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Franco M Rabagliati - One of the best experts on this subject based on the ideXlab platform.

  • Styrene/substituted styrene copolymerization by Ph2Zn-metallocene-MAO systems : homo-and copolymerization of p-methoxystyrene with styrene
    Polymer International, 2020
    Co-Authors: Franco M Rabagliati, Héctor E. Muñoz, Gabriela V. Mardones, Francisco J. Rodríguez
    Abstract:

    BACKGROUND: The present work is part of a general study regarding the homo- and copolymerization of styrene using Diphenylzinc–additive initiator systems, with the aim of improving the properties of commercial atactic polystyrene. The study is focused on syndiotactic polystyrene and/or copolymers of styrene (S) with substituted styrene, styrene derivatives or various α-olefins. This research has been ongoing over the last 15 years. RESULTS: The reported experiments show that binary metallocene–methylaluminoxane (MAO) and ternary Ph2Zn–metallocene–MAO, depending on the metallocene employed, are capable of inducing both homo- and copolymerization of styrene and p-methoxystyrene (p-MeOS). The results indicate that for a styrene/p-MeOS mole ratio with p-MeOS > 25% the product obtained has only a minor incorporation of styrene units. The efficiency of the metallocenes studied follows the order bis(n-butylcyclopentadienyl)titanium dichloride ((n-BuCp)2TiCl2) > indenyltitanium trichloride (IndTiCl3) > Cp2TiCl2. CONCLUSION: Metallocenes (n-BuCp)2TiCl2, Cp2TiCl2 and IndTiCl3 in binary systems combined with MAO, as well as in ternary systems combined with Ph2Zn and MAO, induce the homopolymerization of p-MeOS and its copolymerization with styrene. The styrene/p-MeOS copolymer obtained was enriched in p-MeOS with respect to the initial feed, in agreement with the I+ inductive effect of the methoxy group in the para position of styrene. As already reported, the role of Ph2Zn was nullified by its complexation with the p-MeOS comonomer. Copyright © 2008 Society of Chemical Industry

  • STYRENE/STYRENE-DERIVATIVE COPOLYMERIZATION BY PH2Zn-METALLOCENE-MAO SYSTEMS: HOMO- AND COPOLYMERIZATION OF á-METHYLSTYRENE WITH STYRENE
    Journal of The Chilean Chemical Society, 2020
    Co-Authors: Franco M Rabagliati, Héctor E. Muñoz, Gabriela V. Mardones
    Abstract:

    The copolymerization of styrene with α-methylstyrene has been tested using combined metallocene-MAO initiator systems with and without Diphenylzinc. The metallocenes used were biscyclopentadienyltitanium dichloride, Cp 2 TiCl 2 , bis(n-butylcyclopentadienyl)titanium dichloride, (n-BuCp) 2 TiCl 2 , and the halfsandwich metallocene indenyltitanium trichloride, IndTiCl 3 . The results indicate that both binary metallocene-MAO, and ternary Ph 2 Zn-metallocene-MAO systems are capable of polymerizing α-methylstyrene to poly(α-methylstyrene) as well of its copolymerization with styrene. These initiator systems also show that despite the I+ inductive effect of the methyl group, which enhances electron density at the vinyl double bond of styrene, the steric consequence of vinyl substitution hinders monomer coordination to active species, causing a decrease in conversion of either α-MeS to homopolymer or S/α-MeS to the corresponding copolymer. The nature and structure of the metallocene included in the initiator system are determinant of the initiator system’s efficiency. For the metallocenes used the efficiency follows the order IndTiCl 3 > Cp 2 TiCl 2 > (n-BuCp) 2 TiCl 2 , with the half-sandwich metallocene IndTiCl 3 showing greater efficiency than the true metallocenes.

