Pd-catalysed oxidative C–H/C–H coupling polymerization for polythiazole-based derivatives

Zhang, Qiang; Li, Yuefeng; Lu, Yan; Zhang, Huijing; Li, Miaomiao; Yang, Yang; Wang, Jing; Chen, Yongsheng; Li, Chenxi

doi:10.1016/j.polymer.2015.05.035

Cited by 134 publications

(176 citation statements)

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“…Such nanocomposite hydrogels containing charged inorganic CNPs may undergo exceptional changes either in mechanical or optical behavior in response to the alternating application and removal of an electric field, with these changes arising from the varied alignment of CNPs and the polymeric chains. 130 4. High functional applications of clay mineral-containing nanocomposite hydrogels…”

Section: Stimuli-responsivenessmentioning

confidence: 99%

Recent advances in clay mineral-containing nanocomposite hydrogels

et al. 2015

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Clay mineral-containing nanocomposite hydrogels have been proven to have exceptional composition, properties, and applications, and consequently have attracted a significant amount of research effort over the past few years. The objective of this paper is to summarize and evaluate scientific advances in clay mineral-containing nanocomposite hydrogels in terms of their specific preparation, formation mechanisms, properties, and applications, and to identify the prevailing challenges and future directions in the field. The state-of-the-art of existing technologies and insights into the exfoliation of layered clay minerals, in particular montmorillonite and LAPONITE s , are discussed first. The formation and structural characteristics of polymer/clay nanocomposite hydrogels made from in situ free radical polymerization, supramolecular assembly, and freezing-thawing cycles are then examined. Studies indicate that additional hydrogen bonding, electrostatic interactions, coordination bonds, hydrophobic interaction, and even covalent bonds could occur between the clay mineral nanoplatelets and polymer chains, thereby leading to the formation of unique three-dimensional networks. Accordingly, the hydrogels exhibit exceptional optical and mechanical properties, swelling-deswelling behavior, and stimuli-responsiveness, reflecting the remarkable effects of clay minerals. With the pivotal roles of clay minerals in clay mineral-containing nanocomposite hydrogels, the nanocomposite hydrogels possess great potential as superabsorbents, drug vehicles, tissue scaffolds, wound dressing, and biosensors. Future studies should lay emphasis on the formation mechanisms with in-depth insights into interfacial interactions, the tactical functionalization of clay minerals and polymers for desired properties, and expanding of their applications.

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Section: Stimuli-responsivenessmentioning

confidence: 99%

Recent advances in clay mineral-containing nanocomposite hydrogels

et al. 2015

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“…Compared to the Yamamoto‐type polymerization in the literature, which yields P4* with M n of 16 600 and PDI of 6.7 in a total yield of 22 % over two steps, the C−H/C−H‐type DArP produces P4 with a higher M n of 22 400, a lower PDI of 1.54, and a higher yield of 56 % in one step, which shows remarkable superiority. The advantage could possibly be a result of either the poor air‐stability of Ni(COD) 2 that promotes the Yamamoto reaction or the high reactivity of the C5−H bond of thiazole that facilitates the C−H/C−H‐type coupling …”

Section: Methodsmentioning

confidence: 99%

Oxidative Direct Arylation Polymerization Using Oxygen as the Sole Oxidant: Facile, Green Access to Bithiazole‐Based Polymers

Guo

You

2016

ChemSusChem

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The most appealing oxidant, molecular oxygen, is employed for the first time as the sole oxidant in the transition metal-catalyzed oxidative direct arylation polymerization (C-H/C-H-type DArP), which eliminates by-product formation of stoichiometric metal salts except for water . Compared to conventional approaches, other than the avoidance of an end-capping procedure, the current protocol is remarkably advanced in the aspect of eco-friendliness, step- and cost-economy, and, of special significance, the purity of polymer products. As illustrative examples, six 5,5'-bithiazole-based polymers are synthesized using this new method, demonstrating higher number-average molecular weight (M up to 33 700) in better yields (up to 93 %) through only one step. The evolution of C-H/C-H-type DArP from heavy metal salts to O alone as the oxidant could solve the problem of metal residues in polymers, which is considered harmful to the performance of devices.

