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- Title
Explicit Water Molecules Play a Key Role in the Mechanism of Rhodium-Substituted Human Carbonic Anhydrase.
- Authors
Piazzetta, Paolo; Marino, Tiziana; Russo, Nino; Salahub, Dennis R.
- Abstract
The efficient conversion of carbon dioxide into useful products is a prime challenge to modern chemistry. An alternative route to address this challenge based on a rhodium-substituted human carbonic anhydrase is described that can be considered the first cofactor-independent reductase. This artificial enzyme is able to convert CO2 into formic acid, with potential applications in renewable energy. Our quantum mechanical investigation (QM/QM′ method), which considers the entire catalytic pocket (390 atoms), provides evidence that the catalytic process is governed by an energetically favored σ-bond-metathesis mechanism and the rate-limiting step is the release of formic acid (11.7 kcal mol−1). Water molecules are found to play an active role during the chemical process by contributing to reduce dramatically the energy of the rate-limiting step and favoring an efficient regeneration of the catalyst.
- Subjects
CARBONIC anhydrase; CARBON dioxide; HYDROGENATION; RHODIUM; CHEMICAL synthesis; ENZYMES; QUANTUM mechanics
- Publication
ChemCatChem, 2017, Vol 9, Issue 6, p1047
- ISSN
1867-3880
- Publication type
Article
- DOI
10.1002/cctc.201601433