  • Styrene–substituted-styrene copolymerization using Diphenylzinc–metallocene–methylaluminoxane systems
    Polymer International, 2020
    Co-Authors: Franco M Rabagliati, Francisco J. Rodríguez, Abdel Alla, Sebastián Muñoz-guerra
    Abstract:

    Homopolymerization of disubstituted styrenes (2,4- and 2,5-dimethylstyrene) and trisubstituted styrene (2,4,6-trimethylstyrene) and their copolymerization with styrene were carried out using Diphenylzinc–metallocene–methylaluminoxane initiator systems for metallocene (n-BuCp)2TiCl2 and for half-metallocene CpTiCl3. The studied comonomers were found to be less reactive than p-tertbutylstyrene, p-methylstyrene and styrene. The results indicate that, even though the methyl group has I+ inductive effect, di- and tri-methylstyrenes are reluctant to undergo either homopolymerization or copolymerization. This behavior suggests that the reactivity is regulated not only by the inductive effect of the alkyl group but also by the steric impediment caused by the crowding of the substituents on the benzene ring. Copyright © 2006 Society of Chemical Industry

  • HOMO- AND COPOLYMERIZATION OF STYRENE AND STYRENE RELATED MONOMERS. SYNTHESIS AND CHARACTERIZATION
    Journal of The Chilean Chemical Society, 2016
    Co-Authors: Franco M Rabagliati, Rodrigo A. Cancino, Francisco J. Rodríguez, Monica A Perez, Héctor E. Muñoz, Maria V. Cuevas, G. A. Mardones, Marcela Saavedra, M. Vidal, Lisa Muñoz
    Abstract:

    Systems including Diphenylzinc, metallocene, and methylaluminoxane, at various combinations has been attempted, as initiating systems for homo- and copolymerization of styrene and various styrene related comonomers including : substituted styrenes, styrene derivatives, α-olefins, dienes and more recently cycohexenes including norbornene. The used metallocenes were those containing titanium, zirconium and for comparatives reasons hafnium. The metallocene efficiency towards syndiotactic polystyrene polymerization showed the order : titanocene > zirconocene > hafnocene. While the polymerization as well the copolymerization of Styrene with related to styrene compounds resulted to be much influenced by both electrical and steric hindrance effect. For styrene substituted derivative those group or element having I+ inductive effect depending its position at styrene’s its phenyl ring favours homopolymerization as well their copolymerization with styrene. The steric hindrance also showed a determinant influence on reactivity, so methyl and tert-butyl group, having a I+ effect, when at para -position improve activity and stereoregularity of their polymerization processes. But when placing at orto- position showed a very low capacity to polymerize. The present and previous results indicate that polymerization processes are initiated by monomer coordination to active metal species either of the binary metallocene-MAO or of the ternary Ph2Zn-metallocene-MAO.

  • styrene substituted styrene copolymerization using Diphenylzinc metallocene methylaluminoxane systems
    Polymer International, 2006
    Co-Authors: Franco M Rabagliati, Francisco J. Rodríguez, Abdel Alla, Sebastian Munozguerra
    Abstract:

    Homopolymerization of disubstituted styrenes (2,4- and 2,5-dimethylstyrene) and trisubstituted styrene (2,4,6-trimethylstyrene) and their copolymerization with styrene were carried out using Diphenylzinc–metallocene–methylaluminoxane initiator systems for metallocene (n-BuCp)2TiCl2 and for half-metallocene CpTiCl3. The studied comonomers were found to be less reactive than p-tertbutylstyrene, p-methylstyrene and styrene. The results indicate that, even though the methyl group has I+ inductive effect, di- and tri-methylstyrenes are reluctant to undergo either homopolymerization or copolymerization. This behavior suggests that the reactivity is regulated not only by the inductive effect of the alkyl group but also by the steric impediment caused by the crowding of the substituents on the benzene ring. Copyright © 2006 Society of Chemical Industry

Jesus Contreras - One of the best experts on this subject based on the ideXlab platform.

