期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 290, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2021.120036
关键词
Ru; Solid micelles; Single-atom catalysts; CO2 hydrogenation; Formic acid
资金
- ANR (France) Nano4FUT project [ANR-16-CE06-0013]
- VLAIO [HBC.2017.0692]
- UGent High-Performance Computing (HPC)
- Ghent University
- FWO
- Flemish Government -department EWI
- Fund for Scientific Research Flanders (FWO)
The newly designed solid micellar Ru single-atom catalyst allows for efficient and stable water-free CO2 hydrogenation to formic acid, producing concentrated formate solutions. The incorporation of Ru(III) single sites into the MCM-41 walls creates a solid micelle structure, while the presence of CTA(+) surfactant in the pores of MCM-41 stabilizes the Ru sites and prevents catalyst deactivation. DFT modelling indicates that the reaction proceeds via heterolytic hydrogen splitting, forming a Ru-H species and subsequent hydride transfer to CO2.
The catalytic hydrogenation of CO2 to formic acid is one of the most promising pathways towards a renewable hydrogen-storage system. The reaction is usually performed in aqueous phase in the presence of basic molecules over homogeneous or heterogeneous catalysts, generating relatively dilute formate solutions (<1 M). The newly designed solid micellar Ru single-atom catalyst enables efficient and stable water-free CO2 hydrogenation to formate under mild reaction conditions. Concentrated formate solutions (up to 4 M) are produced directly from the hydrogenation of carbon dioxide in water-free tertiary amine. In the catalyst, Ru(III) single sites are incorporated into the walls of MCM-41 during hydrolysis creating a solid micelle structure. The presence of the CTA(+) surfactant in the pores of MCM-41 stabilizes the Ru sites and prevents catalyst deactivation. DFT modelling suggests that the reaction proceeds via heterolytic hydrogen splitting, forming a Ru-H species and subsequent hydride transfer to CO2.
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