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Molecular self-assembly of peptides into ordered nanotubes is highly important for various technological applications. Very short peptide building blocks, as short as dipeptides, can form assemblies with unique mechanical, optical, piezoelectric, and semiconductive properties. Yet, the control over nanotube length in solution has remained challenging, due to the inherent sequential self-assembly mechanism. Here, in line with polymer chemistry paradigms, we applied a supramolecular polymer coassembly methodology to modulate peptide nanotube elongation. Utilizing this approach, we achieved a narrow, controllable nanotube length distribution by adjusting the molecular ratio of the diphenylalanine assembly unit and its end-capped analogue. Kinetic analysis suggested a slower coassembly organization process as compared to the self-assembly dynamics of each of the building blocks separately. This is consistent with a hierarchal arrangement of the peptide moieties within the coassemblies. Mass spectrometry analysis demonstrated the bimolecular composition of the coassembled nanostructures. Moreover, the peptide nanotubes' length distribution, as determined by electron microscopy, was shown to fit a fragmentation kinetics model. Our results reveal a simple and efficient mechanism for the control of nanotube sizes through the coassembly of peptide entities at various ratios, allowing for the desired end-product formation. This dynamic size control offers tools for molecular engineering at the nanoscale exploiting the advantages of molecular coassembly.
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http://dx.doi.org/10.1021/acsnano.6b01587 | DOI Listing |
Mikrochim Acta
December 2024
State Key Laboratory of Supramolecular Structure and Materials, Jilin University, Changchun, 130012, People's Republic of China.
A highly sensitive aptamer sensor (aptasensor) is proposed based on metal-organic frameworks-silver nanoparticles (AgNPs@MOF) to detect sulfadimethoxine (SDM) by surface-enhanced Raman spectroscopy (SERS). AgNPs@MOF with SERS activity was successfully fabricated by synthesizing AgNPs in situ on the surface of MIL-101(Fe), and SDM aptamer and Raman reporter 4-aminophenthiophenol (4-ATP) were selected as specific recognition elements and signal probes, respectively. When SDM was absent, the SDM aptamers were effectively adsorbed on the surface of AgNPs@MOF, thus keeping AgNPs@MOF in a dispersed state, resulting in a weakened SERS signal of 4-ATP.
View Article and Find Full Text PDFSmall
December 2024
Chemical Biology Unit, Institute of Nano Science and Technology (INST), Sector 81, Mohali, Punjab, 140306, India.
Dynamic peptide networks represent an attractive structural space of supramolecular polymers in the realm of emergent complexity. Point mutations in the peptide sequence exert profound effects over the landscapes of self-assembly with an intricate interplay among the structure-function relationships. Herein, the pathway complexity of an arginine-rich peptide is studied, FmocVFFARR derived by the mutation of minimalist amyloid-inspired peptide amphiphile FmocVFFAKK, thereby focusing on its pathway-dependent self-assembly behavior.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2024
State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry, Jilin University, NO.2699 Qianjin Street, Chaoyang District, 130000, Changchun, CHINA.
Carbonized polymer dots (CPDs) are a class of exceptional fluorescent materials with diverse applications. However, their photoluminescence (PL) mechanism remained enigmatic and controversial, hindering further development and application. While molecular fluorophores explain primary fluorescence in some CPDs, the overall PL of CPDs still cannot be fully explained, such as their excitation-dependent behaviors, let alone the modulation of PL.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2024
Donghua University - Songjiang Campus: Donghua University, College of chemistry, chemical engineering and biotechnology, 2999 Renmin North Road, Shanghai, 201620, Shanghai, CHINA.
Developing new organic radical emission systems and regulating their luminescence properties presents a significant challenge. Herein, we build dynamic and multi-emission band radical luminescence systems by co-assembling inorganic metal salts with carbonyl compounds in ionic liquids. After the assembling, dual-band, and excitation wavelength-dependent emission was observed upon light irradiation, one emission band originates from carbonyl radical after light irradiation, the other band from the ligand-metal charge transfer (LMCT) state, which benefits from the charge transfer from the radicals to the metal salts.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2024
South China University of Technology, South China Advanced Institute for Soft Matter Science and Technology, South China Advanced Institute for Soft Matter Science and Technology, 510640, Guangzhou, CHINA.
Nanoimprint lithography (NIL) has been broadly applied in the fabrication of nano-patterned polymer films for cost-efficiency and high through-put; however, the intrinsic tradeoff between mechanical strength and residual stress of polymer films significantly limits the NIL resolution while the harsh processing conditions limit its versatile applications to different substrates. Herein, 1 nm metal oxide cluster, phosphotungstic acid (PTA), is used to complexed with polyvinyl alcohol (PVA) for high-resolution NIL that can be operated at large-scale and mild conditions. The ultra-small size of PTA enables dense supramolecular interaction with PVA for the diminished crystallinity and accelerated chain dynamics that help relax the residual stress during film casting.
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