Near-infrared plasmonic nanoparticles demonstrate great potential in disease theranostic applications. Herein a nanoplatform, composed of mesoporous silica-coated gold nanorods (AuNRs), is tailor-designed to optimize the photodynamic therapy (PDT) for tumor based on the plasmonic effect. The surface plasmon resonance of AuNRs was fine-tuned to overlap with the exciton absorption of indocyanine green (ICG), a near-infrared photodynamic dye with poor photostability and low quantum yield. Such overlap greatly increases the singlet oxygen yield of incorporated ICG by maximizing the local field enhancement, and protecting the ICG molecules against photodegradation by virtue of the high absorption cross section of the AuNRs. The silica shell strongly increased ICG payload with the additional benefit of enhancing ICG photostability by facilitating the formation of ICG aggregates. As-fabricated AuNR@SiO2-ICG nanoplatform enables trimodal imaging, near-infrared fluorescence from ICG, and two-photon luminescence/photoacoustic tomography from the AuNRs. The integrated strategy significantly improved photodynamic destruction of breast tumor cells and inhibited the growth of orthotopic breast tumors in mice, with mild laser irradiation, through a synergistic effect of PDT and photothermal therapy. Our study highlights the effect of local field enhancement in PDT and demonstrates the importance of systematic design of nanoplatform to greatly enhancing the antitumor efficacy.
Single-site cocatalysts engineered on supports offer a cost-efficient pathway to utilize precious metals, yet improving the performance further with minimal catalyst loading is still highly desirable. Here we have conducted a photochemical reaction to stabilize ultralow Pt co-catalysts (0.26 wt%) onto the basal plane of hexagonal ZnIn2S4 nanosheets (PtSS-ZIS) to form a Pt-S3 protrusion tetrahedron coordination structure. Compared with the traditional defect-trapped Pt single-site counterparts, the protruding Pt single-sites on h-ZIS photocatalyst enhance the H2 evolution yield rate by a factor of 2.2, which could reach 17.5 mmol g−1 h−1 under visible light irradiation. Importantly, through simple drop-casting, a thin PtSS-ZIS film is prepared, and large amount of observable H2 bubbles are generated, providing great potential for practical solar-light-driven H2 production. The protruding single Pt atoms in PtSS-ZIS could inhibit the recombination of electron-hole pairs and cause a tip effect to optimize the adsorption/desorption behavior of H through effective proton mass transfer, which synergistically promote reaction thermodynamics and kinetics.
Herein, the structural effect of MoS as a cocatalyst of photocatalytic H generation activity of g-C N under visible light irradiation is studied. By using single-particle photoluminescence (PL) and femtosecond time-resolved transient absorption spectroscopies, charge transfer kinetics between g-C N and two kinds of nanostructured MoS (nanodot and monolayer) are systematically investigated. Single-particle PL results show the emission of g-C N is quenched by MoS nanodots more effectively than MoS monolayers. Electron injection rate and efficiency of g-C N /MoS -nanodot hybrid are calculated to be 5.96 × 10 s and 73.3%, respectively, from transient absorption spectral measurement, which are 4.8 times faster and 2.0 times higher than those of g-C N /MoS -monolayer hybrid. Stronger intimate junction between MoS nanodots and g-C N is suggested to be responsible for faster and more efficient electron injection. In addition, more unsaturated terminal sulfur atoms can serve as the active site in MoS nanodot compared with MoS monolayer. Therefore, g-C N /MoS nanodot exhibits a 7.9 times higher photocatalytic activity for H evolution (660 µmol g- h ) than g-C N /MoS monolayer (83.8 µmol g h ). This work provides deep insight into charge transfer between g-C N and nanostructured MoS cocatalysts, which can open a new avenue for more rationally designing MoS -based catalysts for H evolution.
The advancement of miniaturized electronic devices requires the development of high-performance microsupercapacitors. The low areal energy density of microsupercapacitors with the interdigitated architecture is the major challenge hindering the application. Here, a simple method for the scalable fabrication of all-solid-state, flexible microsupercapacitors is demonstrated by direct graphene-carbon nanotube composite ink writing technology. The microsupercapacitors demonstrate good electrochemical performance with a high areal energy density of 1.36 µWh cm -2 and power density of 0.25 mW cm -2 , good cycling stability, and excellent mechanical flexibility. The method developed here sheds light on the simple method of preparing high-performance, all-solid-state, flexible microsupercapacitors in a straightforward and scalable process.
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