Computationally guided design of a new Rh catalyst for selective formic acid dehydrogenation: Validation with caution

Chao Guan, Dan-Dan Zhang, Tonghuan Zhang, Mei-Hui Huang, Priyanka Chakraborty, Huaifeng Li, Changguang Yao, Chunhui Zhou, Jinsong Hu, Kuo-Wei Huang

Research output: Contribution to journalArticlepeer-review

3 Scopus citations

Abstract

Formic 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.
Original languageEnglish (US)
Pages (from-to)28421-28429
Number of pages9
JournalInternational Journal of Hydrogen Energy
Volume44
Issue number53
DOIs
StatePublished - Apr 1 2019

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