Integrating Metabolic Engineering and Heterogeneous Chemocatalysis: New Opportunities for Biomass to Chemicals
Integrating Metabolic Engineering and Heterogeneous Chemocatalysis: New Opportunities for Biomass to Chemicals
复制标题
DOI：
10.1002/chin.201629286
复制
发表时间：
2016-06
期刊：
影响因子：
--
通讯作者：
Yanping Huo;H. Zeng;Yugen Zhang
中科院分区：
文献类型：
--
作者：
Yanping Huo;H. Zeng;Yugen Zhang
在不断节能降耗的要求下，追求高台阶经济性和原子经济性是化学合成中一个永无止境的过程。[1]近年来，生物催化与化学催化的结合得到了广泛的应用。[2，3]将各个反应步骤合并到一锅中，即使来自相同类型的技术，如化学催化或生物催化，在节省溶剂，能源，时间和空间以及减少废物产生方面具有巨大潜力。[3，4]因此，来自不同领域的反应步骤的整合将在揭示新的机会和实现具有挑战性的任务方面更具吸引力。在生物催化中，反应由酶和工程代谢过程催化，这些过程通常在低浓度的水中进行。该系统通常会从发酵中产生生物杂质。使用有机催化剂或金属催化剂的化学催化通常在有时可能对杂质敏感的各种溶剂和催化剂中进行。结合生物催化和化学催化的一个主要挑战在于两个系统的相容性，包括反应条件、转化率和选择性。[4，5]虽然Bekkum小组在1980年报道了该主题的开创性工作，说明了与D-葡萄糖的酶促异构化偶联的非均相金属催化氢化用于合成D-甘露醇，但令人惊讶的是，该策略直到最近才应用于生物质转化。[6]生物质和衍生物通常是具有高氧含量的高度官能化的底物。将生物质升级为燃料和化学品通常从降低其氧含量开始，这在使用化学催化时通常具有较少的结构通用性。[7]或者，在生物催化（特别是代谢过程）中，生物质及其衍生物在许多自然过程中充当底物和/或营养物。可以生产具有不同碳链结构和不同官能度的各种产物。[8]代谢工程与非均相化学催化相结合的策略，
Driven by the constant energy-and resource-saving demand, pursuing high step-and atom-economy is an endless process in chemical synthesis.[1] Recently, several comprehensive reviews involving the combination of biocatalysis and chemocatalysis were published.[2, 3] Combining individual reaction steps into one pot, even from the same type of technology such as chemocatalysis or biocatalysis, has great potential in terms of saving solvent, energy, time and space, as well as reducing waste production.[3, 4] The integration of reaction steps from different fields will hence be more attractive in unveiling new opportunities and achieving challenging tasks. In biocatalysis, reactions are catalyzed by enzymes and engineered metabolic processes that are typically carried out in water at low concentrations. This system would typically generate biogenic impurities from fermentation. Chemocatalysis using organo-or metal catalysts is generally carried out in various solvents and catalysts that may sometimes be sensitive to impurities. One major challenge in combining biocatalysis and chemocatalysis lies in the compatibility of the two systems, including reaction conditions, conversions, and selectivities.[4, 5] Although the groundbreaking pioneering work in this topic was reported by the Bekkum group in 1980 illustrating a heterogenized metal-catalyzed hydrogenation coupled with an enzymatic isomerization of D-glucose for the synthesis of D-mannitol, surprisingly this strategy has not been applied to biomass transformation until very recently.[6]Biomass and derivatives generally are highly functionalized substrates with high oxygen content. Upgrading biomass to fuel and chemicals generally starts with reducing its oxygen content, which often has less structure versatility when using chemocatalysis.[7] Alternatively, in biocatalysis (especially metabolic processes) biomass and its derivatives serve as substrates and/or nutrition in many natural processes. Various products with different carbon chain structures and different functionalities could be produced.[8] The strategy of combining metabolic engineering and heterogeneous chemocatalysis is particularly