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Molecular configuration-mediated thermo-responsiveness in oligo(ethylene glycol) derivatives attached on gold nanoparticles

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Title: Molecular configuration-mediated thermo-responsiveness in oligo(ethylene glycol) derivatives attached on gold nanoparticles
Authors: Xiong, Kun Browse this author
Mitomo, Hideyuki Browse this author →KAKEN DB
Su, Xueming Browse this author
Shi, Yier Browse this author
Yonamine, Yusuke Browse this author →KAKEN DB
Sato, Shin-ichiro Browse this author →KAKEN DB
Ijiro, Kuniharu Browse this author →KAKEN DB
Issue Date: 26-Mar-2021
Publisher: Royal Society of Chemistry
Journal Title: Nanoscale advances
Publisher DOI: 10.1039/d1na00187f
Abstract: Biomolecular systems actively control their local environment on a sub-nm scale via changes in molecular configuration from their flexible structures and derive emergent functions. Although this functional emergence based on local environmental control is attracting a great deal of attention in chemistry, it remains challenging to realize this artificially. Herein, we report the tuning of the thermo-responsive properties of oligo(ethylene glycol) (OEG) derivatives attached on gold nanoparticles via local environmental control not only by the hydrophobic moiety at their terminus but also by their molecular configuration. OEG-attached alkane thiol-modified AuNPs showed thermo-responsive assembly/disassembly in water through the hydration/dehydration of the OEG portions in a manner dependent both on the hydrophobicity at their terminus and the surface curvature of the core nanoparticles. Further, the assembly temperature (T-A) was also tuned by ligand mixing with a non-thermo-responsive ligand with a shorter OEG length. Molecular dynamics simulations show that the distribution of the hydrophobic terminus in the normal direction along the gold surface varied in accordance with the surface curvature, indicating variations in molecular configuration. It is expected that a bent configuration could accelerate the thermo-responsiveness of OEG by allowing them greater accessibility to the hydrophobic terminus. Experimental and simulation results support the notion that local OEG density tuning by surface curvature or ligand mixing with a different OEG length leads to different degrees of accessibility to the hydrophobic terminus via changes in molecular configuration, promoting local environmental control-directed assembly temperature tuning.
Type: article
Appears in Collections:電子科学研究所 (Research Institute for Electronic Science) > 雑誌発表論文等 (Peer-reviewed Journal Articles, etc)

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