Biocatalytic Activation of Macromolecular Building Blocks

更多地利用所有生物资源馏分对于振兴森林部门至关重要，森林部门在加拿大不断增长的生物经济和国家减少碳排放的承诺中发挥着核心作用。此外，抓住这一机会将实现加拿大供应全球生物产品市场的潜力，同时利用其在基础设施和生物资源利用和管理方面的专业知识方面的历史投资。***除了创新地使用可再生生物质原料外，生物经济还体现在更多地应用可持续的、生物催化的过程。事实上，微生物酶对于扩大植物源性生物质产品范围的重要性是公认的。然而，迄今为止，生物技术主要集中在微生物发酵或化学转化为商品燃料和化学品的生物资源的解构。虽然原糖和单脂醇衍生的产品对于捕获可再生植物生物质的全部潜力是必要的，但这些产品放弃了初始生物质资源的固有功能属性。***生物催化剂升级（而不是降解）生物聚合物化学的潜力提供了一种替代目前主导生物炼制概念的“解构重建”的做法。因此，拟议的项目将侧重于发现和应用酶系统，而不是用于木质纤维素解构的靶酶，这些酶系统可以激活未充分利用的半纤维素片段，允许它们重新组装成生物聚合物结构，从而捕获这一主要生物质部分的固有功能，从而产生生物基交联剂、表面涂层和流变改性剂。强调生物催化途径来激活构建块将有助于确保最终产物和合成途径都是可持续的，同时也利用生物催化方法提供的催化精度。为实现项目目标，将遵循以下四个综合步骤：1)生物信息学分析优先选择碳水化合物氧化酶和转氨酶，并为蛋白质工程策略提供信息；2)利用高通量和重组方法生产蛋白靶点；3)分离酶和反应产物的生化表征，以确定互补和兼容的酶系统；4)应用已建立的偶联途径，证明酶激活低聚物重新组装的潜力。除了加速基因组学研究在生物制品领域的应用之外，拟议的研究将推动无细胞生物催化级联的新兴趋势，并创造新的工具来促进从未充分利用的生物质馏分中设计和开发新型生物基材料。

Greater use of all bioresource fractions will be critical to an invigorated forest sector that plays a central role in Canada's growing bioeconomy and national commitments to reduced carbon emissions. Moreover, seizing this opportunity will realize Canada's potential to supply global bioproduct markets while capitalizing on its historical investment in infrastructure and know-how in bioresource use and management. ***In addition to innovative use of renewable biomass feedstocks, bio-economies are exemplified by increased application of sustainable, biologically catalyzed processes. Indeed, the importance of microbial enzymes to expanding the range of products that can be made from plant-derived biomass is well recognized. However, biotechnologies to date largely focus on the deconstruction of the bioresource for microbial fermentation or chemical conversion to commodity fuels and chemicals. While products derived from primary sugars and monolignols will be necessary for capturing the full potential of renewable plant biomass, these products relinquish the inherent functional attributes to the starting biomass resource. ***The potential of biocatalysts to upgrade (rather than degrade) biopolymer chemistries presents an alternative to the practice of “deconstruct to reconstruct” which dominates current biorefinery concepts. Accordingly, rather than target enzymes for lignocellulose deconstruction, the proposed program will focus on the discovery and application of enzyme systems that activate underused hemicellulose fragments, permitting their reassembly into biopolymer structures that capture the innate function of this major biomass fraction, leading to bio-based crosslinkers, surface coatings, and rheology modifiers. The emphasis on biocatalytic routes to activated building blocks will help ensure that both end-products and synthesis pathways are sustainable, while also harnessing the catalytic precision offered by a biocatalytic approach. The following four integrated steps will be followed to achieve the program goals: 1) bioinformatics analyses to prioritize carbohydrate oxidase and transaminase selections and inform protein engineering strategies; 2) production of protein targets using high-throughput and recombinant approaches; 3) biochemical characterization of isolated enzymes and reaction products to identify complementary and compatible enzyme systems, and 4) application of established coupling pathways to demonstrate the potential to re-assemble the enzymatically activated oligomers. In addition to accelerating the application of genomics research in the bioproducts sector, the proposed research will advance emerging trends in cell-free biocatalytic cascades, and create new tools to facilitate the design and development of novel bio-based materials from underused biomass fractions.