  • Ring‐opening copolymerization of L‐lactide with ε‐caprolactone initiated by Diphenylzinc
    Polymer International, 2020
    Co-Authors: Jesus Contreras, Darymar Davila
    Abstract:

    Copolymerization of mixtures of L-lactide and e-caprolactone has been initiated by Diphenylzinc. The reaction conditions were investigated, to discover the effects on yield, molecular weight and microstructure of copolymers obtained. The temperature used varied between 50 and 120 °C, the molar ratio of monomer to initiator ranged between 90 and 1440 mol/mol, and the molar ratio of e-caprolactone to L-lactide employed was between 100/0 and 0/100 mol/mol. Copolymers were characterized by 1H-NMR, 13C-NMR, DSC and gel permeation chromatography. The results indicate that incorporation of L-lactide to the growing chain is preferred and e-caprolactone is copolymerized after most of the L-lactide has been depleted. The microstructure of obtained copolyesters was affected considerably by transesterification reactions. It was observed that increasing reaction temperature, reaction time and concentration initiator was advantageous to the transesterification. The crystallinity of copolyester obtained was determined by differential scanning calorimetry. The results are in good agreement with both molar composition and sequence distribution of copolyesters. Copyright © 2006 Society of Chemical Industry

  • Ring-opening polymerization of ε-caprolactone initiated by Diphenylzinc
    European Polymer Journal, 2020
    Co-Authors: M Vivas, Jesus Contreras
    Abstract:

    Abstract In the present work the polymerization of e -caprolactone ( e -CL) using Ph 2 Zn as initiator is reported. The effects of reaction temperature, molar ratio of monomer/initiator and reaction time on the yield and the molecular weight are investigated. The temperature is varied between 20 and 120 °C and the molar ratio of monomer to initiator between 200 and 800 mol/mol. The results indicate that the Ph 2 Zn induces the polymerization of e -CL to high conversion and produces polymer with high molecular weight at temperatures around 40–60 °C.

  • Synthesis of ε-caprolactone-b-l-lactide block copolymers by mean sequential polymerization, using Diphenylzinc as initiator
    Polymer Bulletin, 2014
    Co-Authors: Jesus Contreras, Francisco López-carrasquero, Jennifer Pestana, Carlos Torres
    Abstract:

    Block copolymers of ε-caprolactone (CL) and l -lactide ( l -LA) were synthesized by sequential polymerization using Diphenylzinc as initiator. The composition of the copolymers was adjusted changing the comonomers in ratio. Copolymers were characterized by ^1H-NMR, ^13C-NMR, DSC, and GPC. Results indicate that poly(ε-caprolactone)- b -poly( l -lactide) (PCL- b -PLA) block copolymers had a narrow molecular weight distribution and well-controlled sequences without random placement.

  • synthesis of e caprolactone b l lactide block copolymers by mean sequential polymerization using Diphenylzinc as initiator
    Polymer Bulletin, 2014
    Co-Authors: Jesus Contreras, Francisco Lopezcarrasquero, Jennifer Pestana, Carlos F Torres
    Abstract:

    Block copolymers of e-caprolactone (CL) and l-lactide (l-LA) were synthesized by sequential polymerization using Diphenylzinc as initiator. The composition of the copolymers was adjusted changing the comonomers in ratio. Copolymers were characterized by 1H-NMR, 13C-NMR, DSC, and GPC. Results indicate that poly(e-caprolactone)-b-poly(l-lactide) (PCL-b-PLA) block copolymers had a narrow molecular weight distribution and well-controlled sequences without random placement.

  • Synthesis of ε-caprolactone-b-l-lactide block copolymers by mean sequential polymerization, using Diphenylzinc as initiator
    Polymer Bulletin, 2014
    Co-Authors: Jesus Contreras, Francisco López-carrasquero, Jennifer Pestana, Carlos F Torres
    Abstract:

    Block copolymers of e-caprolactone (CL) and l-lactide (l-LA) were synthesized by sequential polymerization using Diphenylzinc as initiator. The composition of the copolymers was adjusted changing the comonomers in ratio. Copolymers were characterized by 1H-NMR, 13C-NMR, DSC, and GPC. Results indicate that poly(e-caprolactone)-b-poly(l-lactide) (PCL-b-PLA) block copolymers had a narrow molecular weight distribution and well-controlled sequences without random placement.

