Enhancing blue-light-initiated photopolymerization in a three-component system: kinetic and modeling of conversion strategies

Lin, Jui‐Teng; Chen, Kuo-Ti; Chang, Po-Kuang; Cheng, Da‐Chuan

doi:10.1007/s10965-020-02398-6

Cited by 17 publications

(27 citation statements)

References 17 publications

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“…As reported by van der Laan et al [4], the effectiveness of a photoinhibitor in a two-color system is strongly monomer-dependent, which also requires: (i) a high conversion of bluephotoinitiation in the absence of the UV-active inhibitor; (ii) a strong chain termination with significant reduction of blue and UV conversion in the presence of UV-active inhibitor and (iii) short induction time or rapid elimination of the inhibitor species in the dark (or absence of UVlight) [22]. Synergic effects have been reported using co-initiator and/or additives and 2-and 3wavelength systems [8,10]. Conversion efficiency may be also improved by reduction of the oxygen inhibition effect [23].…”

Section: Enhancement Strategiesmentioning

confidence: 99%

“…The present comprehensive model (with minimum mathematics) will focus on the enhancement mechanisms/pathways, provides analytic formulas which can be used to analyze reported data, and, more importantly, serves as guidance for exploring new functional materials or new kinetic schemes for improved conversion or procedures in applications such as additive manufacturing (AM), 3D and 4D bioprinting. The present article will skip most of the detailed derivations of the formulas with an emphasis on the synergic and enhancement schemes, whereas more complex kinetics with detailed mathematical approaches, may refer to the modeling published by Lin et al [7][8][9][10][11]17,23]. Furthermore, a greater details on the schemes of various systems can be found in Lin et al [25].…”

Section: Introductionmentioning

confidence: 99%

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Unified Theory for Hybrid-Photocatalysts: A Review on New Strategies for Synergic, Enhanced Conversion Efficacy and Photoredox Cycle

Lin¹

2021

Preprint

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This article presents, for the first time, comprehensive model based on the proposed mechanism of Rahal et al [17], Bonardi {20], Tar et al [20], and Mau et al [24], for 3-component systems of G1/Iod/EDB, G1/Iod/amine (in gold chloride), and Iod/Benzoic/Borate (for reduced oxygen inhibition) for the hybri free radical (FRP) and cationic (CP) photopolymerization of interpenetrated polymer network (IPN) systems. Analytic formulas are developed to explore the new features including: (i) conversion efficacy(CE) of FRP is an increasing function of the light intensity (I), the effective absorption coefficient (b), for transient state, whereas, CE at steady-state is independent to the light intensity; (ii) initiator regeneration (RGE) provides a catalytic cycle for improved CE for FRP and CP; (iii) in the IPN system, the synergic effects due to the co-exist of FRP and CP include: (i) CP can increase the medium viscosity limiting the diffusional oxygen replenishment, such that OIH is reduced; (ii) the cationic monomer also acts as a diluting agent for the radical polymer network, and (iii) the exothermic property of the CP polymerization. We have proposed ascaling law for the transient and steady-state dependence of CE on the key parameter P=bIC0, given by a an m-order power law of Pm, with m = 0.5 to 1.5, depending on various conditions. The CE also has an optimal value for maximum CE. The presented comprehensive model (with minimum mathematics) focusing on the enhancement mechanisms/pathways, provides analytic formulas which can be used to analyze reported data, and, more importantly, serves as guidance for exploring new functional materials or new kinetic schemes for improved conversion or procedures for both industrial and medical applications such as additive manufacturing (AM), 3D and 4D bioprinting. Finally, we have proposed new directions/experiments based on our theoretical predictions.