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“…-/0 的价层分子轨道图 Figure 12 Valence molecular orbitals for the ground states of (a) NbMoS 7 and (b) [82,83] : Figure 14 Optimized ground states for NbMoS n -/0 (n＝3～7) clusters at the B3LYP/Basis-II level of theory Figure 15 The averaged binding energy (E b ) and second-order energy difference (△ 2 E) of NbMoS n -/0 (n＝3～7) as a function of S content (n) 能促进 H 2 解离成活性氢原子 [87] . 此外, 铌硫化物也被报道在 HDS 等反应中表现出了优异的催化性能 [88] .…”

Section: Nbmosmentioning

confidence: 99%

Theoretical Investigations on the Structures and the Chemical Bonding of NbMoS_n^-/0 (n=3~7) Clusters

王彬¹,

王剑福²,

张晓菲³

et al. 2017

Acta Chim. Sinica

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307化学学报 Abstract Recently, transition metal sulfides (TMS) have played an important role in many catalytic reactions. In particular, they are widely used in the petrochemical industry, such as the hydrodesulfurization (HDS) and the hydrodenitrogenation (HDN) processes. In this work, density functional theory (DFT) and coupled cluster theory [CCSD(T)] calculations were used to study the niobium-mixed di-nuclear molybdenum sulfide clusters NbMoS n -/0 (n＝3～7). In our calculations, their ground-state structures were determined and the effects of doping metal, adjusting the sulfur content (n) and changing the charge states of clusters were discussed on the geometries, electronic structures and chemical bonding of NbMoS n -/0 (n＝ 3～7). NbMoS n -/0 (n＝3～7) clusters can be viewed as linking different sulfur ligands to the NbMoS 2 four-membered rings. Among them, diverse poly-sulfur ligands, such as bridging S 2 , terminal S 2 and terminal S 3 groups, emerged in the sulfur-rich clusters. Generalized Koopmans' Theorem was employed to predict the vertical detachment energies (VDEs), and simulate the corresponding anionic photoelectron spectra (PES). The first VDEs (VDE 1st ) of NbMoS n -(n＝3～6) increased gradually as a function of n, and then decreased suddenly when the sulfur content (n) reached 7. The VDE 1st reached the maximum by 4.69 eV when the sulfur content equaled to 6. The driving forces (-ΔG) of the reduction reactions between NbMoS n -/0 (n ＝3～7) and H 2 were evaluated. The NbMoS-anion with the terminal 2 2 S -group yielded the negative value of ΔG, which indicated that the reaction is thermodynamically favored even at the room temperature. We predicted that doping niobium into the molybdenum sulfides may improve the emergence of S 2 group which may be helpful in producing the coordinatively unsaturated sites (CUS) under the H 2 /H 2 S atmosphere. Molecular orbital analyses are performed to improve our understanding on the structural evolution and the chemical bonding of NbMoS n -/0 (n＝3～7) clusters.

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Pd-catalysed oxidative C–H/C–H coupling polymerization for polythiazole-based derivatives

Cited by 134 publications

References 28 publications

Recent advances in clay mineral-containing nanocomposite hydrogels

Recent advances in clay mineral-containing nanocomposite hydrogels

Oxidative Direct Arylation Polymerization Using Oxygen as the Sole Oxidant: Facile, Green Access to Bithiazole‐Based Polymers

Theoretical Investigations on the Structures and the Chemical Bonding of NbMoS_n^-/0 (n=3~7) Clusters

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Pd-catalysed oxidative C–H/C–H coupling polymerization for polythiazole-based derivatives

Cited by 134 publications

References 28 publications

Recent advances in clay mineral-containing nanocomposite hydrogels

Recent advances in clay mineral-containing nanocomposite hydrogels

Oxidative Direct Arylation Polymerization Using Oxygen as the Sole Oxidant: Facile, Green Access to Bithiazole‐Based Polymers

Theoretical Investigations on the Structures and the Chemical Bonding of NbMoSn-/0 (n=3~7) Clusters

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Theoretical Investigations on the Structures and the Chemical Bonding of NbMoS_n^-/0 (n=3~7) Clusters