EAGER: Catalytic Transformation and Kinetics of Lignin-Carbohydrate Complexes

摘要：木质纤维素是纤维素、半纤维素和木质素在空间和组成上复杂的混合物。在理解和控制纤维素和半纤维素的分解化学方面，在它们的组成碳水化合物中间体向上转化为乙醇、BTX、呋喃和其他化学物质方面，已经有了很大的进展。相比之下，在木质素和木质素与纤维素组分在该过程中的相互作用的影响方面的进展较少。木质素与碳水化合物的结合对木质纤维素生物质的利用提出了严峻的挑战。威廉·马什·赖斯大学的研究人员迈克尔·王和KiOR公司的康拉德·张提出了这一建议。描述了一个为期一年的大学和工业公司之间的合作研究计划，重点是“界面”之间的化学结构单元的木质素和纤维素的不同饲料，并研究这种化学的影响，在热催化转化过程中的速率和产品分布曲线。与其他研究，无论是只集中在模型木质素或纤维素分解产物，这个项目的重点是木质素-碳水化合物复合物（LCC）作为一个模型的木质纤维素分解中间体。据推测，木质纤维素的热解分解产生LCC作为化学中间体，其化学是，到目前为止，不占。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，并建立一些设计催化材料的一般标准，这些催化材料可以控制LCC的转化途径和动力学。木质纤维素生物质作为可持续的燃料、化学品和能源的新的学术和工业兴趣是巨大的，以响应世界范围内对能源安全的关注，全球变暖和可持续发展。将木质纤维素转化为高价值产品的各种方法正在研究中，催化转化为运输燃料和基本化学品是一个有前途的方向。木质纤维素中的木质素和纤维素级分之间的“界面”的未知性质在生物质的催化上转化中提出了技术挑战。研究木质素水合物复合物解决了这些挑战，可能降低商业化改进的活化障碍。该项目作为一所大学和一家公司之间的合作，还将为1名博士后研究助理提供化学动力学，多相催化和材料化学，最先进的分析技术和工业合作方面的多学科培训。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.