Despite recent advances in the assembly of organic nanotubes, conferral of sequence-defined engineering and dynamic response characteristics to the tubules remains a challenge. Here we report a new family of highly designable and dynamic nanotubes assembled from sequence-defined peptoids through a unique “rolling-up and closure of nanosheet” mechanism. During the assembly process, amorphous spherical particles of amphiphilic peptoid oligomers crystallize to form well-defined nanosheets before folding to form single-walled nanotubes. These nanotubes undergo a pH-triggered, reversible contraction–expansion motion. By varying the number of hydrophobic residues of peptoids, we demonstrate tuning of nanotube wall thickness, diameter, and mechanical properties. Atomic force microscopy-based mechanical measurements show peptoid nanotubes are highly stiff (Young’s Modulus ~13–17 GPa). We further demonstrate the precise incorporation of functional groups within nanotubes and their applications in water decontamination and cellular adhesion and uptake. These nanotubes provide a robust platform for developing biomimetic materials tailored to specific applications.
Photocatalysts possessing high efficiency in degrading aquatic organic pollutants are highly desirable. Although graphene-based nanocomposites exhibit excellent photocatalytic properties, the role of graphene has been largely underestimated. Herein, the photothermal effect of graphene-based nanocomposites is demonstrated to play an important role in the enhanced photocatalytic performance, which has not been considered previously. In our study on degradation of organic pollutants (methylene blue), the contribution of the photothermal effect caused by a nanocomposite consisting of P25 and reduced graphene oxide can be as high as ∼38% in addition to trapping and shuttling photogenerated electrons and increasing both light absorption and pollutant adsorptivity. The result reveals that the photothermal characteristic of graphene-based nanocomposite is vital to photocatalysis. It implies that designing graphene-based nanocomposites with the improved photothermal performance is a promising strategy to acquire highly efficient photocatalytic activity.
SiC nanocrystals (NCs) exhibit unique surface chemistry and possess special properties. This provides the opportunity to design suitable surface structures by terminating the surface dangling bonds with different atoms thereby boding well for practical applications. In this article, we report the photoluminescence properties of 3C-SiC NCs in water suspensions with different pH values. Besides a blue band stemming from the quantum confinement effect, the 3C-SiC NCs show an additional photoluminescence band at 510 nm when the excitation wavelengths are longer than 350 nm. Its intensity relative to the blue band increases with the excitation wavelength. The 510 nm band appears only in acidic suspensions but not in alkaline ones. Fourier transform infrared, X-ray photoelectron spectroscopy, and X-ray absorption near-edge structure analyses clearly reveal that the 3C-SiC NCs in the water suspension have Si-H and Si-OH bonds on their surface, implying that water molecules only react with a Si-terminated surface. First-principle calculations suggest that the additional 510 nm band arises from structures induced by H(+) and OH(-) dissociated from water and attached to Si dimers on the modified (001) Si-terminated portion of the NCs. The size requirement is consistent with the observation that the 510 nm band can only be observed when the excitation wavelengths are relatively large, that is, excitation of bigger NCs.
Hexagonal hierarchical microtubular structures are produced by diphenylalanine self-assembly and the ratio of the relative humidity in the growth chamber to the diphenylalanine concentration (defined as the RH-FF ratio) determines the microtubular morphology. The hexagonal arrangement of the diphenylalanine molecules first induces the hexagonal nanotubes with opposite charges on the two ends, and the dipolar electric field on the nanotubes serves as the driving force. Side-by-side hexagonal aggregation and end-to-end arrangement ensue finally producing a hexagonal hierarchical microtubular structure. Staining experiments and the external electric field-induced parallel arrangement provide evidence of the existence of opposite charges and dipolar electric field. In this self-assembly, the different RH-FF ratios induce different contents of crystalline phases. This leads to different initial nanotube numbers finally yielding different microtubular morphologies. Our calculation based on the dipole model supports the dipole-field mechanism that leads to the different microtubular morphologies.
Spontaneous polarization reversal: Saturated polarization–electric field loops with a concave region were obtained from diphenylalanine peptide microtubes (FF PMTs) by combining the action of light during the hysteresis loop measurements (see picture; Ec=coercive field). The existence of ferroelectricity in FF peptide nanostructures was shown experimentally. The ferroelectricity of the FF PMTs is expected to extend their applications to biomedicine and microelectronics.
Good understanding of the reaction mechanism in the electrochemical reduction of water to hydrogen is crucial to renewable energy technologies. Although previous studies have revealed that the surface properties of materials affect the catalytic reactivity, the effects of a catalytic surface on the hydrogen evolution reaction (HER) on the molecular level are still not well understood. Contrary to general belief, water molecules do not adsorb onto the surfaces of 3C-SiC nanocrystals (NCs), but rather spontaneously dissociate via a surface autocatalytic process forming a complex consisting of -H and -OH fragments. In this study, we show that ultrathin 3C-SiC NCs possess superior electrocatalytic activity in the HER. This arises from the large reduction in the activation barrier on the NC surface enabling efficient dissociation of H(2)O molecules. Furthermore, the ultrathin 3C-SiC NCs show enhanced HER activity in photoelectrochemical cells and are very promising to the water splitting based on the synergistic electrocatalytic and photoelectrochemical actions. This study provides a molecular-level understanding of the HER mechanism and reveals that NCs with surface autocatalytic effects can be used to split water with high efficiency thereby enabling renewable and economical production of hydrogen.
Tungsten trioxide dihydrate (WO3·2H2O) nanoplates are prepared by in situ anodic oxidation of tungsten disulfide (WS2) film on carbon fiber paper (CFP). The WO3·2H2O/WS2 hybrid catalyst exhibits excellent synergistic effects which facilitate the kinetics of the hydrogen evolution reaction (HER). The electrochromatic effect takes place via hydrogen intercalation into WO3·2H2O. This process is accelerated by the desirable proton diffusion coefficient in the layered WO3·2H2O. Hydrogen spillover from WO3·2H2O to WS2 occurs via atomic polarization caused by the electric field of the charges on the planar defect or edge active sites of WS2. The optimized hybrid catalyst presents a geometrical current density of 100 mA cm(-2) at 152 mV overpotential with a Tafel slope of ∼54 mV per decade, making the materials one of the most active nonprecious metal HER catalysts.
Photoluminescence (PL) spectra reveal that deficiency of water molecules in the channel cores of bioinspired hierarchical diphenylalanine ( L -Phe- L -Phe, FF) peptide nanotubes (PNTs) not only modifies the bandgap of the subnanometer crystalline structure formed by the self-assembly process, but also induces a characteristic ultraviolet PL peak the position of which is linearly proportional to the number of water molecules in the PNTs. Addition or loss of water molecules gives rise to the UV PL redshift or blueshift. Density functional theory calculation also confirms that addition of water molecules to the PNTs causes splitting of the valence-band peak, which corresponds to the shift and splitting of the observed UV PL peak. Water molecules play an important role in the biological properties of FF PNTs and the results demonstrate that the PL spectra can be used to probe the number of water molecules bonded to the FF molecules.
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