Gold Nanoparticles Stabilized by 1,2,3-Triazolyl Dendronized Polymers as Highly Efficient Nanoreactors for the Reduction of 4-Nitrophenol

Xiong, Liu; Mu, Shengdong; Long, Yanru; Qiu, Guirong; Ling, Qiangjun; Gu, Haibin; Lin, Wei

doi:10.1007/s10562-019-02662-5

Cited by 28 publications

(12 citation statements)

References 64 publications

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“…These results demonstrate that properties of the self-assembled polymer microenvironment influence the catalytic performance. Varying the properties of the polymer microenvironment in this case requires synthesis of different types of 1, 2, 3-triazlyl ligands as well as click-compatible polymer tails [ 15 ].…”

Section: Introductionmentioning

confidence: 99%

Accelerated Reaction Rates within Self-Assembled Polymer Nanoreactors with Tunable Hydrophobic Microenvironments

et al. 2020

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Performing reactions in the presence of self-assembled hierarchical structures of amphiphilic macromolecules can accelerate reactions while using water as the bulk solvent due to the hydrophobic effect. We leveraged non-covalent interactions to self-assemble filled-polymer micelle nanoreactors (NR) incorporating gold nanoparticle catalysts into various amphiphilic polymer nanostructures with comparable hydrodynamic nanoreactor size and gold concentration in the nanoreactor dispersion. We systematically studied the effect of the hydrophobic co-precipitant on self-assembly and catalytic performance. We observed that co-precipitants that interact with gold are beneficial for improving incorporation efficiency of the gold nanoparticles into the nanocomposite nanoreactor during self-assembly but decrease catalytic performance. Hierarchical assemblies with co-precipitants that leverage noncovalent interactions could enhance catalytic performance. For the co-precipitants that do not interact strongly with gold, the catalytic performance was strongly affected by the hydrophobic microenvironment of the co-precipitant. Specifically, the apparent reaction rate per surface area using castor oil (CO) was over 8-fold greater than polystyrene (750 g/mol, PS 750); the turnover frequency was higher than previously reported self-assembled polymer systems. The increase in apparent catalytic performance could be attributed to differences in reactant solubility rather than differences in mass transfer or intrinsic kinetics; higher reactant solubility enhances apparent reaction rates. Full conversion of 4-nitrophenol was achieved within three minutes for at least 10 sequential reactions demonstrating that the nanoreactors could be used for multiple reactions.

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Section: Introductionmentioning

confidence: 99%

Accelerated Reaction Rates within Self-Assembled Polymer Nanoreactors with Tunable Hydrophobic Microenvironments

et al. 2020

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“…Moreover, the difference in pore size of AuNP composites can also be explained by their different preparation methods. AuNPs‐HG‐1 exhibits the smallest pore size because the in situ ‐formed AuNPs could be well stabilized by the 1,2,3‐triazole structure and Fcium groups of oxidized P(NCHO‐ b ‐NFc‐ b ‐NTEG‐ b ‐NCHO) and thus probably improve the crosslinking degree among gelatin molecules. For the AuNPs‐HG‐2 , similar but decreased interactions are expected to take place.…”

Section: Resultsmentioning

confidence: 99%

AuNPs composites of gelatin hydrogels crosslinked by ferrocene‐containing polymer as recyclable supported catalysts

