Upgrading Biomass Using In Silico Designed Ionic Liquids

拟议的工作将开发使用离子液体解构和升级木质纤维素生物质的综合工艺，这些离子液体经过计算设计，具有功能和环境友好性。尽管在为生产液体运输燃料和化学品而进行的木质纤维素生物质增值研究方面做出了重大努力，但仍然缺乏经济上可行和有效的工艺。拟议的研究项目将结合最先进的计算方法与合成和过程化学，迭代设计新型离子液体，使木质纤维素中含有的生物聚合物直接转化为小分子构建块（平台）化学品。最终目标是开发一种系统的方法来计算设计用于木质纤维素加工的特定任务的离子液体，以优化其功能和环境性能。离子液体是“设计”溶剂，可以调整以促进木质纤维素生物质加工的关键步骤。由于三个原因，它们的潜力尚未实现：i)同时优化必须满足工业使用的众多物理化学性质和反应性指标的挑战；Ii)许多离子液体的环境毒性；iii)与传统溶剂相比，成本显著提高。虽然计算方法被应用于识别具有特定功能的离子液体，如纤维素的溶解和脱晶，但它们并没有被用于迭代设计新的离子液体，以同时优化多个性能标准。此外，几乎没有系统设计的离子液体具有最小的毒性和高生物降解性。该研究旨在开发数据驱动的计算方法，以功能和生物作用机制的见解为指导，有效地为具有理想功效和降低人类和环境毒性的新il的设计提供信息。这项工作如果成功，可能会导致更安全的离子液体的开发，可用于生物质加工和基于功能优化的特定任务离子液体的下一代生物质升级工艺。如果研究成功，将对农村地区的环境可持续性和经济发展产生重要的社会影响。除了培养研究生的研究能力外，研究小组还计划为化学专业的学生开设一门毒理学课程，并在乔治华盛顿大学开设一个新的环境与绿色化学硕士课程。该项目将涉及与绿色和可持续化学相关的推广活动，旨在促进STEM教育，包括在乔治华盛顿大学举办的绿色化学、公共卫生和科学政策论坛，以及对有意将绿色化学概念纳入其课程的当地高中教师进行指导。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。

The proposed work will develop integrated processes for deconstruction and upgrading of lignocellulosic biomass using ionic liquids that are computationally designed to be functional and environmentally benign. Despite significant efforts in research aimed at valorization of lignocellulosic biomass for producing liquid transportation fuels and chemicals, economically-viable and efficient processes are still lacking. The proposed research project will combine state-of-the-art computational methodology with synthetic and process chemistry to iteratively design novel ionic liquids to enable direct conversion of the biopolymers contained in lignocellulose to small-molecule building-block (platform) chemicals. The ultimate objective is the development of a systematic approach for computational design of task-specific ionic liquids for lignocellulose processing that are optimized for function and environmental performance.Ionic liquids are 'designer' solvents that can be tuned to facilitate key steps of lignocellulosic biomass processing. Their potential has not materialized for three reasons: i) challenges in simultaneously optimizing numerous physicochemical properties and reactivity metrics that must be met for industrial use; ii) environmental toxicity of many ionic liquids; and iii) significantly higher cost compared to conventional solvents. Although computational methods are being applied to identify ILs with specific functions, such as dissolution and de-crystallization of cellulose, they are not used to iteratively design new ionic liquids with the goal of simultaneously optimizing multiple performance criteria. Furthermore, there is little to no systemic design of ionic liquids with minimal toxicity and high biodegradability. The proposed research aims to develop data-driven computational approaches, guided by insights from mechanism of function and biological action, to effectively inform the design of new ILs with desirable efficacy and reduced potential for human and environmental toxicity. The proposed work, if successful, may lead to the development of safer ionic liquids that can be used in biomass processing and next-generation processes for biomass upgrading based on task-specific ionic liquids optimized for function. The proposed research, if successful, can have important societal impact related to environmental sustainability and economic development of rural areas. In addition to training graduate students in research, the research team plans to develop a toxicology coursework for chemistry students and a new MS program in Environmental and Green Chemistry at George Washington University. The project will involve outreach activities related to green and sustainable chemistry aiming to promote STEM education, including a Green Chemistry, Public Health and Science Policy forum at George Washington University and mentoring of local high school teachers interested in integrating Green Chemistry concepts into their curricula.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.