Two-dimensional self-assembly of benzotriazole on an inert substrate

Fine tuning of experimental conditions allows dimensional control of benzotriazole species adsorbed on Au(111), revealing a subtle interplay between H-bonding, vdW inter-adsorbate and surface-adsorbate interactions, as highlighted both experimentally and theoretically.

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Investigation of Au SAMs Photoclick Derivatization by PM-IRRAS

10.26434/chemrxiv.11347976 ◽

2019 ◽

Author(s):

Mark Workentin ◽

François Lagugné-Labarthet ◽

Sidney Legge

Keyword(s):

Cell Adhesion ◽

Self Assembly ◽

Materials Science ◽

Fibroblast Cell ◽

Fine Tuning ◽

Chemical System ◽

Infrared Reflection ◽

Assembled Monolayers ◽

One Step ◽

High Degree

In this work we present a clean one-step process for modifying headgroups of self-assembled monolayers (SAMs) on gold using photo-enabled click chemistry. A thiolated, cyclopropenone-caged strained alkyne precursor was first functionalized onto a flat gold substrate through self-assembly. Exposure of the cyclopropenone SAM to UV-A light initiated the efficient photochemical decarbonylation of the cyclopropenone moiety, revealing the strained alkyne capable of undergoing the interfacial strain-promoted alkyne-azide cycloaddition (SPAAC). Irradiated SAMs were derivatized with a series of model azides with varied hydrophobicity to demonstrate the generality of this chemical system for the modification and fine-tuning of the surface chemistry on gold substrates. SAMs were characterized at each step with polarization-modulation infrared reflection-absorption spectroscopy (PM-IRRAS) to confirm successful functionalization and reactivity. Furthermore, to showcase the compatibility of this approach with biochemical applications, cyclopropenone SAMs were irradiated and modified with azide-bearing cell adhesion peptides to promote human fibroblast cell adhesion, then imaged by live cell fluorescence microscopy. Thus, the “photoclick” methodology reported here represents an improved, versatile, catalyst-free protocol that allows for a high degree of control over the modification of material surfaces, with applicability in materials science as well as biochemistry.<br>

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Faculty Opinions recommendation of Self-assembly of coherently dynamic, auxetic, two-dimensional protein crystals.

Faculty Opinions – Post-Publication Peer Review of the Biomedical Literature ◽

10.3410/f.726325825.793518578 ◽

2016 ◽

Author(s):

Christopher Chang

Keyword(s):

Self Assembly ◽

Protein Crystals ◽

Two Dimensional

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Kinetic Constraints in the Specific Interaction between Phosphorylated Ubiquitin and Proteasomal Shuttle Factors

Biomolecules ◽

10.3390/biom11071008 ◽

2021 ◽

Vol 11 (7) ◽

pp. 1008

Author(s):

Ling-Yun Qin ◽

Zhou Gong ◽

Kan Liu ◽

Xu Dong ◽

Chun Tang

Keyword(s):

Exchange Rate ◽

Self Assembly ◽

Solution Structure ◽

Specific Interaction ◽

Dissociation Rate ◽

Fine Tuning ◽

Binding Mechanism ◽

Kinetics Analysis ◽

Kinetic Constraint ◽

Thermodynamic Basis

Ubiquitin (Ub) specifically interacts with the Ub-associating domain (UBA) in a proteasomal shuttle factor, while the latter is involved in either proteasomal targeting or self-assembly coacervation. PINK1 phosphorylates Ub at S65 and makes Ub alternate between C-terminally relaxed (pUbRL) and retracted conformations (pUbRT). Using NMR spectroscopy, we show that pUbRL but not pUbRT preferentially interacts with the UBA from two proteasomal shuttle factors Ubqln2 and Rad23A. Yet discriminatorily, Ubqln2-UBA binds to pUb more tightly than Rad23A does and selectively enriches pUbRL upon complex formation. Further, we determine the solution structure of the complex between Ubqln2-UBA and pUbRL and uncover the thermodynamic basis for the stronger interaction. NMR kinetics analysis at different timescales further suggests an indued-fit binding mechanism for pUb-UBA interaction. Notably, at a relatively low saturation level, the dissociation rate of the UBA-pUbRL complex is comparable with the exchange rate between pUbRL and pUbRT. Thus, a kinetic constraint would dictate the interaction between Ub and UBA, thus fine-tuning the functional state of the proteasomal shuttle factors.

