Power to value-added products via electro-biotechnology: Production of bulk chemicals by combining electrochemical and biocatalytic steps in “one-pot” with “green” electricity

通过电子生物技术为增值产品提供动力：通过将电化学和生物催化步骤与“绿色”电力相结合来生产大宗化学品

• 批准号: 536444156
• 负责人: Professor Dr. Harald Gröger
• 金额: --
• 依托单位: Arbeitsgruppe Organische Chemie I
• 依托单位国家: 德国
• 项目类别: Priority Programmes
• 资助国家: 德国
• 项目状态: 未结题
• 来源: https://gepris.dfg.de/gepris/projekt/536444156?language=en
• 关键词: Power; value; added; products; via

By bridging the expertises in electrochemistry (Schäfer group, Osnabrück University) and biocatalysis (Gröger group, Bielefeld University), this tandem project centers on the development of a novel type of chemoenzymatic one-pot cascade process technology consisting of an electrochemical functionalization of an organic molecule, followed by an enzyme-catalyzed step in which the intermediate is then converted into the final desired target molecule. Such types of combinations of electrochemistry and biotechnology will enable “formal” access to so-called “dream reactions”, defined as chemical transformations, for which no (single) catalyst exists yet. For instance, in this project a direct one-pot amination of (substituted) toluenes under formation of (substituted) benzylamines will be addressed. Taking advantage of utilizing solely O2 (from air) and ammonia, such a sustainable process technology would be also highly attractive for future applications in bioeconomy in terms of novel manufacturing routes for value-added bulk chemicals and power-to-product processes. Such a one-pot cascade strategy is based on an initial electrochemical oxidation of toluene(s) leading to benzaldehyde(s) and subsequent enzymatic reductive amination under formation of benzylamines. It is noteworthy that as a second electrochemical step, reduction of the in situ-formed oxidative form of the cofactor, NAD+, thus regenerating the cofactor NADH being needed for the enzymatic reductive amination, will be conducted. Thus, for this process only O2 and NH3 are needed as reagents and “green energy” (solar energy, wind energy). A challenge, however, will be to realize the individual steps preferably in water as well as to achieve compatibility of these steps.

通过将电化学(Schäfer组，奥斯纳布吕克大学)和生物催化(Gröger组，比勒费尔德大学)方面的专家联系起来，这个串联项目集中于开发一种新型的化学酶一锅级联工艺技术，包括有机分子的电化学官能化，然后是酶催化步骤，在该步骤中中间体被转化为最终所需的目标分子。这种类型的电化学和生物技术的结合将使“正式”获得所谓的“梦幻反应”，这种反应被定义为化学转化，目前还不存在(单一的)催化剂。例如，在这个项目中，将讨论(取代的)甲苯在生成(取代的)苄胺的情况下的直接一锅胺化反应。利用仅利用氧气(来自空气)和氨的优势，这种可持续的工艺技术也将在未来的生物经济应用中具有极大的吸引力，因为它可以为增值的大宗化学品和电力到产品的工艺提供新的制造路线。这种一锅串联的策略是基于甲苯(S)最初的电化学氧化生成苯甲醛(S)，然后在生成苯甲胺的情况下进行酶还原胺化。值得注意的是，作为第二个电化学步骤，将进行辅因子NAD+的原位形成的氧化形式的还原，从而再生酶还原胺化所需的辅因子NADH。因此，这个过程只需要O2和NH3作为试剂和“绿色能源”(太阳能、风能)。然而，一个挑战将是实现单独的步骤，最好是在水中，以及实现这些步骤的兼容性。