Light-driven CO 2 reduction with a heptacoordinated iron(ii) polypyridine complex F. Droghetti 1 , A. Ruggi 2 , F. Lemken 3 , L. Rulíšek 3 , M. Natali 1 1 University of Ferrara, Italy, 2 University of Fribourg, Switzerland, 3 Institute of Organic Chemistry and Biochemistry of the CAS, Czech Republic The growing necessity to mitigate human-induced CO 2 emissions has driven research toward innovative approaches for converting them into value-added products. Recent findings in designing molecular catalysts for the CO 2 reduction reaction (CO 2 RR) have focused on metal complexes with ligands that exhibit a significant degree of electronic delocalization, a feature crucial for reducing overpotential and enhancing selectivity over the competitive hydrogen evolution reaction (HER) [1,2] . In this communication, we report the catalytic activity of a Fe(II)-based molecular catalyst for CO 2 reduction, featuring a hexadentate, redox-active DBPy-PyA ligand (1-([2,2’-bipyridin]-6-yl)-N-([2,2’-bipyridin]-6-ylmethyl)- N-(pyridin-2-ylmethyl)-methanamine), under electrochemical and photochemical conditions. We optimize the catalytic performance of the Fe(II) complex through a fine-tuning of the proton donor, photon flux, and different photosensitizers, achieving over 99% selectivity and one of the highest reported quantum efficiencies [3] . Furthermore, time-resolved spectroscopy and DFT calculations provide a mechanistic understanding of electrochemical and photochemical behavior [4,5] . References 1. H. Takeda, C. Cometto, O. Ishitani, M. Robert, ACS Catal 2017 , 7 , 70–88. 2. F. Droghetti, A. Amati, A. Ruggi, M. Natali, ChemComm 2023 , 60 , 658–673. 3. F. Droghetti, L. Villa, A. Sartorel, L. Dell’Amico, A. Ruggi, M. Natali, ChemSusChem 2025 , DOI 10.1002/cssc.202402627. 4. F. Droghetti, F. Lemken, L. Rulíšek, A. Ruggi, M. Natali, ACS Catal 2024 , 16920–16935. 5. F. Droghetti, A. Amati, F. Pascale, A. Crochet, M. Pastore, A. Ruggi, M. Natali, ChemSusChem 2024 , 17 , DOI 10.1002/ cssc.202300737.
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