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Topologically Precise and Discrete Bottlebrush Polymers: Synthesis, Characterization, and Structure-Property Relationships.

ABSTRACT: As the complexity of polymer structure grows, so do the challenges for developing an accurate understanding of their structure-property relationships. Here, the synthesis of bottlebrush polymers with topologically precise and fully discrete structures is reported. A key feature of the strategy is the synthesis of discrete macromonomer libraries for their polymerization into topologically precise bottlebrushes that can be separated into discrete bottlebrushes (Đ = 1.0). As the system becomes more discrete, packing efficiency increases, distinct three-phase Langmuir-Blodgett isotherms are observed, and its glass transition temperature becomes responsive to side-chain sequence. Overall, this work presents a versatile strategy to access a range of precision bottlebrush polymers and unravels the impact of side-chain topology on their macroscopic properties. Precise control over side chains opens a pathway for tailoring polymer properties without changing their chemical makeup.

SUBMITTER: Ogbonna ND

PROVIDER: S-EPMC9088296 | biostudies-literature | 2022 Apr

REPOSITORIES: biostudies-literature

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Topologically Precise and Discrete Bottlebrush Polymers: Synthesis, Characterization, and Structure-Property Relationships.

Ogbonna Nduka D ND Dearman Michael M Cho Cheng-Ta CT Bharti Bhuvnesh B Peters Andrew J AJ Lawrence Jimmy J

JACS Au 20220318 4

As the complexity of polymer structure grows, so do the challenges for developing an accurate understanding of their structure-property relationships. Here, the synthesis of bottlebrush polymers with topologically precise and fully discrete structures is reported. A key feature of the strategy is the synthesis of discrete macromonomer libraries for their polymerization into topologically precise bottlebrushes that can be separated into discrete bottlebrushes (<i>Đ</i> = 1.0). As the system becom ...[more]

PMID: 35557765

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Project description:The 3D coordination polymers of lead (II) [Pb4(O)(L)3(H2O)]n, where H2L = C6H4(CO2H)2 (benzene-1,3-dicarboxylic acid), were synthesized in crystalline (1(a, b)) and amorphous (2(a, b)) phases. Hydrothermal and branch tube methods were used to self-assemble lead (II) from the bottom up to create the crystalline phases. Single-crystal X-ray diffraction (SC-XRD) was used to investigate two crystallized metal-organic frameworks (MOFs) with the same space group and chemical formula (P21/c). Through controlled green sonochemical methods, an ultrasonic bath and a probe homogenizer were used to prepare nano [Pb4(O)(L)3(H2O)]n in the amorphous phase. An extensive study has been conducted on the effect of initial reagent concentration, ultrasonic power, temperature, reaction time, and surfactant presence on the size and morphology of synthesized nanocoordination polymers. Analyses of the synthesized compounds were performed using scanning electron microscopy (SEM), powder X-ray diffraction (PXRD), FT-IR spectroscopy, and CHNS elemental analysis. By using thermal gravimetry (TGA-DTA), the thermal stability of nanostructures was examined and compared with that of crystalline structures. A Hirschfeld surface and a two-dimensional fingerprint diagram were used to analyze intermolecular interactions in crystalline phases. Photocatalytic degradation of methylene blue was investigated using 1a and 2b_2, which represent the synthetic compounds. Calculation of the band gap of synthesized polymers was conducted using the Tauc diagram (based on the DRS results). During optimal conditions of C0 = 0.6 mg L1, pH = 7, and irradiation time = 60 min, the maximum photodegradation efficiencies of methylene blue (MB) were observed for 1a and 2b_2. In terms of degradation efficiency, 1a's reusability was 73.5 % for the first cycle and 70.6 % for the fifth, while 2b_2's reusability was 88.2 % for the first cycle and 81.7 % for the fifth. These materials can be used in multiple photocatalytic cycles based on the results obtained.

Dataset Information

Topologically Precise and Discrete Bottlebrush Polymers: Synthesis, Characterization, and Structure-Property Relationships.

Publications

Topologically Precise and Discrete Bottlebrush Polymers: Synthesis, Characterization, and Structure-Property Relationships.

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