Monica A Perez - One of the best experts on this subject based on the ideXlab platform.

Francisco J. Rodríguez - One of the best experts on this subject based on the ideXlab platform.

  • Styrene–substituted-styrene copolymerization using Diphenylzinc–metallocene–methylaluminoxane systems
    Polymer International, 2020
    Co-Authors: Franco M Rabagliati, Francisco J. Rodríguez, Abdel Alla, Sebastián Muñoz-guerra
    Abstract:

    Homopolymerization of disubstituted styrenes (2,4- and 2,5-dimethylstyrene) and trisubstituted styrene (2,4,6-trimethylstyrene) and their copolymerization with styrene were carried out using Diphenylzinc–metallocene–methylaluminoxane initiator systems for metallocene (n-BuCp)2TiCl2 and for half-metallocene CpTiCl3. The studied comonomers were found to be less reactive than p-tertbutylstyrene, p-methylstyrene and styrene. The results indicate that, even though the methyl group has I+ inductive effect, di- and tri-methylstyrenes are reluctant to undergo either homopolymerization or copolymerization. This behavior suggests that the reactivity is regulated not only by the inductive effect of the alkyl group but also by the steric impediment caused by the crowding of the substituents on the benzene ring. Copyright © 2006 Society of Chemical Industry

  • Styrene/substituted styrene copolymerization by Ph2Zn-metallocene-MAO systems : homo-and copolymerization of p-methoxystyrene with styrene
    Polymer International, 2020
    Co-Authors: Franco M Rabagliati, Héctor E. Muñoz, Gabriela V. Mardones, Francisco J. Rodríguez
    Abstract:

    BACKGROUND: The present work is part of a general study regarding the homo- and copolymerization of styrene using Diphenylzinc–additive initiator systems, with the aim of improving the properties of commercial atactic polystyrene. The study is focused on syndiotactic polystyrene and/or copolymers of styrene (S) with substituted styrene, styrene derivatives or various α-olefins. This research has been ongoing over the last 15 years. RESULTS: The reported experiments show that binary metallocene–methylaluminoxane (MAO) and ternary Ph2Zn–metallocene–MAO, depending on the metallocene employed, are capable of inducing both homo- and copolymerization of styrene and p-methoxystyrene (p-MeOS). The results indicate that for a styrene/p-MeOS mole ratio with p-MeOS > 25% the product obtained has only a minor incorporation of styrene units. The efficiency of the metallocenes studied follows the order bis(n-butylcyclopentadienyl)titanium dichloride ((n-BuCp)2TiCl2) > indenyltitanium trichloride (IndTiCl3) > Cp2TiCl2. CONCLUSION: Metallocenes (n-BuCp)2TiCl2, Cp2TiCl2 and IndTiCl3 in binary systems combined with MAO, as well as in ternary systems combined with Ph2Zn and MAO, induce the homopolymerization of p-MeOS and its copolymerization with styrene. The styrene/p-MeOS copolymer obtained was enriched in p-MeOS with respect to the initial feed, in agreement with the I+ inductive effect of the methoxy group in the para position of styrene. As already reported, the role of Ph2Zn was nullified by its complexation with the p-MeOS comonomer. Copyright © 2008 Society of Chemical Industry

  • HOMO- AND COPOLYMERIZATION OF STYRENE AND STYRENE RELATED MONOMERS. SYNTHESIS AND CHARACTERIZATION
    Journal of The Chilean Chemical Society, 2016
    Co-Authors: Franco M Rabagliati, Rodrigo A. Cancino, Francisco J. Rodríguez, Monica A Perez, Héctor E. Muñoz, Maria V. Cuevas, G. A. Mardones, Marcela Saavedra, M. Vidal, Lisa Muñoz
    Abstract:

