We herein reported a sustainable synthesis of 3,3-disubstituted oxindoles via a Michael-type reaction based on the CuBr-catalysed capture of carboxylic oxonium ylides with isatylidene malononitrile.The reaction is cha...We herein reported a sustainable synthesis of 3,3-disubstituted oxindoles via a Michael-type reaction based on the CuBr-catalysed capture of carboxylic oxonium ylides with isatylidene malononitrile.The reaction is characterized by a high atom economy and low economic constraints.The catalyst CuBr could be conveniently recyclized.The products of the reaction were found to be inhibitory against Na ion channels.We expect the reaction to shed the light on synthesis of biologically interesting molecules directed by principles of green chemistry.展开更多
Core-shell structured ZSM-5@Silicalite-1 zeolite could effectively hinder the deactivation of catalyst surface. Currently, organic structure directing agents(OSDAs) are necessary in the conventional route for the synt...Core-shell structured ZSM-5@Silicalite-1 zeolite could effectively hinder the deactivation of catalyst surface. Currently, organic structure directing agents(OSDAs) are necessary in the conventional route for the synthesis of this core-shell zeolite under hydrothermal conditions, which is costly and environmental-unfriendly. In this research, a synthesis of the core-shell structured ZSM-5@Silicalite-1 zeolite with a strategy of alcohol filling and zeolite seeding without any organic template or solvent is exhibited. The obtained products are well characterized by X-ray powder diffractometer(XRD), scanning electron microscopy(SEM), transmission electron microscopy(TEM), N2 sorption isotherms, solid magic angle spinning(MAS) NMR, temperature-programmed-desorption of ammonia(NH3-TPD), and X-ray photoelectron spectroscopy(XPS) techniques, in order to confirm the core-shell structure. More importantly, the core-shell structured ZSM-5@Silicalite-1 zeolite exhibits a long lifetime and a high p-xylene selectivity in the alkylation of toluene with methanol, compared with the conventional ZSM-5 catalyst.展开更多
In conventional heterogeneous catalytic process, the activation of C-H bond remains a grand challenge. It is even more difficult to activate the inert C-H bond with other functional groups (e.g. OH) in the same mole...In conventional heterogeneous catalytic process, the activation of C-H bond remains a grand challenge. It is even more difficult to activate the inert C-H bond with other functional groups (e.g. OH) in the same molecule, remaining intact [1]. Although the transformation of C1 species (e.g. CO, CO2, CH4 and CH3OH) into C2 molecules (e.g. C2H4, C2HsOH and HOCH2CH2OH) via C-C coupling has been a hot research topic but the yield of aimed product is still needed to be improved. Ethylene glycol (EG) is a versatile chemical with many important applications, in particular for the manufacture of polyesters, predominantly poly(ethylene terephthalate) [2]. Recently, Wang, Deng and co-workers at Xiamen University cleverly designed a new process for the conversion of methanol to ethylene glycol, in which the EG selectivity can reach 90% (Eq. (1)) [3].展开更多
Polymers from renewable resources are receiving tremendous attention due to the increasing concerns on the depletion of fossil oils and deteriorated environments.Cardanol,as an abundant and renewable chemical raw mate...Polymers from renewable resources are receiving tremendous attention due to the increasing concerns on the depletion of fossil oils and deteriorated environments.Cardanol,as an abundant and renewable chemical raw material,has been widely used for the production of renewable polymer materials via converting into various of chemical monomers with active functional groups.This comprehensive review deals with various aspects of cardanol as a starting material the preparing various polymer and polymer composites such as benzoxazine resins,phenolic resin,polyurethanes,epoxy resin,vinyl ester polymers,polyamide and cyanate ester resins.The assessment of the future prospects for the use of cardanol to synthesise novel and valuable renewable materials is presented.展开更多
