The effect of water on gold supported chiral graphene nanoribbons: rupture of conjugation by an alternating hydrogenation pattern
Year: 2023
Type: article
Abstract: In the last few years we have observed a breakpoint in the development of graphene-derived technologies, such as liquid phase filtering and their application to electronics. In most of these cases, they imply exposure of the material to solvents and ambient moisture, either in the fabrication of the material or the final device. The present study demonstrates the sensitivity of graphene nanoribbon (GNR) zigzag edges to water, even in extremely low concentrations. We have addressed the unique reactivity of (3,1)-chiral GNR with moisture on Au(111). Water shows a reductive behaviour, hydrogenating the central carbon of the zigzag segments. By combining scanning tunnelling microscopy (STM) with simulations, we demonstrate how their reactivity reaches a thermodynamic limit when half of the unit cells are reduced, resulting in an alternating pattern of hydrogenated and pristine unit cells starting from the terminal segments. Once a quasi-perfect alternation is reached, the reaction stops regardless of the water concentration. The hydrogenated segments limit the electronic conjugation of the GNR, but the reduction can be reversed both by tip manipulation and annealing. Selective tip-induced dehydrogenation allowed the stabilization of radical states at the edges of the ribbons, while the annealing of the sample completely recovered the original, pristine GNR.
Source: Nanoscale
DOI: 10.1039/d3nr02933f
Institutions: Material Physics Center, Donostia International Physics Center, Czech Academy of Sciences, Regional Centre of Advanced Technologies and Materials, FZU - Institute of Physics of the Czech Academy of Sciences, Palacký University Olomouc, Czech Technical University in Prague, Universidade de Santiago de Compostela, Centro Singular de Investigación en Química Biológica y Materiales Moleculares, Texas Tech University, VSB - Technical University of Ostrava, Czech Academy of Sciences, Institute of Organic Chemistry and Biochemistry, Consejo Superior de Investigaciones Científicas, Nanomaterials and Nanotechnology Research Center
Language: English
Subfield: Materials Chemistry
Field: Materials Science
Domain: Physical Sciences
Open Access status: hybrid
Funders: National Science Foundation, European Commission, Ministerstvo Školství, Mládeže a Tělovýchovy, Grantová Agentura České Republiky, Univerzita Palackého v Olomouci, Xunta de Galicia, Centro Singular de Investigación de Galicia, European Regional Development Fund, Agencia Estatal de Investigación, Division of Chemistry, H2020 Marie Skłodowska-Curie Actions, NextGenerationEU
Awards: G1175115578, G1218400627, Atomic-scale control and visualization of charge delocalization in light-harvesting molecular nanomodels, G1819502802, G1902886428, G193230900, G210041235, G2165797334, G2262748287, G2507177754, G2538972755, G2601397997, G2629758493, Research infrastructure CzechNanoLab, G300979063, G3094748848, G34346518, G3480869486, G3516499063, G3681454997, G3857021370, G4042783231, G4092263876, Controlling Chemical Reactions For Carbon-Based Functional Materials Production on Surfaces, G4177275134, G425668148, G434337789, G485196324, G4912030886, G5080475149, G5195188938, G535059049, e-Infrastructure CZ, G5798604787, G5804263762, 1D molecular chains on surfaces, G692825579, G707751529, G7084143925, SPin Research IN Graphene, G7358480839, G7545815938, G8113226877, Collaborative Research: Aggregation Mechanisms in Carbon Nanomaterials Based on Pi-conjugated Polycyclic Aromatic Hydrocarbons, G8340473533, G8631275686, G8684520763, Controlling Chemical Reactions For Carbon-Based Functional Materials Production on Surfaces
OpenAlex ID: W4388777964