficient alkenes,which are limited to 1,4-Michael acceptors.This report presents the first NHC-catalyzed asym-metric homoenolate addition of enals to 1,6-Michael acceptors.The strategy leads to the challenging nonspirocyclic 3,3-disubstituted oxindoles with two adjacent stereocenters,a quaternary and a trisubsti-tuted one,in good yields and high stereoselectivities with a wide variety of substrates.
基金Financial support from the National Natural Science Foundation of China
文摘Simple and readily available chiral N-(sulfinyl)allylamines have been developed as efficient novel ligands for the rhodium-catalyzed enantioselective 1,2-addition of arylboronic acids to challenging aliphatic a-ketoesters. By employing the linear or branched sulfinamide-olefin ligands, interesting enantioselectivity as well as regioselectiw ity reversal in the related asymmetric additions were observed.
基金theNationalNaturalScienceFoundationofChina (No .2 0 0 72 0 33)andNaturalScienceFoundationofZhejiangProvince ,China
文摘A series of homoallyl β', γ'-unsaturated amines were synthesized via1,2-addition of α,β-unsaturated imines with allylsamarium bromide in excellent yields under mildand neutral conditions.
基金The Shanghai Pujiang Program(No09PJ1400800)the Fundamental Research Funds for the Central Universities and the Scientific Research Foundation for the Returned Overseas Chinese Scholars,State Education Ministry
文摘Stereoselective approach for preparation ofα-difluoromethylα-propargylamines has been developed.1,2-Addition of lithium acetylides to diverse chiral difluoromethylated(S)-N-tert-butanesulfinyl ketimines by using Ti(O^iPr)_4 as catalyst and THF as solvent afforded N-tert-butanesulfinamides in good to excellent yields(51-93%) and good diastereoselectivities(dr.85:15 to 93:7).The N-tert -butanesulfinyl group can be readily cleaved under mild acidic condition(4 mol/L HCl in dioxane) to provide the correspondingα-difiuoromethylα-propargylamine in excellent yields(90-95%).
基金support from the National Natural Science Foundation of China (Nos. 21901235 and 22071224)the USTC Research Funds of the Double First-Class Initiative (No. YD20600002010)+1 种基金the Anhui Provincial Natural Science-Foundation (No. 1908085MB34)the Science, Technology and Innovation Commission of Shenzhen (No. JCYJ20190807155201669)
文摘Herein,we report a highly efficient versatile synthetic route to Chiraphos derivatives through Rh/Ph-bod catalyzed asymmetric addition of aryl boronic acids to phosphinyl dienes.Various substituted phosphinyl dienes,both on the parent skeleton and the phosphine atoms,were well tolerated with this method and provided chiral phosphine oxides in satisfied yield and up to 95%ee.The corresponding Chiraphos derivative displayed an advantage over Chiraphos in the representative Pd-catalyzed asymmetric 1,4-addition reaction.
基金Project (No. 29571004) supported by the National Natural Science Foundation of China
文摘The addition of methanol to C60 in the presence of acetylglycine (AG) was carried out under irradiation.The novel compound,1,4-dimethoxyl-l,4-dihydrofullerene (1),was isolated and characterized by FTIR,UV-vis,1H and 13C NMR,and FDMS.