Converting CO2 to formic acid by tuning quantum states in metal chalcogenide clusters

• Published in: Communications chemistry 2023-03, Vol.6 (1), p.53-53, Article 53
• Main Authors: Sengupta, Turbasu, Khanna, Shiv N.
• Format: Article
• Language: English
• Subjects: 639/301/1034/1038; 639/638/563/934; 639/638/77/885; 639/925/357/995; Carbon dioxide; Catalysts; Catalytic converters; Chalcogenides; Chemistry; Chemistry and Materials Science; Chemistry/Food Science; Clusters; Conversion; Density functional theory; First principles; Formic acid; Hydrogenation; Ligands; Mathematical analysis
• ISSN: 2399-3669; 2399-3669
• DOI: 10.1038/s42004-023-00851-3

The catalytic conversion of CO 2 into valuable chemicals is an effective strategy for reducing its adverse impact on the environment. In this work, the formation of formic acid via CO 2 hydrogenation on bare and ligated Ti 6 Se 8 clusters is investigated with gradient-corrected density functional theory. It is shown that attaching suitable ligands (i.e., PMe 3 , CO) to a metal-chalcogenide cluster transforms it into an effective donor/acceptor enabling it to serve as an efficient catalyst. Furthermore, by controlling the ratio of the attached donor/acceptor ligands, it is possible to predictably alter the barrier heights of the CO 2 hydrogenation reaction and, thereby, the rate of CO 2 conversion. Our calculation further reveals that by using this strategy, the barrier heights of CO 2 hydrogenation can be reduced to ~0.12 eV or possibly even lower, providing unique opportunities to control the reaction rates by using different combinations of donor/acceptor ligands. Finding an efficient catalyst to convert CO 2 into useful products is a challenging problem. Here, the authors use first-principles calculations to show how the attached donor/acceptor ligands on the Ti 6 Se 8 cluster can be utilized to design effective catalysts for CO 2 hydrogenation to formic acid.