Long

Song

Shi

et al. 2019

J of Applied Polymer Sci

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To fabricate a recyclable supported catalyst based on gold nanoparticles (AuNPs) and gelatin hydrogel (HG) composites, a ferrocene (Fc)-containing tetrablock copolymer [P(NCHO-b-NFc-b-NTEG-b-NCHO)] was used as both reducing and stabilizing agents for AuNPs and as a crosslinker for HG. First, the effects of Fc-containing polymers, including homopolymer PNFc and copolymer P(NCHO-b-NFc-b-NTEG-b-NCHO), and different solvent systems on the morphology and aggregation of AuNPs were examined by using ultraviolet-visible spectroscopy, transmission electron microscopy, and dynamic light scattering. Second, two strategies (blending and soaking) were applied to prepare different AuNPs/HG composites (AuNPs-HG), and their structure and properties were studied by using various techniques including scanning electron microscopy, X-ray diffraction, and thermogravimetry. Finally, the catalytic performance and reusability of AuNPs-HG-1 (via blending) and AuNPs-HG-2 (via soaking) were evaluated utilizing the model catalytic reduction of 4-nitrophenol to 4-aminophenol by NaBH 4 . Results indicated that P(NCHO-b-NFc-b-NTEG-b-NCHO) dissolved in N,Ndimethylformamide was the optimal reductant and stabilizer to prepare AuNPs. The in situ reduction of Au III ions to Au 0 particles was very essential for the fabrication of AuNPs-HG in terms of hydrogel pore size, Au 0 distribution and immobilization stability, and hydrogel thermal stability. Due to the stronger interactions among AuNPs, P(NCHO-b-NFc-b-NTEG-b-NCHO), and gelatin molecules in the blending strategy, AuNPs-HG-1 showed better mechanical stability and catalytic performance and more reusing cycles than AuNPs-HG-2. This work highlights the design and fabrication of robust recyclable supported AuNP catalyst by using eco-friendly Fccontaining HGs.

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“…Related amphiphilic Janus dendrimers bearing benzotriazole units and hydrophilic oligo (ethylene glycol) (OEG) chain on one side and a hydrophobic benzyl ether dendron functionalized by two long aliphatic chains formed micelles as well and incorporated Ag and Cu NPs [80] (Figure 5b). In a final most recent variant a 1,2,3-triazolyl dendronized polymer formed micellar catalytic nanoreactors when decorated by Au NPs (Figure 5c) [81] Random copolymerization [82] and controlled di-block polymer formation [83] with ferrocene-containing dendrons, by ring-opening metathesis, afforded mixed dendronized polymers that self-assemble into spherical micelles (Figures 5 d, e), are capable of Ag and Au NP stabilization and the composites may perform 4nitrophenol reduction with extremely high turnover number up to 25000. (c) 1,2,3-triazolyl dendronized polymer.…”

Section: The Benchmark Reaction Of P-nitrophenolmentioning

confidence: 98%

“…(c) 1,2,3-triazolyl dendronized polymer. Provided by the Springer Nature SharedIt content-sharing initiative from [81]. (d) Synthesis and self-assembly of mixed dendronized triethylene glycol -ferrocene random copolymer.…”

Section: The Benchmark Reaction Of P-nitrophenolmentioning

confidence: 99%

Catalytic Neutralization of Water Pollutants Mediated by Dendritic Polymers

Arkas¹,

Anastopoulos²,

Giannakoudakis³

et al. 2021

Preprint

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Radially polymerized dendritic compounds are nowadays an established polymer category next to their linear, branched and cross-linked counterparts. Their uncommon tree-like architecture is characterized by adjustable internal cavities and external groups. They are therefore exceptional absorbents and this attainment of high concentrations into their interior renders them ideal reac-tion media. In this framework they are applied in many environmentally benign implementa-tions. One of the most important among them is water purification though pollutant decomposi-tion. Simple and composite catalysts and photo-catalysts containing dendritic polymers and ap-plied in water remediation will be discussed jointly with some unconventional solutions and fu-ture prospects.

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Gold Nanoparticles Stabilized by 1,2,3-Triazolyl Dendronized Polymers as Highly Efficient Nanoreactors for the Reduction of 4-Nitrophenol

Cited by 28 publications

References 64 publications

Accelerated Reaction Rates within Self-Assembled Polymer Nanoreactors with Tunable Hydrophobic Microenvironments

Accelerated Reaction Rates within Self-Assembled Polymer Nanoreactors with Tunable Hydrophobic Microenvironments

AuNPs composites of gelatin hydrogels crosslinked by ferrocene‐containing polymer as recyclable supported catalysts

Catalytic Neutralization of Water Pollutants Mediated by Dendritic Polymers

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