计算化学所2024年催化反应与机制论坛
时间：2024年10月25日 9:00-12:00
地点：会议中心一层第二会议室
9:00-10:00
报告题目：Sustainability: Activation of Carbon Dioxide and Recycling of Noble Metals
报告人：Timo Repo 教授 芬兰赫尔辛基大学 芬兰科学与人文院院士
报告摘要：Green chemistry and syntheses in line with sustainable development are at the center of my research group at the University of Helsinki, and this presentation provides a brief background on the goals and recent challenges. The core focus of the research is on the catalytic activation of small molecules and, thus, their utilization in synthesis. Whereas we have extensively studied metal-free hydrogen activation and hydrogenation reactions with frustrated Lewis pairs (FLPs) and aerobic oxidation of alcohols, the recent focus has been on efficient methods to activate CO2 and it as a C1-building block. This opens attractive and sustainable pathways for the synthesis of highly valuable pharmaceuticals, chemicals, and materials on which our modern society is depending on. Heterocycles are attractive target compounds. For example, whereas cyclic carbonates are widely used as aprotic polar solvents and synthetic intermediates, 5-membered carbamates (2-oxazolidinones) find their importance in antibiotics. Recently, we have focused on the ability of superbases to activate CO2 effectively, which opens a general approach to synthesizing many biologically active molecules and even to capturing CO2 from the air (Direct air capture, DAC).
报告人简介：Timo Repo received his Ph.D. in 1997 from the University of Helsinki (Finland), where he was nominated as a full professor of inorganic chemistry in 2007. His research is focused on green chemistry and homogeneous catalysis, including catalyst development for the activation of small molecules (e.g., O2, CO2, H2), oxidation, reduction, C-H activation, biomass valorization, and dissolution of noble metals into organic solvents. He has been a member of the Finnish Academy of Science and Letters since 2017. Until now, he has published over 200 publications in high-impact scientific journals. He is currently a member of the Scientific Council for Natural Sciences and Engineering, Research Council of Finland, and an Adjunct professor in the Department of Chemistry at Hashemite University, Jordan.
10:00-11:00
报告题目：Frustrated Lewis Pairs for Transition Metal Free Hydroboration Catalysis and CO2 Activation
报告人：Petra Vasko 教授 芬兰赫尔辛基大学
报告摘要：Frustrated Lewis pairs (FLPs) consist of sterically hindered Lewis acid and base components that cannot readily form a traditional Lewis adduct. In this context, boron-based Lewis acids like B(C6F5) and various phosphine or amine moieties serve as common components. The FLP concept provides a unique method for metal-free small molecule activation, with emerging catalytic applications.For effective reactivity, it is crucial that the FLP's donor and acceptor sites do not directly bond but can polarize target chemical bonds to facilitate heterolytic cleavage. Challenges in utilizing FLPs as catalysts across different applications stem from high catalyst loadings and low turnover numbers.Our research focuses on fundamental transformations like hydroboration of alkynes using pinacolborane and reactions of germylene Lewis acid-based FLPs with CO2. This work combines experimental and computational methods to explore these topics. We delve into the mechanism of FLP-mediated hydroboration reactions of alkynes and introduce CO2 insertion reactions facilitated by a novel combination of cyclic (alkyl)(amino)carbene (cAAC) Lewis base and an amido-stabilized chlorogermylene Lewis acid.
报告人简介： Dr Petra Vasko obtained her PhD in 2015 from the University of Jyväskylä in Finland. Since then, she moved to the University of Oxford for 3 years to work as a postdoctoral researcher in the group of Prof. Simon Aldridge. Currently, she holds a position of an Academy Research Fellow and leads the main group chemistry research group at the University of Helsinki. Dr Vasko is conversant in both experimental and computational methods which allows for a comprehensive understanding of the studied systems. Her research focuses on the exploration of novel main group containing compounds that exhibit reactivity towards environmentally important small molecules. She is interested in the fundamental bonding properties of these species as well as reactivity, which could help in designing greener catalysts for the future. To date, Dr Vasko has published more than 40 articles in high impact scientific journals, and she has been awarded more than 1 M€ in research funding.
11:00-12:00
报告题目：Combining Chemical Theory and Machine Learning Techniques to Accelerate Chemical Discovery
报告人：Thijs Stuyver 教授 巴黎文理研究大学 (PSL University)
报告摘要：In this talk, Prof. Thijs Stuyver will highlight recent work from his research group, focusing on how they integrated automated reaction profiling with graph neural networks to screen over 5M cycloaddition reactions for bioorthogonal click potential, identifying over 100,000 plausible reactions. Additionally, he will discuss repurposing existing DFT descriptor datasets to create informative representations for reactivity predictions, demonstrating extreme data efficiency, particularly for hydrogen atom transfer reactions where they achieved accurate predictions with limited data. Lastly, he will present thier tool, TS-tools, for automated transition state localization, which performs well with a 95% success rate on mono- and bimolecular pathways at the xTB level. For tri- and multi-molecular pathways, though DFT becomes essential, TS-tools maintains its effectiveness in various chemical processes, including solvent, auto-, and enzyme catalysis.
报告人简介：Thijs Stuyver is a professor at ENSCP-PSL University, specializing in machine learning, artificial intelligence, and chemical reactivity. With a PhD in Chemistry from the Vrije Universiteit Brussel, his research focuses on applying computational techniques like valence bond theory and density functional theory to predict and understand chemical reactions. He has led several research projects funded by organizations like the European Commission and the Swiss Federal Commission for Scholarships for Foreign Students, and his work has resulted in 48 peer-reviewed publications, including notable contributions in journals like the JACS. and Nat. Commun. He is also actively involved in developing new computational methods for reaction discovery and design, leveraging the power of machine learning to accelerate the development of new chemical processes.