Lignin-derivable alternatives to petroleum-derived non-isocyanate polyurethane thermosets with enhanced toughness
Lignin-derivable alternatives to petroleum-derived non-isocyanate polyurethane thermosets with enhanced toughness
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木质素衍生的石油衍生非异氰酸酯聚氨酯热固性材料的替代品，具有增强的韧性
DOI：
10.1039/d2ma00895e
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发表时间：
2023
影响因子：
5
通讯作者：
Korley, LaShanda T.
中科院分区：
文献类型：
--
作者：
Mhatre, Sampanna V.;Mahajan, Jignesh S.;Epps, Thomas H.;Korley, LaShanda T.
木质素衍生的双愈创木酚和石油衍生的双酚A/F（BPA/BPF）之间的结构相似性表明，双愈创木酚可能是非异氰酸酯聚氨酯（NIPU）热固性材料中BPA/BPF的理想生物基替代品。在本文中，双愈创木酚/双酚衍生的环状碳酸酯的甲氧基含量和桥接碳取代的变化与两个不同链长的三胺固化，并检查这些差异对NIPU网络的热机械性能的影响。木质素衍生的环状碳酸酯中存在的甲氧基导致热固性材料与BPA/BPF基基准（韧性<$26 -35 MJ m−3，εb <$86 -166%）相比具有显著改善的韧性（<$49 -59 MJ m− 3）和断裂伸长率（εb <$195 -278%）。此外，在桥连碳上添加二甲基取代导致屈服强度（σy）增加-从具有未取代的桥连碳的网络的1.28MPa增加到二甲基取代的材料的1.45MPa。这些机械性能的增强是在保持基本的热固性性能的同时实现的，例如与应用相关的模量和热稳定性。最后，三胺交联剂提供了热机械性能的显著可调性，并产生了从具有高屈服强度（σy = 65-88 MPa）的刚性材料到柔性和坚韧网络的NIPU。总的来说，提出的结构-性能关系突出了一个有前途的框架，用于设计多功能的，生物衍生的，NIPU热固性材料。
The structural similarities between lignin-derivable bisguaiacols and petroleum-derived bisphenol A/F (BPA/BPF) suggest that bisguaiacols could be ideal biobased alternatives to BPA/BPF in non-isocyanate polyurethane (NIPU) thermosets. Herein, bisguaiacol/bisphenol-derived cyclic carbonates with variations in methoxy content and bridging-carbon substitution were cured with two triamines of different chain lengths, and the impact of these differences on the thermomechanical properties of NIPU networks was examined. The methoxy groups present in the lignin-derivable cyclic carbonates led to thermosets with significantly improved toughness (∼49–59 MJ m−3) and elongation at break (εb ∼195–278%) vs. the BPA/BPF-based benchmarks (toughness ∼ 26–35 MJ m−3, εb ∼ 86–166%). Furthermore, the addition of dimethyl substitution on the bridging carbon resulted in increased yield strength (σy) – from ∼28 MPa for networks with unsubstituted bridging carbons to ∼45 MPa for the dimethyl-substituted materials. These enhancements to mechanical properties were achieved while retaining essential thermoset properties, such as application-relevant moduli and thermal stabilities. Finally, the triamine crosslinkers provided substantial tunability of thermomechanical properties and produced NIPUs that ranged from rigid materials with a high yield strength (σy ∼ 65–88 MPa) to flexible and tough networks. Overall, the structure-property relationships presented highlight a promising framework for the design of versatile, bio-derivable, NIPU thermosets.
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