NiO is a promising hole transporting material for perovskite solar cells due to its high hole mobility, good stability, easy processibility, and suitable Fermi level for hole extraction. However, the efficiency of NiO‐based cells is still limited by the slow hole extraction due to the poor perovskite/NiO interface and the inadequate quality of the two solution‐processed material phases. Here, large influences of a monolayer surface modification of NiO nanocrystal layers with ethanolamine molecules are demonstrated on the enhancement of hole extraction/transport and thus the photovoltaic performance. The underlying causes have been revealed by a series of studies, pointing to a favorable dipole layer formed by the molecular adsorption along with the enhanced perovskite crystallization and the improved interface contact. Comparatively, the solar cells based on a diethanolamine‐modified NiO layer have achieved a rather high fill factor, indeed one of the highest among NiO‐based perovskite solar cells, and high short‐circuit photocurrent density (Jsc), resulting in a power conversion efficiency of ≈16%, most importantly, without hysteresis.
One-dimension noble nanomaterials have promising applications in many fields, and their growth pattern control is significant to property modulation. Herein, we report a facile strategy with which the growth pattern of Ag on the Au nanorod (NR) or decahedral nanoparticle (NP) surface can be precisely controlled and various structured Ag/Au NRs can be synthesized. Achievement of growth pattern control is mainly attributed to the adjustable reaction kinetics of Ag– to Ag0. Slow and moderate reaction rate favor asymmetrical growth, producing Au-tipped Ag NRs and asymmetrical Ag–Au–Ag NRs, respectively. In the case of a fast reaction rate, symmetrical growth dominates and symmetrical Ag–Au–Ag NRs form. Furthermore, the prepared bimetallic NRs can be used as starting materials to generate other novel nanostructures (nanocups, nanonails, and longer Au-tipped Ag NRs). The result presented here is vital to both exploration of growth theory and constructing nanostructures of not only the Au/Ag bimetallic system but also possibly other noble bimetallic systems. Moreover, these prepared nanostructures could provide model materials for studying the physical properties (such as structure-dependent surface plasmon) or have potential applications in the medical field. For example, hollow nanocups can serve as containers for controlled release of drug, etc.
Engineering a versatile oncotherapy nanoplatform integrating both diagnostic and therapeutic functions has always been an intractable challenge in targeted cancer treatment. Herein, to actualize the theme of precise medicine, a nanoplatform is developed by anchoring Mn-Cdots to doxorubicin (DOX)-loaded mesoporous silica-coated gold cube-in-cubes core/shell nanocomposites and further conjugating them to a Arg-Gly-Asp (RGD) peptide (denoted as RGD-CCmMC/DOX) to achieve an active-targeting effect. Under 635 nm irradiation, the nanoplatform acts as oxygen nanogenerator that produces O2 in situ and amplifies the content of singlet oxygen (1O2) in the hypoxic tumor microenvironment (TME), which has been demonstrated to attenuate tumor hypoxia and synchronously enhance photodynamic efficacy. Moreover, the gold cube-in-cube core in this work has been proven as a photothermal agent for hyperthermia, which exhibits a favorable photothermal effect with a 65.6% calculated photothermal conversion efficiency under 808 nm irradiation. In addition, the nanoplatform achieves heat- and pH-sensitive drug release with precise control to specific-tumor sites, executing combined chemo-phototherapy functions. Besides, it functions as a multimodal bioimaging agent of photothermal, fluorescence, and magnetic resonance imaging for the accurate diagnosis and guidance of therapy. As validated by in vivo and in vitro assays, the TME-responsive nanoplatform is highly biocompatible and effectively obliterates 4T1 tumor xenografts on nude mice after triple-synergetic treatment. This work presents a rational design of versatile nanoplatforms, which modulate the TME to enable high therapeutic performance and multiplexed imaging, which provides an innovative paradigm for targeted tumor therapy.
Cancer nanotheranostics, integrating both diagnostic and therapeutic functions into nanoscale agents, are advanced solutions for cancer management. Herein, a light‐responsive biodegradable nanorattle‐based perfluoropentane‐(PFP)‐filled mesoporous‐silica‐film‐coated gold nanorod (GNR@SiO2‐PFP) is strategically designed and prepared for enhanced ultrasound (US)/photoacoustic (PA) dual‐modality imaging guided photothermal therapy of melanoma. The as‐prepared nanorattles are composed of a thin mesoporous silica film as the shell, which endows the nanoplatform with flexible morphology and excellent biodegradability, as well as large cavity for PFP filling. Upon 808 nm laser irradiation, the loaded PFP will undergo a liquid–gas phase transition due to the heat generation from GNRs, thus generating nanobubbles followed by the coalescence into microbubbles. The conversion of nanobubbles to microbubbles can improve the intratumoral permeation and retention in nonmicrovascular tissue, as well as enhance the tumor‐targeted US imaging signals. This nanotheranostic platform exhibits excellent biocompatibility and biodegradability, distinct gas bubbling phenomenon, good US/PA imaging contrast, and remarkable photothermal efficiency. The results demonstrate that the GNR@SiO2‐PFP nanorattles hold great potential for cancer nanotheranostics.
