Selective Coordination Bonding in Metallo‐Supramolecular Systems on Surfaces

Langner, Alexander; Tait, Steven L.; Lin, Nian; Chandrasekar, Rajadurai; Meded, Velimir; Fink, Karin; Rüben, Mario; Kern, Klaus

doi:10.1002/ange.201108530

Cited by 15 publications

(4 citation statements)

References 38 publications

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“…Owing to the advantage of coordination selectivity and diversity with respect to different alkali metals, various static G–metal coordination frameworks can be fabricated, and furthermore these structures could be responsive to metal/molecule stoichiometric ratios, coverage, the valences of metal ions, and/or temperatures resulting in structural transformations. − Hence, to explore the possibility of forming the G–metal coordination structures at water–solid interface, mixtures of G molecules and metal ions were deposited on HOPG surface. As shown in Figure a, when the water solution containing G molecules and Na + was deposited on HOPG surface, three distinct structures labeled as I, II, and III were separated by the white lines, which can be observed on the same area.…”

Section: Resultsmentioning

confidence: 99%

Structural Transformation of Guanine Coordination Motifs in Water Induced by Metal Ions and Temperature

Jin

Liu

et al. 2018

Langmuir

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The transformation effects of metal ions and temperature on the DNA base guanine (G) metal-organic coordination motifs in water have been investigated by scanning tunneling microcopy (STM). The G molecules form an ordered hydrogen-bonded structure at the water-highly oriented pyrolytic graphite interface. The STM observations reveal that the canonical G/9H form can be transformed into the G/(3H,7H) tautomer by increasing the temperature of the G solution to 38.6 °C. Moreover, metal ions bind with G molecules to form GFe, GFe, and the heterochiral intermixed GNa metal-organic networks after the introduction of alkali-metal ions in cellular environment.

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Section: Resultsmentioning

confidence: 99%

Structural Transformation of Guanine Coordination Motifs in Water Induced by Metal Ions and Temperature

Jin

Liu

et al. 2018

Langmuir

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“…Mechanistic understanding is particularly important for the realization of functional catalytic systems, which can be tuned e. g. by modifying reactants and/or surfaces in order to maximize the energy efficiency. Reactions at surfaces, as demonstrated in catalysis, or on surfaces, e. g. in coordination network formation, are often influenced by the availability, the mobility and/or the site‐specific reactivity of atoms. All these parameters strongly depend on the physicochemistry of the surface as well as on temperature.…”

Section: Figurementioning

confidence: 99%

Probing the Reactivity of Functionalized Surfaces by Porphyrin Metalation

et al. 2016

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The presence of N‐ and Cl‐induced superstructures is shown to drastically alter the physicochemical properties of the Cu(001) substrate. We present coherent evidence that N‐ and Cl‐c(2x2) superstructures on Cu(001) decisively impact the metalation reaction of 5,10,15,20‐tetraphenylporphyrin (2HTPP) as well as the on‐surface diffusion and assembly of this molecule. The N superstructure facilitates the metalation reaction and self‐assembled molecular domains of CuTPP are formed at room temperature (RT). In contrast, the Cl superstructure completely inhibits the self‐metalation reaction requiring metal atoms to be deposited from the top and causes 2HTPP to assemble into small clusters. A spectro‐microscopy correlation approach combining X‐ray Photoelectron Spectroscopy (XPS), Ultraviolet Photoelectron Spectroscopy (UPS), Low Energy Electron Diffraction (LEED) and Scanning Tunneling Microscopy (STM) has been utilized in this study.

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“…In this article, we have investigated the facilitation and inhibition of G tautomerization on the Au(111) surface under ultrahigh vacuum (UHV) conditions. For this kind of study, scanning tunneling microscopy (STM) has proven to be the technique of choice since it allows a direct, real-space determination of topographies of different tautomers, 13,14 hydrogen-bonded structural motifs, and binding sites between molecules and metals 15,16 at the atomic scale. From the interplay of high-resolution STM imaging and density functional theory (DFT) calculations, we show for the first time that G molecules undergo a transition from G/9H to G/7H on Au(111) by heating, and a delicate control experiment of 7-methylguanine (7mG) on Au(111) corroborates the above tautomerization process.…”

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confidence: 99%

Atomic-Scale Investigation on the Facilitation and Inhibition of Guanine Tautomerization at Au(111) Surface

et al. 2014

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Nucleobase tautomerization might induce mismatch of base pairing. Metals, involved in many important biophysical processes, have been theoretically proven to be capable of affecting tautomeric equilibria and stabilities of different nucleobase tautomers. However, direct real-space evidence on demonstrating different nucleobase tautomers and further revealing the effect of metals on their tautomerization at surfaces has not been reported to date. From the interplay of high-resolution STM imaging and DFT calculations, we show for the first time that tautomerization of guanine from G/9H to G/7H is facilitated on Au(111) by heating, whereas such tautomerization process is effectively inhibited by introducing Ni atoms due to its preferential coordination at the N7 site of G/9H. These findings may help to elucidate possible influence of metals on nucleobase tautomerization and provide from a molecular level some theoretical basis on metal-based drug design.

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Selective Coordination Bonding in Metallo‐Supramolecular Systems on Surfaces

Cited by 15 publications

References 38 publications

Structural Transformation of Guanine Coordination Motifs in Water Induced by Metal Ions and Temperature

Structural Transformation of Guanine Coordination Motifs in Water Induced by Metal Ions and Temperature

Probing the Reactivity of Functionalized Surfaces by Porphyrin Metalation

Atomic-Scale Investigation on the Facilitation and Inhibition of Guanine Tautomerization at Au(111) Surface

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