Fluoroacetate dehalogenases(FAcD),a homodimeric enzyme,catalyzes the conversion of fluoroacetic acid to glycolic acid(GoA).It has been proved that the enzyme has a half-of-the-site reactivity.Namely,its catalytic(C)su...Fluoroacetate dehalogenases(FAcD),a homodimeric enzyme,catalyzes the conversion of fluoroacetic acid to glycolic acid(GoA).It has been proved that the enzyme has a half-of-the-site reactivity.Namely,its catalytic(C)subunit converts the first substrate to a covalent intermediate;then,the non-catalytic(NC)subunit binds a second substrate and promotes the conversion of the intermediate in the C subunit into the final product.After the release of the product,the C subunit becomes the NC subunit,and the previous NC subunit becomes the C subunit.To elucidate the detailed mechanism behind this cooperative catalysis,we have conducted microsecond-scale MD simulations along the reaction pathway.The simulations indicate that the substrate in the NC subunit induces W185 and Y141 adopting an open conformation in the C subunit.The opening of W185(C)facilitates the entry of catalytic water,enhancing the catalytic activity for product formation,while the opening of Y141(C)creates an unfavorable environment for product binding,promoting its release.An interaction network analysis reveals that the substrate in the NC subunit can induce conformational changes through a conserved water chain at the interface.展开更多
IM-5 zeolite was synthesized by hydrothermal crystallization method with 1,5-bis(N-methylpyrrolidinium)pentane bromide using the precursors N-methylpyrrolidine and 1,5-dibromopentane as raw materials of template after...IM-5 zeolite was synthesized by hydrothermal crystallization method with 1,5-bis(N-methylpyrrolidinium)pentane bromide using the precursors N-methylpyrrolidine and 1,5-dibromopentane as raw materials of template after pre-reaction,and then aluminum,alkali,water and silicon sources were added into the reaction system.The effects of the proportion of precursors and other materials and the reaction conditions on the crystallinity,crystal morphology and pore structure of the synthesized zeolites were systematically investigated,which provided the basic data for industrial production.The physical properties of the synthesized samples were analyzed by XRD,SEM,and N2 adsorptiondesorption techniques,and the catalytic performance of the samples was evaluated.The results show that IM-5 zeolite can be synthesized effectively by using the template pre-reaction method,and its physical properties and catalytic activity in catalytic alkylation of benzene and methanol are comparable to those of industrial samples synthesized by traditional method.展开更多
基金National Natural Science Foundation of China(51102184,51172163)National High Technology Research and Development Program of China(2013AA031801)+2 种基金National Key Technology Research and Development Program of China(2013BAJ01B01)Shanghai Municipal Science and Technology Commission Nano Special Project,China(12nm0503001,11nm0501600)Science and Technology Innovation Fund of Shanghai Aerospace,China(SAST201254,SAST201321)
基金supported by the Key-Area Research and Development Program of Guangdong Province(2020B0101350001)the Shenzhen Fundamental Research Program(GXWD2020123116580700720200812124825001)+1 种基金the Shenzhen Science and Technology Program(RCBS20210706092258097)supported by the Shenzhen Bay Laboratory Supercomputing Center。
文摘Fluoroacetate dehalogenases(FAcD),a homodimeric enzyme,catalyzes the conversion of fluoroacetic acid to glycolic acid(GoA).It has been proved that the enzyme has a half-of-the-site reactivity.Namely,its catalytic(C)subunit converts the first substrate to a covalent intermediate;then,the non-catalytic(NC)subunit binds a second substrate and promotes the conversion of the intermediate in the C subunit into the final product.After the release of the product,the C subunit becomes the NC subunit,and the previous NC subunit becomes the C subunit.To elucidate the detailed mechanism behind this cooperative catalysis,we have conducted microsecond-scale MD simulations along the reaction pathway.The simulations indicate that the substrate in the NC subunit induces W185 and Y141 adopting an open conformation in the C subunit.The opening of W185(C)facilitates the entry of catalytic water,enhancing the catalytic activity for product formation,while the opening of Y141(C)creates an unfavorable environment for product binding,promoting its release.An interaction network analysis reveals that the substrate in the NC subunit can induce conformational changes through a conserved water chain at the interface.
文摘IM-5 zeolite was synthesized by hydrothermal crystallization method with 1,5-bis(N-methylpyrrolidinium)pentane bromide using the precursors N-methylpyrrolidine and 1,5-dibromopentane as raw materials of template after pre-reaction,and then aluminum,alkali,water and silicon sources were added into the reaction system.The effects of the proportion of precursors and other materials and the reaction conditions on the crystallinity,crystal morphology and pore structure of the synthesized zeolites were systematically investigated,which provided the basic data for industrial production.The physical properties of the synthesized samples were analyzed by XRD,SEM,and N2 adsorptiondesorption techniques,and the catalytic performance of the samples was evaluated.The results show that IM-5 zeolite can be synthesized effectively by using the template pre-reaction method,and its physical properties and catalytic activity in catalytic alkylation of benzene and methanol are comparable to those of industrial samples synthesized by traditional method.
