EAGER: Catalytic Transformation and Kinetics of Lignin-Carbohydrate Complexes

摘要智力价值：木质纤维素可以被认为是纤维素、半纤维素和木质素在空间和组成上的复杂混合物。在了解和控制纤维素和半纤维素的分解化学，将其组成的碳水化合物中间体上转化为乙醇、BTX、呋喃和其他化学物种方面取得了很大进展。相比之下，木质素的研究进展较少，木质素与纤维组分相互作用的研究进展较少。木质素与碳水化合物的结合对木质纤维生物质的利用提出了严峻的挑战。威廉·马什·赖斯大学的Michael Wong和Kior Inc.的Conrad Zhang的研究人员提出了一项为期一年的大学和工业公司合作研究计划，重点是不同饲料的木质素和纤维素构建单元之间的“界面”化学，并研究这种化学对热催化转化过程中的速率和产品分布的影响。与其他只关注木质素模型或纤维素分解产物的研究不同，该项目侧重于木质素-碳水化合物复合体(LCC)作为木质纤维素分解中间体的模型。据推测，木质纤维素的热解产生了LCCS作为化学中间体，其化学到目前为止还没有被解释。这项工作的目标是确定LCC的非均相催化转化途径和动力学，并建立一些通用的标准来设计可以控制LCC转化途径和动力学的催化材料。广泛的影响：由于全球对能源安全、全球变暖和可持续发展的关注，学术界和工业界对木质纤维素生物质作为一种可持续的燃料、化学品和能源产生了巨大的兴趣。人们正在研究将木质纤维素转化为更高价值产品的各种方法，其中催化转化为运输燃料和基础化学品是一个有希望的方向。木质纤维素中木质素和纤维素组分之间的“界面”性质未知，这给生物质的催化上转化带来了技术挑战。研究木质素碳水化合物复合体解决了这些挑战，潜在地降低了商业化改进的激活障碍。作为一所大学和一家公司之间的合作项目，该项目还将提供1名博士后研究助理的多学科培训，涉及化学动力学、多相催化和材料化学、最先进的分析技术和工业合作。博士后成员将根据明确的博士后指导计划接受指导和培训。

ABSTRACT Intellectual Merit: Lignocellulose can be thought as a spatially and compositionally complex mixture of cellulose, hemicellulose, and lignin. There has been great progress in understanding and controlling the breakdown chemistry of cellulose and hemicellulose, in the upconversion of their constituent carbohydrate intermediates into ethanol, BTX, furans, and other chemical species. In contrast, there is less progress on lignin and the effect of lignin interaction with cellulosic components during the process. The association of lignins with carbohydrates presents a serious challenge for the utilization of lignocellulosic biomass. This proposal from Investigators Michael Wong of William Marsh Rice University and Conrad Zhang of KiOR Inc. describes a one-year collaborative research plan between the university and industrial corporation that focuses on the "interface" chemistry between the building units of lignin and cellulose of different feeds, and to study the impact of this chemistry on the rate and product distribution profiles during a thermocatalytic conversion process. Unlike other studies which either focus solely on model lignin or cellulose breakdown products, this project focuses on lignin-carbohydrate complexes (LCCs) as a model of a lignocellulose breakdown intermediate. It is hypothesized that the pyrolytic decomposition of lignocellulose generates LCCs as a chemical intermediate, and its chemistry is, so far, not accounted for. The goals of this work are to determine the heterogeneously catalyzed transformation routes and kinetics of LCCs, and to establish some general criteria for designing catalytic materials that can control LCC transformation pathways and kinetics.Broader Impacts: The renewed academic and industrial interest in lignocellulosic biomass as a sustainable sourceof fuel, chemicals, and energy has been tremendous, in response to the worldwide concerns ofenergy security, global warming, and sustainable development. Various approaches to convert lignocellulose into higher-value products are being investigated, with catalytic conversion into transportation fuel and basic chemicals as a promising direction. The unknown nature of the "interface" between the lignin and cellulose fractions in lignocellulose presents technical challenges in the catalytic upconversion of biomass. Studying lignincarbohydrate complexes addresses these challenges, potentially lowering the activation barrier to improvements in commercialization. This project, as a collaboration between a university and a company, will also provide for the multidisciplinary training of 1 post-doctoral research associate in chemical kinetics, heterogeneous catalysis, and materials chemistry, state-of-the-art analytical techniques, and industrial collaborations. The post-doctoral member will receive guidance and training according to a well-defined postdoctoral mentoring plan.