Room-temperature surface-assisted reactivity of a melanin precursor: silver metal-organic coordination versus covalent dimerization on gold

Nanoscale
F De MarchiF Rosei

Abstract

The ability of catecholamines to undergo oxidative self-polymerization provides an attractive route for preparation of coatings for biotechnology and biomedicine applications. However, efforts toward developing a complete understanding of the mechanism that underpins polymerization have been hindered by the multiple catechol crosslinking reaction pathways that occur during the reaction. Scanning tunneling microscopy allows the investigation of small molecules in a reduced-complexity environment, providing important insight into how the intermolecular forces drive the formation of supramolecular assemblies in a controlled setting. Capitalizing on this approach, we studied the self-assembly of 5,6-dihydroxy-indole (DHI) on Au(111) and Ag(111) to investigate the interactions that affect the two-dimensional growth mechanism and to elucidate the behavior of the catechol group on these two surfaces. X-ray photoelectron spectroscopy, together with density functional theory and Monte Carlo modeling, helps unravel the differences between the two systems. The molecules form large ordered domains, yet with completely different architectures. Our data reveal that some of the DHI molecules deposited on Ag are in a modified redox state, with...Continue Reading

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Citations

May 28, 2019·Dalton Transactions : an International Journal of Inorganic Chemistry·Min ZhangJian-Ping Lang
Aug 17, 2019·Advanced Materials·Haoran ChenKai Wu
Feb 9, 2021·Global Challenges·Hanaa A GalebJohn G Hardy
Feb 16, 2021·The Journal of Physical Chemistry Letters·Yangyang HanLifeng Chi
Jun 25, 2021·Chemical Science·Ana Cristina Gómez-HerreroJohann Coraux
Mar 20, 2019·Journal of the American Chemical Society·Yi-Qi ZhangFlorian Klappenberger
Nov 9, 2021·The Journal of Physical Chemistry Letters·Zhenzhe ZhangRustam Z Khaliullin

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Methods Mentioned

BETA
scanning tunneling microscopy
X-ray

Software Mentioned

Vienna Ab initio Simulation Package ( VASP )
WSxM
Gaussian09

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