Efficient Nicotinamide Adenine Dinucleotide Regeneration with a Rhodium-Carbene Catalyst and Isolation of a Hydride Intermediate
- Authors
- Ganesan, Vinothkumar; Kim, Jennifer Juhyun; Shin, Jeongcheol; Park, Kiyoung; Yoon, Sungho
- Issue Date
- Apr-2022
- Publisher
- NLM (Medline)
- Citation
- Inorganic chemistry, v.61, no.15, pp 5683 - 5690
- Pages
- 8
- Journal Title
- Inorganic chemistry
- Volume
- 61
- Number
- 15
- Start Page
- 5683
- End Page
- 5690
- URI
- https://scholarworks.bwise.kr/cau/handle/2019.sw.cau/61485
- DOI
- 10.1021/acs.inorgchem.2c00059
- ISSN
- 0020-1669
1520-510X
- Abstract
- Regeneration of nicotinamide adenine dinucleotide (NADH) has been the primary interest in the field of enzymatic transformation, especially associating oxidoreductases given the stoichiometric consumption. The synthesized carbene-ligated rhodium complex [(η5-Cp*)Rh(MDI)Cl]+ [Cp* = pentamethylcyclopentadienyl; MDI = 1,1'-methylenebis(3,3'-dimethylimidazolium)] acts as an exceptional catalyst in the reduction of NAD+ to NADH with a turnover frequency of 1730 h-1, which is over twice that of the higher catalytic activity of the commercially available catalyst [Cp*Rh(bpy)Cl]+ (bpy = 2,2'-bipyridine). Offsetting the contentious atmosphere currently taking place over the specific intermediate of the NADH regeneration, this study presents pivotal evidence of a metal hydride intermediate with a bis(carbene) ligand: a stable form of the rhodium hydride intermediate, [(η5-Cp*)Rh(MDI)H]+, was isolated and fully characterized. This enables thorough insight into the possible mechanism and exact intermediate structure in the NAD+ reduction process.
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