ペプトイド配列が2次元集合のメカニズムと動態に及ぼす影響(Influence of Peptoid Sequence on the Mechanisms and Kinetics of 2D Assembly)

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2024-06-24 パシフィック・ノースウェスト国立研究所(PNNL)

この研究では、ペプトイドという分子がミカ表面で2D(二次元)結晶シートを自己組織化する際の機構と動力学、および分子間相互作用が組み立て速度に与える影響を調査しました。ペプトイドは、高い化学的安定性や自己修復能力などの特異な性質を持つ2D材料を形成する能力があります。研究では、ペプトイド配列の詳細がこれらの材料の熱力学的安定性と組み立て速度に大きく影響することが示されました。この発見は、機能的コンポーネントとの共組立てに向けた今後の研究の扉を開きます。

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ペプトイドの配列が2次元集合の機構と速度論に及ぼす影響 Influence of Peptoid Sequence on the Mechanisms and Kinetics of 2D Assembly

Sakshi Yadav Schmid, Xiang Ma, Joshua A. Hammons, Sebastian T. Mergelsberg, Bradley S. Harris, Thomas Ferron, Wenchao Yang, Wenhao Zhou, Renyu Zheng, Shuai Zhang, Benjamin Adam Legg, Anthony Van Buuren, Marcel D. Baer, Chun-Long Chen, Jinhui Tao, and James J. De Yoreo
ACS Nano  Published:January 12, 2024
DOI:https://doi.org/10.1021/acsnano.3c10810

Abstract

ペプトイド配列が2次元集合のメカニズムと動態に及ぼす影響(Influence of Peptoid Sequence on the Mechanisms and Kinetics of 2D Assembly)

Two-dimensional (2D) materials have attracted intense interest due to their potential for applications in fields ranging from chemical sensing to catalysis, energy storage, and biomedicine. Recently, peptoids, a class of biomimetic sequence-defined polymers, have been found to self-assemble into 2D crystalline sheets that exhibit unusual properties, such as high chemical stability and the ability to self-repair. The structure of a peptoid is close to that of a peptide except that the side chains are appended to the amide nitrogen rather than the α carbon. In this study, we investigated the effect of peptoid sequence on the mechanism and kinetics of 2D assembly on mica surfaces using in situ AFM and time-resolved X-ray scattering. We explored three distinct peptoid sequences that are amphiphilic in nature with hydrophobic and hydrophilic blocks and are known to self-assemble into 2D sheets. The results show that their assembly on mica starts with deposition of aggregates that spread to establish 2D islands, which then grow by attachment of peptoids, either monomers or unresolvable small oligomers, following well-known laws of crystal step advancement. Extraction of the solubility and kinetic coefficient from the dependence of the growth rate on peptoid concentration reveals striking differences between the sequences. The sequence with the slowest growth rate in bulk and with the highest solubility shows almost no detachment; i.e., once a growth unit attaches to the island edge, there is almost no probability of detaching. Furthermore, a peptoid sequence with a hydrophobic tail conjugated to the final carboxyl residue in the hydrophilic block has enhanced hydrophobic interactions and exhibits rapid assembly both in the bulk and on mica. These assembly outcomes suggest that, while the π–π interactions between adjacent hydrophobic blocks play a major role in peptoid assembly, sequence details, particularly the location of charged groups, as well as interaction with the underlying substrate can significantly alter the thermodynamic stability and assembly kinetics.

1700応用理学一般
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