Collaborative Research: Low-Energy Tandem Process for Fractionation and Reversible Preservation of Lignocellulose Using Multifunctional Aldehyde Sulfonic Acids

合作研究：使用多功能醛磺酸对木质纤维素进行分馏和可逆保存的低能量串联工艺

• 批准号: 2241487
• 负责人: Qiang Yang
• 金额: $ 27.41万
• 依托单位: Michigan State University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2022
• 资助国家: 美国
• 起止时间: 2022-10-01 至 2025-03-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2241487&HistoricalAwards=false
• 关键词: Collaborative; Research; Low; Energy; Tandem

Lignocellulose is a promising alternative to fossil resources for the production of fuels, chemicals, and materials. However, most current biomass fractionation processes face issues such as unwanted loss of carbohydrate fractions (cellulose fibers and hemicellulose sugars) and significant structure changes of lignin (aromatic compounds) during the process, both of which devalue the fractionated components. The proposed project will develop an energy-efficient, inexpensive, and value-preserving biomass fractionation system using aldehyde sulfonic acids. The success of the proposed research will directly impact the U.S. lignocellulose-based biorefinery, pulp and paper industries, and other related sectors. It will also contribute to a low-carbon bioeconomy by replacing petroleum feedstocks and reducing energy consumption in the fractionation process. The project will promote STEM education in biorefineries, bioenergy, and bioproducts (3B) through graduate and undergraduate student training (particularly female and minority students) and curriculum development. This project will also include outreach activities with K-12 students by providing lab tours, summer practicums, and research projects for the students interested in the 3B fields. The proposed research uses novel aldehyde sulfonic acids (aldehyde-containing aromatic sulfonic acids) to accomplish a rapid and near-complete fractionation of lignocellulosic biomass without the need for significant biomass size-reduction pretreatment. This process not only maximizes the production of cellulose, hemicellulose, and lignin but it also reduces process energy consumption relative to existing methods. Using a model-based molecular design approach, aldehyde sulfonic acids with tunable structure, physical properties, and reactivity will be synthesized from inexpensive aldehyde-containing aromatics by sulfonation. Mechanistically, aldehyde sulfonic acids fractionate lignocellulose through the sulfonic acid group and then protect carbohydrates and lignin from degradation and condensation by interaction with the aldehyde group. Because of their multifunction nature as a catalyst, solvent, and preserver, aldehyde sulfonic acids are expected to fractionate centimeter-sized lignocellulose feedstocks rapidly and nearly completely under mild conditions into cleavable and upgradable lignin, cellulose, and hemicellulose. This research will test the central hypothesis that aldehyde sulfonic acid would be more effective and selective than current combinations of mineral/organic acids and aldehydes in fractionating lignocellulose. Mathematical models will be developed using quantitative structure-performance analysis to predict structural properties and performance of a range of aldehyde sulfonic acids. The tandem depolymerization and reversible preservation of lignin and hemicellulose will be mechanistically elucidated through these modeling studies to understand the cleavage reaction kinetics of the acid-labile linkages and the formation of protective chemical groups.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

木质纤维素是生产燃料、化学品和材料的有前途的化石资源替代品。然而，目前大多数生物质分馏过程都面临着诸如碳水化合物组分（纤维素纤维和半纤维素糖）的不必要损失和木质素（芳香化合物）的显着结构变化等问题，这两者都会使分馏组分贬值。拟议的项目将开发一种使用醛磺酸的节能、廉价和保值的生物质分馏系统。拟议研究的成功将直接影响美国以木质纤维素为基础的生物炼制、纸浆和造纸工业以及其他相关行业。它还将通过替代石油原料和减少分馏过程中的能源消耗，为低碳生物经济做出贡献。该项目将通过研究生和本科生培训（特别是女性和少数民族学生）和课程开发，促进生物炼制、生物能源和生物产品（3B）领域的STEM教育。该项目还将包括与K-12学生的拓展活动，为对3B领域感兴趣的学生提供实验室参观，暑期实习和研究项目。提出的研究使用新型醛磺酸（含醛芳香磺酸）来完成木质纤维素生物质的快速和近乎完全的分馏，而不需要显著的生物质尺寸减少预处理。这一过程不仅最大限度地提高了纤维素、半纤维素和木质素的产量，而且与现有方法相比，它还降低了过程能耗。使用基于模型的分子设计方法，将通过磺化从廉价的含醛芳烃中合成具有可调结构，物理性质和反应性的醛磺酸。从机理上讲，醛磺酸通过磺酸基分解木质纤维素，然后通过与醛基的相互作用保护碳水化合物和木质素不被降解和缩合。由于其作为催化剂、溶剂和保鲜剂的多功能性质，醛磺酸有望在温和条件下迅速、几乎完全地将厘米级的木质纤维素原料分馏成可切割和可升级的木质素、纤维素和半纤维素。这项研究将验证一个中心假设，即在木质纤维素分馏中，醛磺酸将比目前的矿物/有机酸和醛的组合更有效、更有选择性。数学模型将使用定量结构-性能分析来预测一系列醛磺酸的结构特性和性能。通过这些模型研究，将从机理上阐明木质素和半纤维素的串联解聚和可逆保存，以了解酸不稳定键的裂解反应动力学和保护性化学基团的形成。该奖项反映了美国国家科学基金会的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。