Collaborative Research: Towards a Generalized Microkinetic Description of Lignin Liquefaction

合作研究：木质素液化的广义微动力学描述

• 批准号: 1926412
• 负责人: Linda Broadbelt
• 金额: $ 19万
• 依托单位: Northwestern University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2019
• 资助国家: 美国
• 起止时间: 2019-08-15 至 2022-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1926412&HistoricalAwards=false
• 关键词: Collaborative; Research; Towards; Generalized; Microkinetic

Lignin is an abundant natural resource whose higher carbon content, when compared to cellulose and hemicellulose, makes it a very attractive renewable feedstock for producing fuels and chemicals. Lignin liquefaction is a promising process for converting this underutilized resource into monomeric phenols that can be easily upgraded to fuels and chemicals, but the underlying chemical kinetic processes are not well understood. This collaborative research project aims to develop a rational framework that integrates modelling and experimental tools to explicitly account for lignin and its oligomeric intermediate chemical structures at relevant liquefaction conditions in the presence or absence of solvents.Lignin liquefaction can be conducted in aqueous environments (hydrothermal liquefaction), in organic solvents (solvolysis), in ionic liquids or in solvent free conditions (pyrolysis). Assigning a realistic chemical formula to lignin and its oligomeric intermediates is one of the major challenges to rationally describe and control lignin liquefaction reactions. The mechanisms by which solvents and additives impact liquefaction reactions are also poorly understood. Because of this, lignin liquefaction remains an art rather than a science. The main goal of this project is to develop a rational micro-kinetic framework based on detailed micro-kinetic models describing depolymerization and repolymerization reactions and intermediate products removal mechanisms during lignin liquefaction. The practical goal is to use this mathematical model and experimental tools to identify suitable lignin liquefaction strategies in the presence of solvents and acid-base catalysts to maximize mono-phenol production which will facilitate further bio-oil upgrading in existing infrastructure. In addition to training two graduate students the principal investigators plan to host female and underrepresented minority high school students in their laboratories as summer research interns through the Summer Research Opportunity Program at Northwestern University and the Pacific Northwest Louis Stokes Alliance for Minority Participation.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.

木质素是一种丰富的自然资源，与纤维素和半纤维素相比，其碳含量较高，使其成为生产燃料和化学品的非常有吸引力的可再生原料。木质素液化是一种很有前途的工艺，可以将这种未充分利用的资源转化为单体酚，可以轻松升级为燃料和化学品，但其潜在的化学动力学过程尚不清楚。该合作研究项目旨在开发一个整合建模和实验工具的合理框架，以明确解释在存在或不存在溶剂的相关液化条件下木质素及其低聚中间体化学结构。木质素液化可以在水性环境中进行（水热液化） ）、有机溶剂（溶剂分解）、离子液体或无溶剂条件（热解）。为木质素及其低聚中间体指定一个现实的化学式是合理描述和控制木质素液化反应的主要挑战之一。溶剂和添加剂影响液化反应的机制也知之甚少。正因为如此，木质素液化仍然是一门艺术而不是一门科学。该项目的主要目标是基于描述木质素液化过程中解聚和再聚合反应以及中间产物去除机制的详细微观动力学模型，开发合理的微观动力学框架。实际目标是利用这种数学模型和实验工具来确定在溶剂和酸碱催化剂存在下合适的木质素液化策略，以最大限度地提高单酚产量，从而促进现有基础设施的进一步生物油升级。除了培训两名研究生外，主要研究人员还计划通过西北大学和太平洋西北路易斯斯托克斯少数族裔参与联盟的暑期研究机会计划，在实验室接待女性和代表性不足的少数族裔高中生作为暑期研究实习生。该奖项反映了通过使用基金会的智力价值和更广泛的影响审查标准进行评估，NSF 的法定使命被认为值得支持。

项目成果

Progress in Modeling of Biomass Fast Pyrolysis: A Review

生物质快速热解建模进展：综述

• DOI: 10.1021/acs.energyfuels.0c02295
• 发表时间: 2020-09-11
• 期刊: Energy & Fuels
• 影响因子: 5.3
• 作者: Pavlo Kostetskyy;L. Broadbelt
• 通讯作者: L. Broadbelt

A Review on Lignin Liquefaction: Advanced Characterization of Structure and Microkinetic Modeling

木质素液化综述：结构和微动力学建模的高级表征

• DOI: 10.1021/acs.iecr.9b05744
• 发表时间: 2020-01-15
• 期刊: Industrial & Engineering Chemistry Research
• 影响因子: 4.2
• 作者: Evan Terrell;Lauren D. Dellon;A. Dufour;Erika Bartolomei;L. Broadbelt;M. García
• 通讯作者: M. García