This paper reviewed the recent research progress of organic reactions catalyzed by four typical earthabundant and 3d metal catalysts:Mn,Fe,Co,and Ni complexes and mainly focused on the reactions in which these 3d meta...This paper reviewed the recent research progress of organic reactions catalyzed by four typical earthabundant and 3d metal catalysts:Mn,Fe,Co,and Ni complexes and mainly focused on the reactions in which these 3d metal catalysts exhibited obvious advantages over other catalysts.The mechanism that makes these 3d metal catalysts show unusual properties is another focus of this paper.An outlook on 3d metal complexes-catalyzed organic reactions was also considered.展开更多
Light-emitting electrochemical cells(LECs)can be fabricated with cost-efficient printing and coating methods,but a current drawback is that the LEC emitter is commonly either a rare-metal complex or an expensive-to-sy...Light-emitting electrochemical cells(LECs)can be fabricated with cost-efficient printing and coating methods,but a current drawback is that the LEC emitter is commonly either a rare-metal complex or an expensive-to-synthesize conjugated polymer.Here,we address this issue through the pioneering employment of metal-free and facile-to-synthesize carbon nanodots(CNDs)as the emitter in functional LEC devices.Circular-shaped(average diameter=4.4 nm)and hydrophilic CNDs,which exhibit narrow cyan photoluminescence(peak=485 nm,full width at half maximum=30 nm)with a high quantum yield of 77%in dilute ethanol solution,were synthesized with a catalyst-free,one-step solvothermal process using low-cost and benign phloroglucinol as the sole starting material.The propensity of the planar CNDs to form emission-quenching aggregates in the solid state was inhibited by the inclusion of a compatible 2,7-bis(diphenylphosphoryl)-9,9’-spirobifluorene host compound,and we demonstrate that such pristine host-guest CND-LECs turn on to a peak luminance of 118 cd·m^(−2)within 5 s during constant current-density driving at 77 mA·cm^(−2).展开更多
基金the National Natural Science Foundation of China(Nos.82003592(TS),92056201(WH)and 82201376(SC))Key-Area Research and Development Program of Guangdong Province(No.2022B1111050003)(WH)+1 种基金Shenzhen Science and Technology Innovation Project(No.20200812143116001)(SC)Basic Research Foundation of Guangdong province(No.2021A1515011129)(SC).
文摘We herein reported a sustainable synthesis of 3,3-disubstituted oxindoles via a Michael-type reaction based on the CuBr-catalysed capture of carboxylic oxonium ylides with isatylidene malononitrile.The reaction is characterized by a high atom economy and low economic constraints.The catalyst CuBr could be conveniently recyclized.The products of the reaction were found to be inhibitory against Na ion channels.We expect the reaction to shed the light on synthesis of biologically interesting molecules directed by principles of green chemistry.
基金This work was supported by the National Key Research and Development Program of China(No.2017YFB0702803)the Fundamental Research Funds for the Central Universities,China(No.2021QNA4028)the National Natural Science Foundation of China(Nos.21802121,2217020097,21720102001).
文摘Core-shell structured ZSM-5@Silicalite-1 zeolite could effectively hinder the deactivation of catalyst surface. Currently, organic structure directing agents(OSDAs) are necessary in the conventional route for the synthesis of this core-shell zeolite under hydrothermal conditions, which is costly and environmental-unfriendly. In this research, a synthesis of the core-shell structured ZSM-5@Silicalite-1 zeolite with a strategy of alcohol filling and zeolite seeding without any organic template or solvent is exhibited. The obtained products are well characterized by X-ray powder diffractometer(XRD), scanning electron microscopy(SEM), transmission electron microscopy(TEM), N2 sorption isotherms, solid magic angle spinning(MAS) NMR, temperature-programmed-desorption of ammonia(NH3-TPD), and X-ray photoelectron spectroscopy(XPS) techniques, in order to confirm the core-shell structure. More importantly, the core-shell structured ZSM-5@Silicalite-1 zeolite exhibits a long lifetime and a high p-xylene selectivity in the alkylation of toluene with methanol, compared with the conventional ZSM-5 catalyst.
