<br>通过选择性木质素分馏和部分解聚调节生物基 PU 涂料的性能,ACS Sustainable Chemistry & Engineering

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通过选择性木质素分馏和部分解聚调节生物基 PU 涂料的性能
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2023-04-21 , DOI: 10.1021/acssuschemeng.3c00889
Arjan T Smit _{1,

2} , Emanuela Bellinetto ₃ , Thomas Dezaire ₂ , Oussama Boumezgane ₃ , Luke A Riddell ₂ , Stefano Turri ₃ , Michiel Hoek ₁ , Pieter C A Bruijnincx ₂ , Gianmarco Griffini ₃

Affiliation

采用分馏和部分催化解聚相结合的新策略来调整木质素摩尔质量和羟基反应性（PU 涂料中使用的关键参数），制备出具有高木质素含量和可调性能的聚氨酯 (PU) 涂料。从山毛榉木片的中试规模分馏中获得的丙酮有机溶剂木质素在公斤级进行加工，生产具有特定摩尔质量范围（ M _w 1000-6000 g/mol）和降低的多分散性的木质素馏分。脂肪族羟基在木质素部分上相对均匀地分布，允许使用脂肪族多异氰酸酯连接体详细研究木质素摩尔质量和羟基反应性之间的相关性。正如预期的那样，高摩尔质量分数表现出低交联反应性，产生具有高玻璃化转变温度（ T _g ）的刚性涂层。较低的M _w部分显示出增加的木质素反应性、交联程度，并且使涂层具有增强的柔韧性和较低的T _g 。通过山毛榉木木质素及其高摩尔质量分数的木质素部分解聚还原（PDR）可以进一步调整木质素特性；观察到 PDR 工艺从实验室到未来工业场景中涂层应用所需的中试规模的出色转化。木质素解聚显着提高了木质素反应性，由_{PDR 木质素生产的涂料显示出最低的 Tg}值和最高的涂料柔韧性。总体而言，这项研究为生产具有定制性能和高（>90%）生物质含量的PU涂料提供了强有力的策略，为开发完全绿色和循环的PU材料铺平了道路。

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Tuning the Properties of Biobased PU Coatings via Selective Lignin Fractionation and Partial Depolymerization

Polyurethane (PU) coatings with high lignin content and tunable properties were made using a combination of fractionation and partial catalytic depolymerization as a novel strategy to tailor lignin molar mass and hydroxyl group reactivity, the key parameters for use in PU coatings. Acetone organosolv lignin obtained from pilot-scale fractionation of beech wood chips was processed at the kilogram scale to produce lignin fractions with specific molar mass ranges (M_w 1000–6000 g/mol) and reduced polydispersity. Aliphatic hydroxyl groups were distributed relatively evenly over the lignin fractions, allowing detailed study of the correlation between lignin molar mass and hydroxyl group reactivity using an aliphatic polyisocyanate linker. As expected, the high molar mass fractions exhibited low cross-linking reactivity, yielding rigid coatings with a high glass transition temperature (T_g). The lower M_w fractions showed increased lignin reactivity, extent of cross-linking, and gave coatings with enhanced flexibility and lower T_g. Lignin properties could be further tailored by lignin partial depolymerization by reduction (PDR) of the beech wood lignin and its high molar mass fractions; excellent translation of the PDR process was observed from laboratory to the pilot scale necessary for coating applications in prospective industrial scenarios. Lignin depolymerization significantly improved lignin reactivity, and coatings produced from PDR lignin showed the lowest T_g values and highest coating flexibility. Overall, this study provides a powerful strategy for the production of PU coatings with tailored properties and high (>90%) biomass content, paving the path to the development of fully green and circular PU materials.

更新日期：2023-04-21

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