Computationally guided design of a new Rh catalyst for selective formic acid dehydrogenation: Validation with caution
KAUST DepartmentPhysical Sciences and Engineering (PSE) Division
Chemical Science Program
KAUST Catalysis Center (KCC)
Permanent link to this recordhttp://hdl.handle.net/10754/653023
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AbstractFormic acid possesses many desirable properties as a promising hydrogen energy carrier. Density functional theory (DFT) was utilized to design new Rh complexes with 2,2′-biimidazoline ligands to explore their potential as catalysts for formic acid dehydrogenation. These designed complexes were prepared and examined as catalysts under various temperatures and ratios of formic acid to sodium formate. It was found that although our complexes gave a high TOF of 20,000 h−1 at 90 °C under certain formic acid/sodium formate ratios, the dehydrogenation reaction was prematurely deactivated once 30% of the formic acid was consumed. Possible deactivation mechanisms were investigated by NMR and HRMS. Our observations suggest that while guided rational design of catalysts by DFT has much potential, the method does have limitations as evidenced by our experimental comparisons and thus pure DFT design should be conducted with caution.
CitationGuan C, Zhang D-D, Zhang T, Huang M-H, Chakraborty P, et al. (2019) Computationally guided design of a new Rh catalyst for selective formic acid dehydrogenation: Validation with caution. International Journal of Hydrogen Energy. Available: http://dx.doi.org/10.1016/j.ijhydene.2019.02.227.
SponsorsThis work was supported by funding from King Abdullah University of Science and Technology (KAUST).