Metallo-responsive self-assembly of lipophilic guanines in hydrocarbon solvents: a systematic SAXS structural characterization

Gonnelli, A.; Pieraccini, Silvia; Baldassarri, E.; Funari, Sérgio S.; Masiero, Stefano; Ortore, María Grazia; Mariani, Paolo

doi:10.1039/c9nr08556d

Cited by 3 publications

(6 citation statements)

References 63 publications

(78 reference statements)

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“…A second guanosine-based motif, the G-ribbon, can form an extended sheet of interacting guanines. It has been shown that lipophilic-derivatized guanosine molecules can form either G-quartet or G-ribbon based supramolecular structures based on the presence of metal cations [18,19].…”

Section: Introductionmentioning

confidence: 99%

Impact of C-Terminal Chemistry on Self-Assembled Morphology of Guanosine Containing Nucleopeptides

et al. 2020

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Herein, we report the design and characterization of guanosine-containing self-assembling nucleopeptides that form nanosheets and nanofibers. Through spectroscopy and microscopy analysis, we propose that the peptide component of the nucleopeptide drives the assembly into β-sheet structures with hydrogen-bonded guanosine forming additional secondary structures cooperatively within the peptide framework. Interestingly, the distinct supramolecular morphologies are driven not by metal cation responsiveness common to guanine-based materials, but by the C-terminal peptide chemistry. This work highlights the structural diversity of self-assembling nucleopeptides and will help advance the development of applications for these supramolecular guanosine-containing nucleopeptides.

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Section: Introductionmentioning

confidence: 99%

Impact of C-Terminal Chemistry on Self-Assembled Morphology of Guanosine Containing Nucleopeptides

et al. 2020

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“…On this subject, many efforts have been devoted to exploit H-bonds as a key for encoding chemical information, and the structures expressed have spanned the range of dimensions and shapes. Guanosines and guanosine derivatives were shown to undergo a hierarchical self-assembly process in water and in organic solvents [6,7]. The process is essentially driven by ion complexation and solvophobic effects, resulting in nanoribbons [6,7] or in a stack of disks, which define the helicoidal nanowire (G-quadruplex) of 25 Å diameter and up to hundred nanometers long with an open central channel [10].…”

Section: Discussionmentioning

confidence: 99%

“…Guanosines and guanosine derivatives were shown to undergo a hierarchical self-assembly process in water and in organic solvents [6,7]. The process is essentially driven by ion complexation and solvophobic effects, resulting in nanoribbons [6,7] or in a stack of disks, which define the helicoidal nanowire (G-quadruplex) of 25 Å diameter and up to hundred nanometers long with an open central channel [10]. Noteworthy, guanosine-rich single-stranded sequences of DNA have been demonstrated to adopt various tertiary structures, including G-quadruplexes.…”

Section: Discussionmentioning

confidence: 99%

“…In several SAXS curves, a Bragg peak appears (see Figure 11), suggesting that the particle number density is so high, and the particle-particle repulsive interactions so low, that the G-quadruplexes adopt a liquid-crystalline order [7,10,32]). Because in all the different cases only one Bragg peak was detected, peak indexing was not possible, but previous structural results [32] provided continuity arguments to describe the liquid-crystalline phase.…”

Section: Condensed Phasesmentioning

confidence: 99%

“…Guanine (G) has gained considerable interest in the last years because of the four DNA bases is the only one able to give rise to supramolecular aggregation phenomena in solution, leading to complex structures ranging from G-quartets to G-quadruplexes and G-ribbons [1][2][3][4][5][6][7]. G-quartets and G-quadruplexes form by self-assembly in water solution: G-quartets are planar rings made by four guanine molecules bound to one another through extended hydrogen bonds (according to the so-called Hoogsteen's scheme) (Figure 1a,b), while G-quadruplexes are four-stranded helical structures made by the out-of-register stacking of planar G-quartets coordinated by monovalent cations (Figure 1c,d).…”

Section: Introductionmentioning

confidence: 99%

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K+ vs. Na+ Effects on the Self-Assembly of Guanosine 5′-Monophosphate: A Solution SAXS Structural Study

et al. 2020

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The hierarchical process of guanosine (G) self-assembly, leading in aqueous solution and in the presence of metal cations to the formation of G-quadruplexes, represents an intriguing topic both for the biological correlation with telomerase activity and for the nano-technological applications, as demonstrated by the current measured in a quadruplex wire 100 nm long. Similar to G-rich DNA sequences and G-oligonucleotides, the guanosine 5′-monophosphate (GMP) self-aggregates in water to form quadruplexes. However, due to the absence of a covalent axial backbone, this system can be very useful to understand the chemical-physical conditions that govern the guanosine supramolecular aggregation. We have then investigated by in-solution Synchrotron Small Angle X-ray Scattering technique the role of different cations in promoting the quadruplex formation as a function of concentration and temperature. Results show how potassium, with its peculiar biological traits, favours the G-quadruplex elongation process in respect to other cations (Na + , but also NH 4 + and Li + ), determining the longest particles in solution. Moreover, the formation and the elongation of G-quadruplexes have been demonstrated to be controlled by both GMP concentration and excess cation content, even if they specifically contribute to these processes in different ways. The occurrence of condensed liquid crystalline phases was also detected, proving that excess cations play also unspecific effects on the effective charges on the G-quadruplex surface.

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Global fitting of multiple data frames from SEC–SAXS to investigate the structure of next-generation nanodiscs

Barclay

Johansen

Tidemand

et al. 2022

Acta Crystallogr D Struct Biol

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The combination of online size-exclusion chromatography and small-angle X-ray scattering (SEC–SAXS) is rapidly becoming a key technique for structural investigations of elaborate biophysical samples in solution. Here, a novel model-refinement strategy centred around the technique is outlined and its utility is demonstrated by analysing data series from several SEC–SAXS experiments on phospholipid bilayer nanodiscs. Using this method, a single model was globally refined against many frames from the same data series, thereby capturing the frame-to-frame tendencies of the irradiated sample. These are compared with models refined in the traditional manner, in which refinement is based on the average profile of a set of consecutive frames from the same data series without an in-depth comparison of individual frames. This is considered to be an attractive model-refinement scheme as it considerably lowers the total number of parameters refined from the data series, produces tendencies that are automatically consistent between frames, and utilizes a considerably larger portion of the recorded data than is often performed in such experiments. Additionally, a method is outlined for correcting a measured UV absorption signal by accounting for potential peak broadening by the experimental setup.

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Metallo-responsive self-assembly of lipophilic guanines in hydrocarbon solvents: a systematic SAXS structural characterization

Abstract: Elongation, flexibility and thermal stability of metallo-responsive architectures in dodecane.

Cited by 3 publications

References 63 publications

Impact of C-Terminal Chemistry on Self-Assembled Morphology of Guanosine Containing Nucleopeptides

Impact of C-Terminal Chemistry on Self-Assembled Morphology of Guanosine Containing Nucleopeptides

K+ vs. Na+ Effects on the Self-Assembly of Guanosine 5′-Monophosphate: A Solution SAXS Structural Study

Global fitting of multiple data frames from SEC–SAXS to investigate the structure of next-generation nanodiscs

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