Affiliation:
1. State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing 211816, China
Abstract
In 2022, Beller and coworkers achieved the reversible hydrogenation of CO2 to formic acid using a Mn(I)–PN5P complex with excellent activity and reusability of the catalyst. To understand the detailed mechanism for the reversible hydrogen release–storage process, especially the effects of the transition metal center in this process, we employed DFT calculations according to which Ru(II) and Fe(II) are considered as two alternatives to the Mn(I) center. Our computational results showed that the production of formic acid from CO2 hydrogenation is not thermodynamically favorable. The reversible hydrogen release–storage process actually occurs between CO2/H2 and formate rather than formic acid. Moreover, Mn(I) might not be a unique active metal for the reversible hydrogenation of CO2 to formate; Ru(II) would be a better option.
Funder
National Natural Science Foundation of China
Project for Priority Academic Program Development of Jiangsu Higher Education Institutions
Reference52 articles.
1. (2024, March 08). MAUNA LOA Observatory, Hawaii. Available online: https://www.CO2.earth/.
2. Nanomaterials as catalysts for CO2 transformation into value–added products: A review;Alli;Sci. Total Environ.,2023
3. Andizhanova, T., Adilkhanova, A., and Khalimon, A.Y. (2023). Homogeneous Metal–Catalyzed Hydrogenation of CO2 Derivatives: Towards Indirect Conversion of CO2 to Methanol. Inorganics, 11.
4. Enabling storage and utilization of low–carbon electricity: Power to formic acid;Chatterjee;Energy Environ. Sci.,2021
5. Liquid–phase chemical hydrogen storage materials;Yadav;Energy Environ. Sci.,2012