Harnessing Bioluminescent Bacteria to Power Photochemical Transformations

利用光能促进化学反应是当前研究中最活跃、最多才多艺的领域之一。特别是，可见光催化允许特定分子的选择性激发，然后该分子能够与试剂进行能量或电子转移。这是一种有效的策略，可以以高度选择性的方式形成催化量的高活性中间体，如自由基或卡宾。使用这种方法已经产生了大量的新反应和新分子。然而，尽管它在学术和工业实验室中得到了广泛的应用，但它在大规模多吨反应中的应用尚未实现。由于许多光化学方法的可扩展性较差，这一点是合理的。归因于此的主要因素是光的衰减，正如比尔-兰伯特定律所描述的那样。简单地增加反应的规模将大大减少其表面积，随着容器内光强度的指数下降，大部分能量被浪费。在这个项目中，我们试图利用生物发光细菌作为光子源来进行光化学转化。重要的是，一系列荧光蛋白质、发光海洋微生物和土壤微生物随处可得；因此，可以获得各种波长的可见光。最初的研究将集中在使用化学光氧化还原反应获得概念验证，重点是生物相容性。除了使用现代合成生物学方法来调节生物发光的强度和波长外，我们还将评估有机体对光化学中间体存在的生物反应(通过转录)，以创建一种模块化的遗传方法，为一系列光化学反应的细胞产生光。总体而言，这一战略的成功实施将为在不使用高功率光源的情况下为光化学转化提供动力提供一种新的方法。这种能源密集度较低的方法将通过降低成本和有害排放，帮助在制造规模上采用这些反应。

The use of light energy to promote chemical reactions is one of the most vibrant and versatile areas of current research. In particular, visible light photocatalysis allows for the selective excitation of a specific molecule, which is then able to undergo energy or electron transfer with a reagent. This is a powerful strategy to form catalytic quantities of highly reactive intermediates, such as radicals or carbenes, in a highly selective manner. A vast array of novel reactions and new molecules have been generated using this approach. However, despite its widespread use in academic and industrial labs its application in large-scale multi-tonne reactions has not been realised. This can be rationalised by the poor scalability of many photochemical methods. The main factor attributed to this is the attenuation of light as described by the Beer-Lambert law. Simply increasing the scale of a reaction will drastically reduce its surface area and with light intensity decreasing exponentially within the vessel much of this energy is wasted. In this project, we seek to utilise bioluminescent bacteria as a photon source to conduct photochemical transformations. Importantly, a range of fluorescent proteins, luminescent marine and soil microorganisms are readily available; therefore, providing access to a variety of wavelengths of visible light. Initial studies will focus on obtaining proof-of-concept using a chemical photoredox reaction with a focus on biocompatibility. We will assess the biological response of the organism to the presence of photochemical intermediates (via transcriptomics) in addition to using modern synthetic biology approaches to tune the intensity and wavelength of the bioluminescence to create a modular, genetic approach to the cellular generation of light for a range of photochemical reactions. Overall, the successful implementation of this strategy will offer a new method for powering photochemical transformations without a high-powered light source. This less energy intensive approach will assist the adoption of these reactions on manufacturing scales by cutting both costs and harmful emissions.