    Systems including Diphenylzinc, metallocene, and methylaluminoxane, at various combinations has been attempted, as initiating systems for homo- and copolymerization of styrene and various styrene related comonomers including : substituted styrenes, styrene derivatives, α-olefins, dienes and more recently cycohexenes including norbornene. The used metallocenes were those containing titanium, zirconium and for comparatives reasons hafnium. The metallocene efficiency towards syndiotactic polystyrene polymerization showed the order : titanocene > zirconocene > hafnocene. While the polymerization as well the copolymerization of Styrene with related to styrene compounds resulted to be much influenced by both electrical and steric hindrance effect. For styrene substituted derivative those group or element having I+ inductive effect depending its position at styrene’s its phenyl ring favours homopolymerization as well their copolymerization with styrene. The steric hindrance also showed a determinant influence on reactivity, so methyl and tert-butyl group, having a I+ effect, when at para -position improve activity and stereoregularity of their polymerization processes. But when placing at orto- position showed a very low capacity to polymerize. The present and previous results indicate that polymerization processes are initiated by monomer coordination to active metal species either of the binary metallocene-MAO or of the ternary Ph2Zn-metallocene-MAO.

  • styrene substituted styrene copolymerization using Diphenylzinc metallocene methylaluminoxane systems
    Polymer International, 2006
    Co-Authors: Franco M Rabagliati, Francisco J. Rodríguez, Abdel Alla, Sebastian Munozguerra
    Abstract:

    Homopolymerization of disubstituted styrenes (2,4- and 2,5-dimethylstyrene) and trisubstituted styrene (2,4,6-trimethylstyrene) and their copolymerization with styrene were carried out using Diphenylzinc–metallocene–methylaluminoxane initiator systems for metallocene (n-BuCp)2TiCl2 and for half-metallocene CpTiCl3. The studied comonomers were found to be less reactive than p-tertbutylstyrene, p-methylstyrene and styrene. The results indicate that, even though the methyl group has I+ inductive effect, di- and tri-methylstyrenes are reluctant to undergo either homopolymerization or copolymerization. This behavior suggests that the reactivity is regulated not only by the inductive effect of the alkyl group but also by the steric impediment caused by the crowding of the substituents on the benzene ring. Copyright © 2006 Society of Chemical Industry

  • further studies on styrene styrene derivative copolymerizations using combined Diphenylzinc additive initiator systems
    Polymer International, 2005
    Co-Authors: Franco M Rabagliati, Francisco J. Rodríguez, Monica A Perez, Carlos J Caro, Nicolas Crispel
    Abstract:

    A combination of Diphenylzinc, a metallocene and methylaluminoxane (Ph2Zn-metallocene-MAO) is a suitable initiator system for the polymerization of styrene and for its copolymerization with para-alkyl substituted styrenes. This paper reports new experimental results which reinforce our previous findings indicating that polymerization processes are initiated by monomer coordination to active species resulting from these particular combined systems. Polymerization propagates by a cationic pathway. Further to our previous observation that the I+ inductive effect of para-substituents in styrene improves conversion to polymer, we now find that methyl substitution on the vinyl double bond of styrene, in spite of the I+ inductive effect and as a result of increased steric hindrance, makes the polymerization process difficult. On the other hand, the replacement of titanocenes by zirconocenes or hafnocenes generates Ph2Zn-metallocene-MAO initiator systems which are also able to induce homo- and copolymerization, but with lower yields and producing practically amorphous polymers. The efficiency of our Ph2Zn-metallocene-MAO initiator systems follows the order titanocene > zirconocene > hafnocene, at least for the studied metallocenes. Copyright © 2004 Society of Chemical Industry

Raul Quijada - One of the best experts on this subject based on the ideXlab platform.