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Catalysts for Asymmetric Reactivity of Alcohols as Electrophiles: A Career Integration Project

Final Report Summary - CAR-CHASE (Catalysts for Asymmetric Reactivity of Alcohols as Electrophiles: A Career Integration Project)

Summary of the Performed Research: Catalyst discovery is a complex multidimensional problem that often requires extensive experimentation to obtain a lead result. Creative screening approaches and high throughput experimentation help accelerate lead hit identification, but the large number of experiments required to explore multiple reaction parameters still poses a daunting challenge. This project allowed our lab to engage in efforts to harness complex mixtures of in situ generated catalysts. We have developed a combinatorial discovery strategy in which complex mixtures of precatalysts and ligands are screened against other reaction parameters to rapidly identify lead conditions. Iterative deconvolution of the resulting hits identifies which components contribute to the lead in situ generated catalyst. Proof of principle of this approach was demonstrated by uncovering new catalytic conditions for reactions catalyzed by boron and nickel. Mechanistic investigations into the “hits” obtained from this process were then leveraged to develop second-generation transformations. We were particularly successful in developing catalysts for the direct use of alcohols in dehydrative C-C bond-forming reactions with water as the only product, a set of reactions that are of interest for sustainable chemical synthesis. More generally, we have demonstrated that taking a “systems” approach to catalysis for organic synthesis can be an effective way to rapidly discover new reactivity, new mechanistically interesting cooperative effects and to uncover catalysts that are mutually compatible for use in one-pot sequences of catalytic transformations (multi-catalysis). This work has led to 9 publications, several of which are in high-profile journals.

Integration and Transfer of Knowledge: I have integrated into and transferred knowledge to the scientific community at Strasbourg by starting collaborations with several groups, including those of Profs. Thomas Ebbesen, Paolo Samori and Marco Cecchini. Two of these have already led to publications in new areas for my group. I also organized the seminar series for ISIS from 2013-2015. I have integrated into the community by teaching two courses at the Master’s level each year. I am a council member of the University’s Doctoral School of Chemical Science (EDSC) since March 2014. I organized the ‘Themed Afternoon Symposium’ (AMT du EDSC), September 23, 2014 for PhD students. I obtained the Habilitation to Direct Research (HDR) on September 23, 2014 and am thus officially able to supervise PhD theses in Europe. In 2016, I led an effort to establish a new international Master’s program in Supramolecular Chemistry funded by the Erasmus program.

Career Development: Since taking up the Career Integration Grant in 2013, I have established a scientifically and financially independent research group at UNISTRA, which currently consists of 4 PhD students, 2 postdoctoral fellows, and 3 Master’s students. My level of research training and competence has increased with respect to project management, mentorship, grantsmanship and ability to write scientific papers. Since obtaining the Marie Curie CIG grant in 2013, I have obtained an ERC Starting Grant (2015-2020), four local LabEx grants, 1 Alsace Region PhD fellowship, and been the “scientist in charge” for two incoming externally funded postdoctoral fellows (1 Marie Curie IEF fellow and 1 Leverhulme Trust fellow). Furthermore, I have participated in 1 COST action. Since 2013, I have given over 20 invited talks or conference presentations at European, North American and Asian universities or research institutions. These have allowed me to integrate into the European research community, though I still hold a temporary position at UNISTRA. After receiving offers for professorships from other European universities in March 2016, I was convinced to stay at UNISTRA by senior colleagues who promised that a competition for a permanent position would be launched with a strong expectation of success. As of April 2017, no such competition has been launched, though I am assured the process is ongoing.