Global environmental crises and energy depletion have spurred the development of sustainable plastics from renewable resources. However, the application of these materials is frequently hindered by complex production processes and their subpar performance compared to conventional plastics. In this study, we introduce a scalable bio-based bisphenol monomer and synthesize sustainable polycarbonates (PCs) using melt polymerization with diphenyl carbonate, a CO2 derivative, and bio-based toughening components. These PCs offer customizable thermal and mechanical properties, with a peak glass transition temperature of 95.5 degrees C and a maximum tensile strength of 63.1 MPa, outperforming commercial plastics such as polystyrene. The triphenylmethane structure in PCs enables excellent clusteroluminescence properties, enabling the development of inks for information encryption and optical anti-counterfeiting applications. Based on the CTE properties of bio-PCs, we further develop a functional bio-based negative photoresist (bio-NP), which demonstrate potential for semiconductor manufacturing (a high resolution of 3 mu m) and optical storage applications (their clusteroluminescence effect). This work establishes a new paradigm for developing high-performance bio-based polymers and exploring their high-value applications.

With the rise of circular economy, self-healing polymers have attracted significant attention for their longer lifespan and greater recyclability compared with traditional thermoplastics and thermosetting polymers. However, addressing the instability of self-healing units to develop high-performance materials remains a challenge. Herein, we report a series of superior self-healing polyimine derivatives, biobased polyacylhydrazones (bio-PHys), via aldehyde-hydrazide condensation. The coexistence of amide bonds and imine bonds, which provide hydrogen bonding and dynamics, imparts remarkable mechanical properties (tensile strength of 103 MPa, elongation at break of 180%) to bio-PHys, along with notable self-healing capabilities under glass transition temperature (Tg). Bio-PHys also exhibits potential for scalable production, excellent processability, and photoluminescence characteristics. We explored its application in adhesive-free laminated substrates and thoroughly investigated the aggregation-induced emission of the acylhydrazone group. Furthermore, we utilized bio-PHys to create recyclable smart paper for anticounterfeiting and dynamic information storage. This work presents a novel approach to developing high-performance self-healing polymers.

Aliphatic polycarbonates (APCs) have become an essential packaging material because of their renewability, biodegradability, and biocompatibility. In this study, a series of high molecular weights APCs have been successfully synthesized using dimethyl carbonate (DMC) and different lengths of aliphatic diols with even carbon (n -CH2 = 4–12) via melt polymerization. Thermal properties, isothermal crystallization behavior, crystal structure, and scale of microstructure of APCs indicated that the flexibility and crystallization of molecular chains gradually increased with the increasing number of methylene groups of repeating units. However, due to the rigidity of ester group was higher than methylene group, and crystallization could increase the rigidity of chain segments, yielding strength and Young’s modulus of APCs decreased first and then gradually increased with the increasing number of methylene groups in the repeating units. Furthermore, the scale of microstructure indicated that Brill transition increased the distance between intermolecular chains. Therefore, although the trans-gauche coexistence chain conformation simultaneously decreased the rigidity and crystallization of chain segments, barrier property of poly(octamethylene carbonate) with Brill transition was similar to long-chain APCs because of the lengthened diffusion path. The analytical mechanism of structure-performance relationship from the viewpoint of molecular interactions and chain structure will provide an entirely new thought for developing new barrier materials.

Adding nucleating agents has been a successful strategy to boost the heat resistance of poly(L-lactic acid) (PLLA) by increasing the crystallinity. In this study, a new series of bio-based complexes as nucleating agents for PLLA, including twelve combinations of three eco-friendly metal ions (Zn, Mg, Ca) and four biomass-derived α-hydroxy acids, were successfully synthesized to respectively investigate the effects of metal ions as well as ligands on nucleation capacity of complexes. By investigating the non-isothermal and isothermal crystallization at 135 °C of PLLA with 0.3 wt% loading of complexes, both zinc and magnesium salts of L-mandelic acid showed excellent nucleation capacities. And magnesium L-mandelate performed better, raising the crystallinity of PLLA to 44.4 % as well as minimizing its crystallization half-time from 73 min to 2.7 min. The growth and denser distribution of PLLA spherulites on the salt surface were also observed by POM, reflecting epitaxial nucleation as the possible mechanism. A novel inspiration, utilizing VESTA software to simulate the crystal structure of zinc L-mandelate (Zn(L-MA)2), was proposed to determine the nucleation mechanism. Also, using polyethylene terephthalate (PET) as a test protocol, the rationality of the model could be approved by checking the fitness of nucleating prediction and experiment results.

A series of complexes consisting of natural amino acids and tin (Sn(AA) 2 ) prepared by conventional neutralization reactions were tested as a new class of cost-effective catalysts with high reactivity and low toxicity towards some biocompatible aliphatic polyesters. In our system, by using a simple catalyst and a benzyl alcohol (BnOH) initiator, biocompatible, and biodegradable aliphatic polyesters, such as poly( l -lactide), poly(ε-caprolactone), and poly(trimethylene carbonate), were well prepared. The results demonstrated that Sn(AA) 2 catalysts, especially the phenylalanine-tin complex (Sn(L-Phe) 2 ) ( M n, up to 194 kg/mol), were suitable for the synthesis of moderate and high-molecular weight poly( l -lactide), which exhibited good biocompatibility. Analysis of the backbone structure and end groups of low-molar-mass polymers by using MALDI-TOF mass spectra and 1 H NMR spectroscopy suggested that the reaction proceeds by a dual activation mechanism. Given their low cost, simple preparation, high reactivity, and low toxicity, complexes consisting of natural amino acids and tin are promising for industrial-scale production of biocompatible aliphatic polyesters.