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Driving Organic Nanocrystals Dissolution Through Electrochemistry.

ABSTRACT: We have recently discussed how organic nanocrystal dissolution appears in different morphologies and the role of the solution pH in the crystal detriment process. We also highlighted the role of the local molecular chemistry in porphyrin nanocrystals having comparable structures: in water-based acid solutions, protonation of free-base porphyrin molecules is the driving force for crystal dissolution, whereas metal (Zn^II ) porphyrin nanocrystals remain unperturbed. However, all porphyrin types, having an electron rich π-structure, can be electrochemically oxidized. In this scenario, a key question is: does electrochemistry represent a viable strategy to drive the dissolution of both free-base and metal porphyrin nanocrystals? In this work, by exploiting electrochemical atomic force microscopy (EC-AFM), we monitor in situ and in real time the dissolution of both free-base and metal porphyrin nanocrystals, as soon as molecules reach the oxidation potential, showing different regimes according to the applied EC potential.

SUBMITTER: Bussetti G

PROVIDER: S-EPMC8340066 | biostudies-literature | 2021 Aug

REPOSITORIES: biostudies-literature

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Driving Organic Nanocrystals Dissolution Through Electrochemistry.

Bussetti Gianlorenzo G Filoni Claudia C Li Bassi Andrea A Bossi Alberto A Campione Marcello M Orbelli Biroli Alessio A Castiglioni Chiara C Trabattoni Silvia S De Rosa Stefania S Tortora Luca L Ciccacci Franco F Duò Lamberto L

ChemistryOpen 20210801 8

We have recently discussed how organic nanocrystal dissolution appears in different morphologies and the role of the solution pH in the crystal detriment process. We also highlighted the role of the local molecular chemistry in porphyrin nanocrystals having comparable structures: in water-based acid solutions, protonation of free-base porphyrin molecules is the driving force for crystal dissolution, whereas metal (Zn<sup>II</sup> ) porphyrin nanocrystals remain unperturbed. However, all porphyri ...[more]

PMID: 34351082

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Project description:Nanoscale conductive filaments, usually associated with resistive memory or memristor technology, may also be used for chemical sensing and nanophotonic applications; however, realistic implementation of the technology requires precise knowledge of the conditions that control the formation and dissolution of filaments. Here we describe and characterize an addressable direct-write nanoelectrochemical approach to achieve repeatable formation/dissolution of Ag filaments across a ∼100 nm poly(ethylene oxide) (PEO) film containing either Ag+ alone or Ag+ together with 50 nm Ag-nanoparticles acting as bipolar electrodes. Using a conductive AFM tip, formation occurs when the PEO film is subjected to a forward bias, and dissolution occurs under reverse bias. Formation-dissolution kinetics were studied for three film compositions: Ag|PEO-Ag+, Ag|poly(ethylene glycol) monolayer-PEO-Ag+, and Ag|poly(ethylene glycol) monolayer-PEO-Ag+/Ag-nanoparticle. Statistical analysis shows that the distribution of formation times exhibits Gaussian behavior, and the fastest average initial formation time occurs for the Ag|PEO-Ag+ system. In contrast, formation in the presence of Ag nanoparticles likely proceeds by a noncontact bipolar electrochemical mechanism, exhibiting the slowest initial filament formation. Dissolution times are log-normal for all three systems, and repeated reformation of filaments from previously formed structures is characterized by rapid regrowth. The direct-write bipolar electrochemical deposition/dissolution strategy developed here presents an approach to reconfigurable, noncontact in situ wiring of nanoparticle arrays-thereby enabling applications where actively controlled connectivity of nanoparticle arrays is used to manipulate nanoelectronic and nanophotonic behavior. The system further allows for facile manipulation of experimental conditions while simultaneously characterizing surface conditions and filament formation/dissolution kinetics.

Dataset Information

Driving Organic Nanocrystals Dissolution Through Electrochemistry.

Publications

Driving Organic Nanocrystals Dissolution Through Electrochemistry.

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