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Chemistry
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On-Surface Synthesis: Methods and Applications
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On-Surface Synthesis: Methods and Applications

A special issue of Chemistry (ISSN 2624-8549). This special issue belongs to the section "Physical Chemistry and Chemical Physics".

Deadline for manuscript submissions: closed (28 February 2022) | Viewed by 14490

Special Issue Editor

Prof. Dr. Albano Cossaro

E-Mail Website
Guest Editor
Department of Chemical and Pharmaceutical Science, University of Trieste, via L. Giorgieri 1, Trieste, Italy
Interests: on-surface synthesis; self-assembly; ultra-thin films; in-situ molecular film growth; charge dynamics at organo-metallic interfaces

Special Issue Information

Dear Colleagues,

A key issue in the design of efficient organic-based devices is the tuning of the electronic, morphologic, and chemical properties at the interface between organic films and electrodes. On-surface synthesis represents a convenient approach to modify the surface and to introduce an interface with the desired properties. The synthesis of covalently bound structures or the formation of organo-metallic complexes may overcome the problems related to the poor robustness that self-assembled thin films often have. With the proper choice of precursors, specific functional groups can be distributed on the surface, thus modelling its chemical properties and eventually promoting the selective recognition of guest molecules. Moreover, extended on-surface confined covalent structures can exhibit delocalized electronic states, possibly originating dispersion in the valence band structure of the interface. In this Special Issue of Chemistry devoted to “On-Surface Synthesis: Methods and Applications”, we invite contributions regarding the on-surface synthesis of organic molecules, 2D covalent organic frameworks, and organo-metallic complexes and, in general, the on-surface modification of molecular precursors. We welcome submissions regarding the mechanisms of the on-surface reactions, the characterization of the synthesized interfaces, and the applications of on-surface-synthesized systems. 

Prof. Dr. Albano Cossaro
Guest Editor

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Chemistry is an international peer-reviewed open access semimonthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 1800 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • 2D covalent structures
  • surface functionalization
  • on-surface molecular anchoring
  • 2D covalent organic frameworks
  • in-situ growth of 2D interfaces

Related Special Issue

Published Papers (5 papers)

