MoSx Electrode for Selective NADH Regeneration
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Solution Overview
Problem
Current electrochemical methods for NAD(P)H regeneration often result in single electron transfers, leading to the formation of biologically inactive products such as NAD dimers or 1,2- and 1,6-dihydropyridine, and lack efficient catalysts for direct hydride transfer, which are costly and inefficient.
Innovation Solution
The use of hydride-forming Group VI transition metal chalcogenide catalysts, such as MoSx, that form and transfer hydrides at cathodic potentials in aqueous solutions, excluding single electron transfers, enabling cost-effective and selective enzyme cofactor regeneration.
Engineering Contradictions & Design Principles
Engineering Contradiction Analysis
1Reliability
If traditional electrochemical methods are used for NAD(P)H regeneration, then the process is simple and low-cost, but single electron transfers occur leading to formation of biologically inactive products (NAD dimers or dihydropyridine)
Solution Approach 1:
The patent changes the electrochemical parameters by operating at specific cathodic potentials (−0.3V to −0.6V) that favor hydride formation over single electron transfer. This parameter optimization enables selective regeneration of active NAD(P)H while avoiding inactive byproducts, resolving the contradiction between selectivity and productivity
Solution Approach 2:
The patent introduces Group VI transition metal chalcogenide catalysts (MoSx, WSex) as intermediaries that facilitate direct hydride transfer to NAD(P)+. These catalysts act as mediators between the electrode and cofactor, enabling efficient two-electron reduction without forming single electron transfer products, thus improving both selectivity and regeneration rate
2Reliability
If precious metal catalysts are used for direct hydride transfer, then selective cofactor regeneration is achieved, but the cost increases significantly
Solution Approach 1:
The patent replaces expensive precious metal catalysts with earth-abundant Group VI transition metal chalcogenides (MoSx, WSex). These cheaper catalysts achieve the same selective hydride transfer function, dramatically reducing manufacturing costs while maintaining high selectivity for active NAD(P)H regeneration
Solution Approach 2:
The patent optimizes the composition and structure of earth-abundant catalysts (controlling x values in MoSx and WSex) to enhance their catalytic activity and stability, making them viable alternatives to precious metals while maintaining selective hydride transfer capability
3Productivity
If single electron transfer is used for cofactor regeneration, then the process is fast, but biologically inactive products are formed
Solution Approach 1:
The patent introduces Group VI transition metal chalcogenide catalysts as intermediaries that enable direct two-electron hydride transfer to NAD(P)+. This mechanism bypasses the single electron transfer pathway that leads to inactive products, achieving both fast regeneration rates and high biological activity of the regenerated cofactor
Solution Approach 2:
The patent optimizes electrochemical parameters (potential range of −0.3V to −0.6V) and catalyst composition (x values in MoSx and WSex) to favor direct hydride transfer kinetics over single electron transfer, simultaneously improving reaction rate and product quality
Applied Scientific Principles
This section explains which scientific principles are used to turn an abstract innovation direction into a practical engineering solution.
Function Achieved in This Case
This approach improves the rate of oxidoreductase-catalyzed reactions by regenerating oxidized cofactors like NAD+ and NADP+ to their active forms, avoiding dimerization and enhancing biocatalytic efficiency, as demonstrated by high yields in NADH regeneration and biocatalytic conversions like benzaldehyde to benzyl alcohol.
Implementation Method 1
holding an electrode including a Group VI transition metal chalcogenide catalyst at a potential sufficient to form a metal hydride in an aqueous electrolyte solution
Implementation Method 2
contacting the electrode with an oxidized cofactor to reduce the cofactor
Implementation Method 3
The ability of Group VI transition metal chalcogenide electrocatalysts to form and transfer hydrides
Data Source
AI summary
Embodiments of the present disclosure describe methods and systems using a hydride-forming Group VI transition metal chalcogenide catalyst, such as MoSx, for selective electrocatalysis of enzyme cofactor regeneration. In particular, a method of electrochemical cofactor regeneration comprising: holding an electrode comprising a Group VI transition metal chalcogenide catalyst at a potential sufficient to form a metal hydride in an aqueous electrolyte solution; and contacting the electrode with an oxidized cofactor to reduce the cofactor, is provided. The reduced cofactor can be used by a cofactor-dependent oxidoreductase to convert a substrate to a desired product and subsequently regenerated.