GRK 2943: SPECtroscopic Tools for challenging REduction reactions - Catalytic coupling of CO2 (SPECTRE)

全球变暖是人类面临的最大挑战之一。我们迫切需要可持续的技术来避免和减少温室气体二氧化碳的演变。通过还原均偶联选择性地将二氧化碳转化为增值的多碳化合物，为将二氧化碳转化为具有碳中性足迹的化学能载体和产品提供了机会。CO2到草酸盐的还原偶联，代表了反应级联产生C2+产物的第一步，但尚未开发。在这个研究培训小组中，将开发新的有机金属、电催化和光催化途径，用于从CO2生成草酸盐。光谱学研究对于现代催化研究，特别是本文提出的方法具有极其重要的意义。它们提供了有关操作过程的重要信息，因此对其优化至关重要。Operando方法允许观察活性和失活的催化物质，与建模相结合，可以阐明途径和机制，并允许对催化系统进行洞察力驱动的优化。均相催化的最新发展以及诸如电催化或光催化等有抱负的学科的加入对应用光谱方法的时间和空间分辨率的实验能力提出了新的要求。在此，我们看到了耦合光谱技术的巨大应用潜力和进一步的新发展。因此，我们的目标是利用新的光谱，化学计量学和量子化学工具来开发和理解二氧化碳催化生成草酸盐的具有挑战性的模型反应，这将有利于现代催化研究。博士研究员将受益于一个跨学科的科学联盟，拥有实验和理论专业知识，在催化，分子化学，物理和理论化学，物理和数学之间的界面，在具有挑战性的科学背景下开发创新的化学方法。罗斯托克大学和莱布尼茨催化研究所的协同作用增强了该培训项目提供优秀的多学科教育。培训的重点是通过一个结构化的、联合的教育和个人发展计划，在多样化的、建设性的科学环境中培养学生的个人资格。特别措施包括参与实验室内外的短期和中期人员交流模块，以及定期研讨会和丰富外部访问科学家的参与。

Global warming is one of the greatest challenges facing humanity. Sustainable technologies to avoid and reduce the evolution of the greenhouse gas CO2 are urgently required. Selective conversion of CO2 into value-added multi-carbon compounds by reductive homocoupling offers the opportunity to convert CO2 into chemical energy carriers and products with a carbon neutral footprint. The reductive coupling of CO2 to oxalate, represents the first yet underdeveloped step of a reaction cascade yielding C2+ products. In this research training group, new organometallic, electrocatalytic and photocatalytic pathways for the formation of oxalate from CO2 will be developed. Spectroscopic studies are of utmost importance for modern catalysis research in general and for the approach proposed here in particular. They provide important information about the operating processes and are therefore essential for their optimisation. Operando methods allow the observation of reactive and deactivated catalytic species, which, in combination with modelling, enables the elucidation of pathways and mechanisms and allow for an insight-driven optimisation of catalytic systems. Recent developments in homogeneous catalysis as well as inclusion of aspiring disciplines such as electro- or photocatalysis place new demands on the experimental capabilities concerning time- and spatial-resolution of applied spectroscopic methods. Here we see great potential for the application and the further and new development of coupled spectroscopic techniques. Accordingly, we aim to harness new spectroscopic, chemometric and quantum chemical tools for the development and understanding of the challenging model reaction of the catalytic formation of oxalate from CO2, which will benefit modern catalysis research in general. The PhD fellows will benefit from an interdisciplinary scientific consortium with experimental and theoretical expertise to develop innovative chemical approaches in a challenging scientific context at the interface between catalysis, molecular chemistry, physical and theoretical chemistry, physics, and mathematics. The training program offers an excellent multidisciplinary education enhanced by the synergetic interaction of the University of Rostock and the Leibniz Institute for Catalysis. The focus of the training is on the individual qualification of the students through a structured, joint educational and personal development program in a diverse, constructive scientific environment. Special measures include both, short- and medium-term personnel exchange modules within and beyond the participating laboratories, as well as regular seminars and the enriching engagement of external visiting scientists.