Achievement of efficient fractionation of lignocellulose and simultaneous valorization of corresponding components in one-pot biorefinery process remains as a great challenge. Here, we established an innovative approach employing bio-acid customized tertiary deep eutectic solvents (TDES) consisting of choline chloride and citric acid (maleic acid and lactic acid) alongside with presence of 1,4-butanediol, yielding three value-added products from biomass poplar: furfural, lignin nanospheres (LNS), and lignin-containing cellulose nanospheres (LCNS). The molecular interaction behaviors within lignin-lignin and lignin-deep eutectic solvents (DES) systems were predicted using density functional theory (DFT) and classical molecular dynamics (MD) methods. The TDES pretreated filtrate, abundant in hemicellulose (85 %), was successfully converted into furfural with a yield of 27 %. The resulting lignin underwent esterification with the bio-acid, in which the carboxyl group content increased by a remarkable 15-fold compared to cellulolytic enzyme lignin (CEL), providing a powerful driving force to obtain lignin nanospheres (<650 nm) through self-assembly process. The cellulose-rich residues with higher carboxyl content (1.25 mmol/g) were homogenized to fabricate lignin-containing nanocellulose spheres (LCNSs) with uniform size (200 nm) for the first time, acting as a promising right-handed chiral photonics with excellent photoluminescence properties. In summary, this work unveiled the potential of bio-acid tailored TDES as a sustainable medium for efficient fractionation of biomass components, achieving value-added nanomaterials and chemicals with substantial industrial downstream applicability.

中文翻译：

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通过生物酸定制的低共熔溶剂一锅处理，将木质纤维素全面升级为高价值的纳米材料和化学品


在一锅生物精炼过程中实现木质纤维素的有效分馏和相应成分的同时增值仍然是一个巨大的挑战。在这里，我们建立了一种创新方法，采用由氯化胆碱和柠檬酸（马来酸和乳酸）以及 1,4-丁二醇组成的生物酸定制三级低共熔溶剂 (TDES)，从而产生三种增值产品生物质杨树：糠醛、木质素纳米球（LNS）和含木质素的纤维素纳米球（LCNS）。使用密度泛函理论（DFT）和经典分子动力学（MD）方法预测木质素-木质素和木质素-低共熔溶剂（DES）系统内的分子相互作用行为。经过 TDES 预处理的滤液富含半纤维素 (85%)，成功转化为糠醛，产率为 27%。所得木质素与生物酸进行酯化反应，其羧基含量比纤维素分解酶木质素（CEL）显着增加15倍，为通过自水解获得木质素纳米球（<650 nm）提供了强大的驱动力。组装过程。具有较高羧基含量（1.25 mmol/g）的富含纤维素的残基首次被均质化，以制造具有均匀尺寸（200 nm）的含木质素的纳米纤维素球（LCNS），作为一种有前途的右手手性光子学，具有优异的光致发光特性。总之，这项工作揭示了生物酸定制 TDES 作为有效分馏生物质成分的可持续介质的潜力，实现具有大量工业下游适用性的增值纳米材料和化学品。