文摘In conventional heterogeneous catalytic process, the activation of C-H bond remains a grand challenge. It is even more difficult to activate the inert C-H bond with other functional groups (e.g. OH) in the same molecule, remaining intact [1]. Although the transformation of C1 species (e.g. CO, CO2, CH4 and CH3OH) into C2 molecules (e.g. C2H4, C2HsOH and HOCH2CH2OH) via C-C coupling has been a hot research topic but the yield of aimed product is still needed to be improved. Ethylene glycol (EG) is a versatile chemical with many important applications, in particular for the manufacture of polyesters, predominantly poly(ethylene terephthalate) [2]. Recently, Wang, Deng and co-workers at Xiamen University cleverly designed a new process for the conversion of methanol to ethylene glycol, in which the EG selectivity can reach 90% (Eq. (1)) [3].
基金supported by the Open Fund Project of Jiangsu Key Laboratory of Biomass Energy and Materials(Grants No.JSBEM201907)the National Natural Science Foundation of China(No.31570563)the fund project of Yele Science and Technology Innovation(Grants No.YL201807).
文摘Polymers from renewable resources are receiving tremendous attention due to the increasing concerns on the depletion of fossil oils and deteriorated environments.Cardanol,as an abundant and renewable chemical raw material,has been widely used for the production of renewable polymer materials via converting into various of chemical monomers with active functional groups.This comprehensive review deals with various aspects of cardanol as a starting material the preparing various polymer and polymer composites such as benzoxazine resins,phenolic resin,polyurethanes,epoxy resin,vinyl ester polymers,polyamide and cyanate ester resins.The assessment of the future prospects for the use of cardanol to synthesise novel and valuable renewable materials is presented.
基金the National Key R&D Program of China(grant no.2021YFA1500200)the National Natural Science Foundation of China(grant nos.92256301,22221002,22025109,21831008,22101286,and 22271249)the Fundamental Research Funds for the Central Universities(grant nos.226-2022-00224 and 226-2023-00115)for financial support.
文摘This paper reviewed the recent research progress of organic reactions catalyzed by four typical earthabundant and 3d metal catalysts:Mn,Fe,Co,and Ni complexes and mainly focused on the reactions in which these 3d metal catalysts exhibited obvious advantages over other catalysts.The mechanism that makes these 3d metal catalysts show unusual properties is another focus of this paper.An outlook on 3d metal complexes-catalyzed organic reactions was also considered.
基金support from J.C.Kempes Minnes Stipendiefond(No.SMK-1849.1)the Swedish Energy Agency(Nos.45419-1,46523-1,and 50779-1)+2 种基金the Swedish Research Council(Nos.2017-04380,2017-04862,2018-03937,and 2019-02345)the Swedish Foundation for Strategic Research,Stiftelsen Olle Engkvist Byggmästare(Nos.186-0637 and 193-0578)Bertil&Britt Svenssons stiftelse för belysningsteknik,the Swedish Foundation for International Cooperation in Research and Higher Education via an Initiation Grant for Internationalization(No.2019-8553)。
文摘Light-emitting electrochemical cells(LECs)can be fabricated with cost-efficient printing and coating methods,but a current drawback is that the LEC emitter is commonly either a rare-metal complex or an expensive-to-synthesize conjugated polymer.Here,we address this issue through the pioneering employment of metal-free and facile-to-synthesize carbon nanodots(CNDs)as the emitter in functional LEC devices.Circular-shaped(average diameter=4.4 nm)and hydrophilic CNDs,which exhibit narrow cyan photoluminescence(peak=485 nm,full width at half maximum=30 nm)with a high quantum yield of 77%in dilute ethanol solution,were synthesized with a catalyst-free,one-step solvothermal process using low-cost and benign phloroglucinol as the sole starting material.The propensity of the planar CNDs to form emission-quenching aggregates in the solid state was inhibited by the inclusion of a compatible 2,7-bis(diphenylphosphoryl)-9,9’-spirobifluorene host compound,and we demonstrate that such pristine host-guest CND-LECs turn on to a peak luminance of 118 cd·m^(−2)within 5 s during constant current-density driving at 77 mA·cm^(−2).