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Template-Free Self-Assembly of Two-Dimensional Polymers into Nano/Microstructured Materials

Molecules ◽

10.3390/molecules26113310 ◽

2021 ◽

Vol 26 (11) ◽

pp. 3310

Author(s):

Shengda Liu ◽

Jiayun Xu ◽

Xiumei Li ◽

Tengfei Yan ◽

Shuangjiang Yu ◽

...

Keyword(s):

Self Assembly ◽

Recent Progress ◽

Two Dimensional ◽

Subsequent Removal ◽

The Past ◽

2D Polymers ◽

Template Free ◽

Self Assembled ◽

The Relationship ◽

Polymer Tubes

In the past few decades, enormous efforts have been made to synthesize covalent polymer nano/microstructured materials with specific morphologies, due to the relationship between their structures and functions. Up to now, the formation of most of these structures often requires either templates or preorganization in order to construct a specific structure before, and then the subsequent removal of previous templates to form a desired structure, on account of the lack of “self-error-correcting” properties of reversible interactions in polymers. The above processes are time-consuming and tedious. A template-free, self-assembled strategy as a “bottom-up” route to fabricate well-defined nano/microstructures remains a challenge. Herein, we introduce the recent progress in template-free, self-assembled nano/microstructures formed by covalent two-dimensional (2D) polymers, such as polymer capsules, polymer films, polymer tubes and polymer rings.

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General Interfacial Self‐Assembly Engineering for Patterning Two‐Dimensional Polymers with Cylindrical Mesopores on Graphene

Angewandte Chemie International Edition ◽

10.1002/anie.201903684 ◽

2019 ◽

Vol 58 (30) ◽

pp. 10173-10178 ◽

Cited By ~ 25

Author(s):

Hao Tian ◽

Jieqiong Qin ◽

Dan Hou ◽

Qian Li ◽

Chen Li ◽

...

Keyword(s):

Self Assembly ◽

Two Dimensional

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Percolation in two-dimensional nanoparticle films from colloidal self-assembly

physica status solidi (a) ◽

10.1002/pssa.200675351 ◽

2007 ◽

Vol 204 (6) ◽

pp. 1856-1862 ◽

Cited By ~ 6

Author(s):

Ching-Ling Hsu ◽

Szu-Ming Chu ◽

Kiwi Wood ◽

Yi-Rong Yang

Keyword(s):

Self Assembly ◽

Two Dimensional ◽

Nanoparticle Films

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Self-assembly of carbon nanotubes into two-dimensional geometries using DNA origami templates

Nature Nanotechnology ◽

10.1038/nnano.2009.311 ◽

2009 ◽

Vol 5 (1) ◽

pp. 61-66 ◽

Cited By ~ 445

Author(s):

Hareem T. Maune ◽

Si-ping Han ◽

Robert D. Barish ◽

Marc Bockrath ◽

William A. Goddard III ◽

...

Keyword(s):

Carbon Nanotubes ◽

Self Assembly ◽

Dna Origami ◽

Two Dimensional

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Square-grid coordination networks of (5,10,15,20-tetra-4-pyridylporphyrinato)zinc(II) in its clathrate with two guest molecules of 1,2-dichlorobenzene: supramolecular isomerism of the porphyrin self-assembly

Acta Crystallographica Section C Crystal Structure Communications ◽

10.1107/s0108270109005691 ◽

2009 ◽

Vol 65 (3) ◽

pp. m139-m142 ◽

Cited By ~ 10

Author(s):

Rajesh Koner ◽

Israel Goldberg

Keyword(s):

Self Assembly ◽

Metal Ion ◽

Three Dimensional ◽

Two Dimensional ◽

Coordination Networks ◽

Guest Molecules ◽

Square Grid ◽

Supramolecular Isomerism ◽

Self Assembled ◽

Solvent Molecules

The title compound, (5,10,15,20-tetra-4-pyridylporphyrinato)zinc(II) 1,2-dichlorobenzene disolvate, [Zn(C40H24N8)]·2C6H4Cl2, contains a clathrate-type structure. It is composed of two-dimensional square-grid coordination networks of the self-assembled porphyrin moiety, which are stacked one on top of the other in a parallel manner. The interporphyrin cavities of the overlapping networks combine into channel voids accommodated by the dichlorobenzene solvent. Molecules of the porphyrin complex are located on crystallographic inversion centres. The observed two-dimensional assembly mode of the porphyrin units represents a supramolecular isomer of the unique three-dimensional coordination frameworks of the same porphyrin building block observed earlier. The significance of this study lies in the discovery of an additional supramolecular isomer of the rarely observed structures of metalloporphyrins self-assembled directly into extended coordination polymers without the use of external ligand or metal ion auxiliaries.

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