Due to its intrinsic structure and characteristics, small size and monodispersity, control of singlecrystalline Cu 2 O polyhedra in aqueous media is a challenge, which is important to overcome to achieve enhanced photocatalytic activity. Here, we use heterogeneous nucleation, rather than homogeneous nucleation, of Cu 2 O with gold nanorods as seeds to realize subsequent uniform crystal growth. We obtained nearly monodisperse octahedral Au@Cu 2 O nanocrystals with single-crystalline shells, which are distinct from the pentagonal column-shaped structures previously described. Due to the fact that one Au@Cu 2 O holds only one Au nanorod, two formulas were deduced for convenient size control of the Cu 2 O shell. The formulas were calculated by adjusting the amount of Au rods that are relatively quantified. The formula also allows the size of the final product to be predicted when a given amount of gold seeds are employed. The experimental results agree well with the calculated data. The result of larger surface area and improved charge separation from core-shell interaction, made five samples of different sizes exhibit excellent photocatalytic activity toward MO degradation. The synthetic strategy reported here provides a clue to monodispersity and size control of core-shell nanocrystals, which is useful in developing new catalysts with better performance that are urgently needed in the fields of both science and technology.
The limited efficacy of “smart” nanotheranostic agents in eradicating tumors calls for the development of highly desirable nanoagents with diagnostics and therapeutics. Herein, to surmount these challenges, we constructed an intelligent nanoregulator by coating a mesoporous carbon nitride (C3N4) layer on a core–shell nitrogen-doped graphene quantum dot (N-GQD)@hollow mesoporous silica nanosphere (HMSN) and decorated it with a P-PEG-RGD polymer, to achieve active-targeting delivery (designated as R-NCNP). Upon irradiation, the resultant R-NCNP nanoregulators exhibit significant catalytic breakdown of water molecules, causing a sustainable elevation of oxygen level owing to the C3N4 shell, which facilitates tumor oxygenation and relieves tumor hypoxia. The generated oxygen bubbles serve as an echogenic source, triggering tissue impedance mismatch, thereby enhancing the generation of an echogenicity signal, making them laser-activatable ultrasound imaging agents. In addition, the encapsulated photosensitizers and C3N4-layered photosensitizer are simultaneously activated to maximize the yield of ROS, actualizing a triple-photosensitizer hybrid nanosystem exploited for enhanced PDT. Intriguingly, the N-GQDs endow the R-NCNP nanoregulator with a photothermal effect for hyperthemia, making it exhibit considerable photothermal outcomes and infrared thermal imaging (IRT). Importantly, further analysis reveals that the polymer-modified R-NCNPs actively target specific tumor tissues and display a triple-modal US/IRT/FL imaging-assisted cooperative PTT/PDT for real-time monitoring of tumor ablation and therapeutic evaluation. The rational synergy of triple-model PDT and efficient PTT in the designed nanoregulator confers excellent anticancer effects, as evidenced by in vitro and in vivo assays, which might explore more possibilities in personalized cancer treatment.
We present a strategy to achieve heterogeneous seeded growth on nanoparticle (NP) surfaces and construct various Pt nanostructures (cage- and ring-like) by using selective etching as surface-free-energy-distribution modifier. Preprepared Au polyhedron NPs (octahedron, decahedron, nanorod, and nanoplate) are mixed with KI, H(2)PtCl(6), and surfactant. Under heating, KI is first oxidized to I(2), which then selectively etches the edges of Au polyhedrons. Consequently, the partial removal of surface Au atoms creates highly active sites (exposed high-index facets, atom steps, and kinks) on the etched edges. Then the reduced Pt(0) atoms deposit on the etched edges preferentially and grow further, generating bimetallic nanostructures, Au octahedrons, or decahedrons with edges coated by Pt. The Pt layer protects the Au on the etched edges against further etching, changing the etching route and causing the Au on {111} facets without a Pt layer to be etched. After the Au is removed completely from the bimetallic nanostructures, ring-like, frame-like, and octahedral cage-like Pt nanostructures form. The evolution from Au polyhedrons to Pt ring or octahedron cage is investigated systematically by high-resolution transmission electron microscopy, transmission electron microscopy, scanning electron microscopy, energy-dispersive X-ray, scanning transmission electron microscopy, and high-angle annular dark field.
A series of α,ω-aldehyde end-capped oligomers of thiophene with three, four, five, six, and eight thiophene units have been synthesized using the palladium-catalyzed Stille's coupling reactions. The UV−vis spectral data indicate that these aldehyde end-capped oligomers have longer conjugation lengths as evidenced by the higher λmax values than the corresponding unsubstituted oligothiophenes. The λmax value increases as the number of thiophene units is increased. The intrinsic conductivity of the solution-cast films of the aldehyde end-capped oligothiophenes is generally higher than that of their corresponding unsubstituted counterparts. Other α,ω-substituted sexithiophenes, such as n-dodecanoyl, tert-butyldimethylsilyl, hydroxymethyl, and [(n-butoxyethoxy)ethoxy]methyl sexithiophenes, have also been synthesized. α,ω-Bis([(n-butoxyethoxy)ethoxy]methyl)sexithiophene has a remarkably high solubility in chloroform (1.8 g/L) and a conductivity (1 × 10-6 S/cm) comparable to the unsubstituted sexithiophene.
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