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Section: Enhancement Strategiesmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Unified Theory for Hybrid-Photocatalysts: A Review on New Strategies for Synergic, Enhanced Conversion Efficacy and Photoredox Cycle

Lin¹

2021

Preprint

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“…Light sources in UV (365 nm) has been conventionally widely, whereas light sources in near-UV (400-410 nm) and visible (430 to 680 nm) and near infrared (700 to 1064 nm) have been explored more recently in various applications such as additive manufacturing (AM), 3D and 4D bioprinting [3,4]. Both spatial and temporal controlled 3D processes were reported using single and multiple wavelength lights [7][8][9][10][11].…”

Section: Introductionmentioning

confidence: 99%

Efficacy Modeling of New Multi-Functional Benzophenone-Based System for Free-Radical/Cationic Hybrid Photopolymerization Using 405 nm LED

Lin¹,

Lalevée²

2021

Preprint

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This article presents, for the first time, the kinetics and the general conversion features of a 3-component system, BT(BC)/iodonium/Amine, based on proposed mechanism of Liu et al, for both free radical polymerization (FRP) of acrylates and the free radical promoted cationic polymerization (CP) of epoxides using the new multi-functional initiator of benzophenone–triphenylamine (BT). The additives, iodonium and EDB, have the dual function of (i) regeneration BT and (ii) produce of extra radicals for improved FRP and CP. Analytic formulas are developed to explore the new features including: (i) the conversion efficacy (CE) of FRP is an increasing function of the light intensity, the effective absorption coefficient, and the concentration sum of each of the components, BT, Iod, amine, for transient state. However, CE at steady-state is independent to the light intensity; (ii) the trifunctional hybrid structures of BT3 leads to larger light absorption than other types of BT; it also provides more active sites for the H-abstraction in the presence of EDB, leading to high CE; (iii) the efficacy of FRP is an increasing function of the amine (EDB) concentration, in contrast to that of CP having an opposite dependence; (iv) the consumption rate of BT3 in the BT3/ Iod/EDB system is slower than that of the BT3/Iod system due to photoredox catalytic cycle, and the larger initiator regeneration (RGE) in the three-component system. A comprehensive model is also proposed that the CE (for both FRP and CP) is governed by (NjKjbI), whereas more complex formulas are developed; where Kj is an effective rate constant proportional to the electron transfer quantum yield, and the combined effects of other coupling rate constants; b is an effective absorption coefficient given by the light absorption and excited state quantum yield.

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“…Both spatial and temporal controlled 3D processes were reported using single and multiple wavelength lights [5,6]. We have reported the kinetics and efficacy analysis for various strategies for improved conversion, such as co initiators, co additives in both single and multiple components systems [7][8][9][10][11].…”

Section: Introductionmentioning

confidence: 99%

Efficacy Analysis of In Situ Synthesis of Nanogold via Copper/Iodonium/Amine/Gold System Under a Visible Light

Lin¹,

Lalevée²,

Tar³

et al. 2021

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. This article presents, for the first time, the kinetics and the general features of a photopolymerization system (under visible light) G1/ Iodonium/ TEA/gold chloride (or A/B/N/G), having initial concentrations of A0, B0, N0 and G0, based on the proposed mechanism of Tar et al. Analytic formulas are developed to explore the new features including: (i) both FRP efficacy and the production of nanogold (NG) are proportional to the relative concentration ratios of (A0+B0+N0)/G0, which may be optimized for maximum efficacy; (ii) the two competing procedure of NG production and efficacy of free radical photopolymerization (FRP) can be tailored for optimal system with nanogold in the polymer matrix;(ii) the FRP efficacy is contributed by 3 components: the coupling of the excited state of copper complex (T) with the radicals (R and S) produced by the iodonium and the amine; (iii) the production of NG is contributed by 2 components: the coupling of T and radical (S) with gold ion; (iv) NG production has a transient state value which is an increasing function of light intensity and the combined concentration ratio [(A0/G0)+(N0/(K'M0). whereas it has a steady-state independent to the light intensity.

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Enhancing blue-light-initiated photopolymerization in a three-component system: kinetic and modeling of conversion strategies

Cited by 17 publications

References 17 publications

Unified Theory for Hybrid-Photocatalysts: A Review on New Strategies for Synergic, Enhanced Conversion Efficacy and Photoredox Cycle

Unified Theory for Hybrid-Photocatalysts: A Review on New Strategies for Synergic, Enhanced Conversion Efficacy and Photoredox Cycle

Efficacy Modeling of New Multi-Functional Benzophenone-Based System for Free-Radical/Cationic Hybrid Photopolymerization Using 405 nm LED

Efficacy Analysis of In Situ Synthesis of Nanogold via Copper/Iodonium/Amine/Gold System Under a Visible Light

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