Secondary Structure in Enzyme‐Inspired Polymer Catalysts Impacts Water Oxidation Efficiency
Name
Advanced Science - 2024 - Sedenho - Secondary Structure in Enzyme‐Inspired Polymer Catalysts Impacts Water Oxidation.pdf
Description
Published version
Size
1.7 MB
Format
Adobe PDF
Checksum (MD5)
f7a90403205c8a1fd4fe6ebb301466d2
Author(s)
Sedenho, Graziela C
Nascimento, Steffane Q
Zamani, Marjon
Crespilho, Frank N
Furst, Ariel L
Date Issued
July 2024
Journal
Advanced Science
Publisher
Wiley
Citation
Sedenho, Graziela C, Nascimento, Steffane Q, Zamani, Marjon, Crespilho, Frank N and Furst, Ariel L. 2024. "Secondary Structure in Enzyme‐Inspired Polymer Catalysts Impacts Water Oxidation Efficiency." Advanced Science, 11 (25).
Version
Final published version
Abstract
Protein structure plays an essential role on their stability, functionality, and catalytic activity. In this work, the interplay between the β-sheet structure and its catalytic implications to the design of enzyme-inspired materials is investigated. Here, inspiration is drawn from the active sites and β-sheet rich structure of the highly efficient multicopper oxidase (MCO) to engineer a bio-inspired electrocatalyst for water oxidation utilizing the abundant metal, copper. Copper ions are coordinated to poly-histidine (polyCuHis), as they are in MCO active sites. The resultant polyCuHis material effectively promotes water oxidation with low overpotentials (0.15 V) in alkaline systems. This activity is due to the 3D structure of the poly-histidine backbone. By increasing the prevalence of β-sheet structure and decreasing the random coil nature of the polyCuHis secondary structures, this study is able to modulates the electrocatalytic activity of this material is modulated, shifting it toward water oxidation. These results highlight the crucial role of the local environment at catalytic sites for efficient, energy-relevant transformations. Moreover, this work highlights the importance of conformational structure in the design of scaffolds for high-performance electrocatalysts.
MIT Department
Massachusetts Institute of Technology. Department of Chemical Engineering
Terms of Use
Creative Commons Attribution
Persistent DSpace Link
DOI of Published Version
https://doi.org/10.1002/advs.202402234
