Surface Reorganization of Transition Metal Dichalcogenide Nanoflowers for Efficient Electrochemical Coenzyme Regeneration

Nicholas Williams, Karley Hahn, Ryan Goodman, Xiaowen Chen, Jing Gu

Research output: Contribution to journalArticlepeer-review

1 Scopus Citations

Abstract

In the past 20 years, enzymatic conversions have been intensely examined as a practical and environmentally friendly alternative to traditional organocatalytic conversions for chemicals and pharmaceutical intermediate production. Out of all commercial enzymes, more than one-fourth are oxidoreductases that operate in tandem with coenzymes, typically nicotinamide adenine dinucleotide (NADH) or nicotinamide adenine dinucleotide phosphate (NADPH). Enzymes utilize coenzymes as a source for electrons, protons, or holes. Unfortunately, coenzymes can be exorbitant; thus, recycling coenzymes is paramount to establishing a sustainable and affordable cell-free enzymatic catalyst system. Herein, cost-effective transition metal dichalcogenides (TMDCs), 2H-MoS2, 2H-WS2, and 2H-WSe2, were employed for the first time for direct electrochemical reduction of NAD+ to the active form of the NADH (1,4-NADH). Of the three TMDCs, 2H-WSe2 shows optimal activity, producing 1,4 NADH at a rate of 6.5 μmol cm-2 h-1 and a faradaic efficiency of 45% at −0.8 V vs Ag/AgCl. Interestingly, a self-induced surface reorganization process was identified, where the native surface oxide grown in the air was spontaneously removed in the electrochemical process, resulting in the activation of TMDCs.

Original languageAmerican English
Pages (from-to)3925-3933
Number of pages9
JournalACS Applied Materials and Interfaces
Volume15
Issue number3
DOIs
StatePublished - 2023

Bibliographical note

Publisher Copyright:
© 2023 The Authors. Published by American Chemical Society.

NREL Publication Number

  • NREL/JA-5100-85278

Keywords

  • catalyst activation
  • electrochemical coenzyme generation
  • surface reorganization
  • transition metal dichalcogenides

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