Upgrading Biomass Using In Silico Designed Ionic Liquids

使用计算机设计的离子液体升级生物质

• 批准号: 1805080
• 负责人: Jakub Kostal
• 金额: $ 30万
• 依托单位: George Washington University
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2018
• 资助国家: 美国
• 起止时间: 2018-09-15 至 2022-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1805080&HistoricalAwards=false
• 关键词: Upgrading; Biomass; Using; Silico; Designed

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.

拟议的工作将开发使用离子液体的木质纤维素生物质的解构和升级的综合过程，这些离子液体在计算上被设计为功能性的和环境友好的。尽管在旨在使用于生产液体运输燃料和化学品的木质纤维素生物质增值的研究中做出了重大努力，但仍然缺乏经济上可行且有效的方法。 拟议的研究项目将联合收割机结合最先进的计算方法与合成和工艺化学，迭代设计新型离子液体，使木质纤维素中所含的生物聚合物直接转化为小分子积木（平台）化学品。最终目标是开发一种系统的方法，用于计算设计用于木质纤维素加工的特定任务的离子液体，其针对功能和环境性能进行优化。离子液体是“设计师”溶剂，可以进行调整以促进木质纤维素生物质加工的关键步骤。由于以下三个原因，它们的潜力尚未实现：i）同时优化工业用途必须满足的许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;以及iii）与常规溶剂相比显著更高的成本。虽然计算方法被应用于识别具有特定功能的离子液体，例如纤维素的溶解和去结晶，但它们并不用于迭代设计新的离子液体，其目标是同时优化多个性能标准。此外，几乎没有具有最小毒性和高生物降解性的离子液体的系统设计。拟议的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，有效地为新IL的设计提供信息，这些IL具有理想的功效，并降低了对人类和环境的毒性。拟议的工作，如果成功的话，可能会导致更安全的离子液体的发展，可用于生物质加工和下一代生物质升级工艺的基础上，任务特定的离子液体优化功能。拟议的研究如果成功，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。除了培训研究生的研究，研究小组计划开发一个毒理学课程的化学学生和一个新的MS程序在环境和绿色化学在乔治华盛顿大学。该项目将涉及与绿色和可持续化学有关的外联活动，旨在促进STEM教育，包括一个绿色化学，乔治华盛顿大学的公共卫生和科学政策论坛，并指导有兴趣将绿色化学概念融入其课程的当地高中教师。该奖项反映了NSF的法定使命，并被认为值得通过使用基金会的知识产权进行评估来支持。优点和更广泛的影响审查标准。

项目成果

Microwave‐Assisted Decarbonylation of Biomass‐Derived Aldehydes using Pd‐Doped Hydrotalcites

使用 Pd 掺杂水滑石进行微波辅助生物质脱羰基衍生醛

• DOI: 10.1002/cssc.201901934
• 发表时间: 2019
• 期刊: ChemSusChem
• 影响因子: 8.4
• 作者: An, Nan;Ainembabazi, Diana;Reid, Christopher;Samudrala, Kavya;Wilson, Karen;Lee, Adam F.;Voutchkova‐Kostal, Adelina
• 通讯作者: Voutchkova‐Kostal, Adelina

Going All In: A Strategic Investment in In Silico Toxicology

• DOI: 10.1021/acs.chemrestox.9b00497
• 发表时间: 2020-04-20
• 期刊: CHEMICAL RESEARCH IN TOXICOLOGY
• 影响因子: 4.1
• 作者: Kostal, Jakub;Voutchkova-Kostal, Adelina
• 通讯作者: Voutchkova-Kostal, Adelina

Selective Lignin Depolymerization via Transfer Hydrogenolysis Using Hydrotalcite Supported Palladium – Model Compounds to Application

使用水滑石负载钯通过转移氢解选择性木质素解聚 — 模型化合物应用

• 发表时间: 2022
• 期刊: ChemRxiv
• 作者: Darren Dolan, Rebekah Brucato

Quantifying Uncertainty in Ecotoxicological Risk Assessment: MUST, a Modular Uncertainty Scoring Tool

• DOI: 10.1021/acs.est.0c02224
• 发表时间: 2020-10-06
• 期刊: ENVIRONMENTAL SCIENCE & TECHNOLOGY
• 影响因子: 11.4
• 作者: Kostal, Jakub;Plugge, Hans;Raderman, Will
• 通讯作者: Raderman, Will

Multifunctional Catalysts for Direct Conversion of Alcohols to Long-Chain Hydrocarbons via Deoxygenative Olefination

• DOI: 10.1021/acssuschemeng.1c05436.s001
• 发表时间: 2021-10
• 期刊: ACS Sustainable Chemistry & Engineering
• 影响因子: 8.4
• 作者: D. Ainembabazi;J. Horlyck;D. Dolan;M. Finn;A. Lee;K. Wilson;A. Voutchkova-Kostal