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1. Aromatics from Lignocellulosic Biomass: A Platform for High-Performance Thermosets

   https://doi.org/10.1021/acssuschemeng.0c04817  

   Mahajan, Jignesh S.; O’Dea, Robert M.; Norris, Joanne B.; Korley, LaShanda T.; Epps, Thomas H. (October 2020, ACS Sustainable Chemistry & Engineering)

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2. Efficient Manufacture, Deconstruction, and Upcycling of High-Performance Thermosets and Composites

   https://doi.org/10.1021/acsaenm.2c00115  

   Lloyd, Evan M.; Cooper, Julian C.; Shieh, Peyton; Ivanoff, Douglas G.; Parikh, Nil A.; Mejia, Edgar B.; Husted, Keith E.; Costa, Letícia C.; Sottos, Nancy R.; Johnson, Jeremiah A.; et al (November 2022, ACS Applied Engineering Materials)

   Thermoset polymers and fiber-reinforced polymer composites possess the chemical, physical, and mechanical properties necessary for energy-efficient vehicles and structures, but their energy-inefficient manufacturing and the lack of end-of-life management strategies render these materials unsustainable. Here, we demonstrate end-of-life deconstruction and upcycling of high-performance poly(dicyclopentadiene) (pDCPD) thermosets with a concurrent reduction in the energy demand for curing via frontal copolymerization. Triggered material deconstruction is achieved through cleavage of cyclic silyl ethers and acetals incorporated into pDCPD thermosets. Both solution-state and bulk experiments reveal that seven- and eight-membered cyclic silyl ethers and eight-membered cyclic acetals are incorporated efficiently with norbornene-derived monomers, permitting deconstruction at low comonomer loadings. Frontal copolymerization of DCPD with these tailored cleavable comonomers enables energy-efficient manufacturing of sustainable, high-performance thermosets with glass transition temperatures of >100 °C and elastic moduli of >1 GPa. The polymers are fully deconstructed, yielding hydroxyl-terminated oligomers that are upcycled to polyurethane-containing thermosets having a higher glass transition temperatures than that of the original polymer upon reaction with diisocyanates. This approach is extended to frontally polymerized fiber-reinforced composites, where large-fiber volume fraction composites (Vf = 65%) containing a cleavable comonomer are deconstructed and the reclaimed fibers are used to regenerate composites via frontal polymerization that display properties nearly identical to those of the original. This work demonstrates that the use of cleavable monomers, in combination with frontal manufacturing, provides a promising strategy to address sustainability challenges for high-performance materials at multiple stages of their lifecycle. 

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3. Synthesis of ultrafast wavepackets with tailored spatiotemporal properties

   https://doi.org/10.1038/s41566-022-01055-2  

   Cruz-Delgado, Daniel; Yerolatsitis, Stephanos; Fontaine, Nicolas K.; Christodoulides, Demetrios N.; Amezcua-Correa, Rodrigo; Bandres, Miguel A. (January 2022, Nature Photonics)
4. Tailored PVDF Graft Copolymers via ATRP as High-Performance NCM811 Cathode Binders

   https://doi.org/10.1021/acsmaterialslett.3c00485  

   Liu, Tong; Parekh, Rohan; Mocny, Piotr; Bloom, Brian P.; Zhao, Yuqi; An, So Young; Pan, Bonian; Yin, Rongguan; Waldeck, David H.; Whitacre, Jay F.; et al (August 2023, ACS Materials Letters)
5. Highly fluorescent purine-containing conjugated copolymers with tailored optoelectronic properties

   https://doi.org/10.1039/D2PY00545J  

   O'Connell, C. Elizabeth; Sabury, Sina; Jenkins, J. Elias; Collier, Graham S.; Sumpter, Bobby G.; Long, Brian K.; Kilbey, S. Michael (August 2022, Polymer Chemistry)

   Conjugated copolymers containing electron donor and acceptor units in their main chain have emerged as promising materials for organic electronic devices due to their tunable optoelectronic properties. Herein, we describe the use of direct arylation polymerization to create a series of fully π-conjugated copolymers containing the highly tailorable purine scaffold as a key design element. To create efficient coupling sites, dihalopurines are flanked by alkylthiophenes to create a monomer that is readily copolymerized with a variety of conjugated comonomers, ranging from electron-donating 3,4-dihydro-2 H -thieno[3,4- b ][1,4]dioxepine to electron-accepting 4,7-bis(5-bromo-3-hexylthiophen-2-yl)benzo[ c ][1,2,5]thiadiazole. The comonomer choice and electronic nature of the purine scaffold allow the photophysical properties of the purine-containing copolymers to be widely varied, with optical bandgaps ranging from 1.96–2.46 eV, and photoluminescent quantum yields as high as ϕ = 0.61. Frontier orbital energy levels determined for the various copolymers using density functional theory tight binding calculations track with experimental results, and the geometric structures of the alkylthiophene-flanked purine monomer and its copolymer are found to be nearly planar. The utility of direct arylation polymerization and intrinsic tailorability of the purine scaffold highlight the potential of these fully conjugated polymers to establish structure–property relationships based on connectivity pattern and comonomer type, which may broadly inform efforts to advance purine-containing conjugated copolymers for various applications. 

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