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Research

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11 pages, 2692 KiB  
Article
Initial Coupling and Reaction Progression of Directly Deposited Biradical Graphene Nanoribbon Monomers on Iodine-Passivated Versus Pristine Ag(111)
by Gianluca Galeotti, Massimo Fritton, Matthias Lischka, Sebastian Obermann, Ji Ma, Wolfgang M. Heckl, Xinliang Feng and Markus Lackinger
Chemistry 2022, 4(2), 259-269; https://doi.org/10.3390/chemistry4020020 - 29 Mar 2022
Cited by 1 | Viewed by 2660
Abstract
The development of widely applicable methods for the synthesis of C-C-bonded nanostructures on inert and insulating surfaces is a challenging yet rewarding milestone in the field of on-surface synthesis. This would enable studies of nearly unperturbed covalent nanostructures with unique electronic properties as [...] Read more.
The development of widely applicable methods for the synthesis of C-C-bonded nanostructures on inert and insulating surfaces is a challenging yet rewarding milestone in the field of on-surface synthesis. This would enable studies of nearly unperturbed covalent nanostructures with unique electronic properties as graphene nanoribbons (GNR) and π-conjugated 2D polymers. The prevalent Ullmann-type couplings are almost exclusively carried out on metal surfaces to lower the temperature required for initial dehalogenation well below the desorption threshold. To overcome the necessity for the activation of monomers on the target surface, we employ a recently developed Radical Deposition Source (RaDeS) for the direct deposition of radicals onto inert surfaces for subsequent coupling by addition reactions. The radicals are generated en route by indirect deposition of halogenated precursors through a heated reactive tube, where the dehalogenation reaction proceeds. Here, we use the ditopic 6,11-diiodo-1,2,3,4-tetraphenyltriphenylene (DITTP) precursor that afforded chevron-like GNR on Au(111) via the usual two-staged reaction comprised of monomer-coupling into covalent polymers and subsequent formation of an extended GNR by intramolecular cyclodehydrogenation (CDH). As a model system for inert surfaces, we use Ag(111) passivated with a closed monolayer of chemisorbed iodine that behaves in an inert manner with respect to dehalogenation reactions and facilitates the progressive coupling of radicals into extended covalent structures. We deposit the DITTP-derived biradicals onto both iodine-passivated and pristine Ag(111) surfaces. While on the passivated surface, we directly observe the formation of covalent polymers, on pristine Ag(111) organometallic intermediates emerge instead. This has decisive consequences for the further progression of the reaction: heating the organometallic chain directly on Ag(111) results in complete desorption, whereas the covalent polymer on iodine-passivated Ag(111) can be transformed into the GNR. Yet, the respective CDH proceeds directly on Ag(111) after thermal desorption of the iodine passivation. Accordingly, future work is aimed at the further development of approaches for the complete synthesis of GNR on inert surfaces. Full article
(This article belongs to the Special Issue On-Surface Synthesis: Methods and Applications)
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6 pages, 1424 KiB  
Article
On-Surface Synthesis of Polypyridine: Strain Enforces Extended Linear Chains
by Laerte L. Patera, Josef Amler and Jascha Repp
Chemistry 2022, 4(1), 112-117; https://doi.org/10.3390/chemistry4010009 - 16 Feb 2022
Cited by 5 | Viewed by 2834
Abstract
Strain-induced on-surface transformations provide an appealing route to steer the selectivity towards desired products. Here, we demonstrate the selective on-surface synthesis of extended all-trans poly(2,6-pyridine) chains on Au(111). By combining high-resolution scanning tunneling and atomic force microscopy, we revealed the detailed chemical [...] Read more.
Strain-induced on-surface transformations provide an appealing route to steer the selectivity towards desired products. Here, we demonstrate the selective on-surface synthesis of extended all-trans poly(2,6-pyridine) chains on Au(111). By combining high-resolution scanning tunneling and atomic force microscopy, we revealed the detailed chemical structure of the reaction products. Density functional theory calculations indicate that the synthesis of extended covalent structures is energetically favored over the formation of macrocycles, due to the minimization of internal strain. Our results consolidate the exploitation of internal strain relief as a driving force to promote selective on-surface reactions. Full article
(This article belongs to the Special Issue On-Surface Synthesis: Methods and Applications)
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10 pages, 5192 KiB  
Article
On-Surface Synthesis of Boroxine-Based Molecules
by Elia Turco, Matus Stredansky, Roberto Costantini, Javier A. Martinez, Martina Dell’Angela, Elena Zerbato, Daniele Toffoli, Giovanna Fronzoni, Alberto Morgante, Luca Floreano and Albano Cossaro
Chemistry 2021, 3(4), 1401-1410; https://doi.org/10.3390/chemistry3040101 - 30 Nov 2021
Cited by 2 | Viewed by 3552
Abstract
The on-surface synthesis of boroxine-containing molecules can be a convenient method of introducing specific functionalities. Here, we show the validity of a previously described synthesis protocol on the Au (111) surface by applying it to a different molecular precursor. We study in detail [...] Read more.
The on-surface synthesis of boroxine-containing molecules can be a convenient method of introducing specific functionalities. Here, we show the validity of a previously described synthesis protocol on the Au (111) surface by applying it to a different molecular precursor. We study in detail the assembly of the precursor, highlighting possible intermediate stages of the condensation process. We combine scanning tunneling microscopy and X-ray spectroscopies to fully characterize both the morphology and the electronic properties of the system. DFT calculations are presented to assign the main electronic transitions originating the B K-edge absorption spectrum. The study paves the way to a facile strategy for functionalizing a surface with molecules of tailored sizes and compositions. Full article
(This article belongs to the Special Issue On-Surface Synthesis: Methods and Applications)
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6 pages, 1999 KiB  
Communication
Spectroscopic Evidence of New Low-Dimensional Planar Carbon Allotropes Based on Biphenylene via On-Surface Ullmann Coupling
by Teng Zhang, Cesare Grazioli, Huixia Yang, Kaiyue Jiang, Iulia Emilia Brumboiu, Liangguang Jia, Liwei Liu, Carla Puglia, Xiaodong Zhuang and Yeliang Wang
Chemistry 2021, 3(3), 1057-1062; https://doi.org/10.3390/chemistry3030076 - 13 Sep 2021
Cited by 6 | Viewed by 2591
Abstract
The bottom-up synthesis and preliminary characterizations of a new biphenylene-based 2D framework are presented. This new low-dimensional carbon allotrope potentially completes the many hypothesized carbon networks based on biphenylene. Full article
(This article belongs to the Special Issue On-Surface Synthesis: Methods and Applications)
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Review

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15 pages, 4904 KiB  
Review
On-Surface Chemistry on Low-Reactive Surfaces
by Elie Geagea, Frank Palmino and Frédéric Cherioux
Chemistry 2022, 4(3), 796-810; https://doi.org/10.3390/chemistry4030057 - 11 Aug 2022
Cited by 3 | Viewed by 1972
Abstract
Zero-dimensional (0D), mono-dimensional (1D), or two-dimensional (2D) nanostructures with well-defined properties fabricated directly on surfaces are of growing interest. The fabrication of covalently bound nanostructures on non-metallic surfaces is very promising in terms of applications, but the lack of surface assistance during their [...] Read more.
Zero-dimensional (0D), mono-dimensional (1D), or two-dimensional (2D) nanostructures with well-defined properties fabricated directly on surfaces are of growing interest. The fabrication of covalently bound nanostructures on non-metallic surfaces is very promising in terms of applications, but the lack of surface assistance during their synthesis is still a challenge to achieving the fabrication of large-scale and defect-free nanostructures. We discuss the state-of-the-art approaches recently developed in order to provide covalently bounded nanoarchitectures on passivated metallic surfaces, semiconductors, and insulators. Full article
(This article belongs to the Special Issue On-Surface Synthesis: Methods and Applications)
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