期刊
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
卷 44, 期 53, 页码 28421-28429出版社
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.ijhydene.2019.02.227
关键词
Formic acid dehydrogenation; Rhodium complexes; N,N '-diimine; DFT prediction; Deactivation
资金
- King Abdullah University of Science and Technology (KAUST)
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 degrees 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. (C) 2019 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
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