Here we report a new and simple synthetic pathway to form ordered, hollow carbon nitride structures, using a cyanuric acid-melamine (CM) complex in ethanol as a starting product. A detailed analysis of the optical and photocatalytic properties shows that optimum hollow carbon nitride structures are formed after 8 h of condensation. For this condensation time, we find a significantly reduced fluorescence intensity and lifetime, indicating the formation of new, nonradiative deactivation pathways, probably involving charge-transfer processes. Enhanced charge transfer is seen as well from a drastic increase of the photocatalytic activity in the degradation of rhodamine B dye, which is shown to proceed via photoinduced hole transfer. Moreover, we show that various CM morphologies can be obtained using different solvents, which leads to diverse ordered carbon nitride architectures. In all cases, the CM-C3N4 structures exhibited superior photocatalytic activity compared to the bulk material. The utilization of CM hydrogen-bonded complexes opens new opportunities for the significant improvement of carbon nitride synthesis, structure, and optical properties toward an efficient photoactive material for catalysis.
Quantum‐dot‐sensitized solar cells (QDSCs) are a promising low‐cost alternative to existing photovoltaic technologies such as crystalline silicon and thin inorganic films. The absorption spectrum of quantum dots (QDs) can be tailored by controlling their size, and QDs can be produced by low‐cost methods. Nanostructures such as mesoporous films, nanorods, nanowires, nanotubes and nanosheets with high microscopic surface area, redox electrolytes and solid‐state hole conductors are borrowed from standard dye‐sensitized solar cells (DSCs) to fabricate electron conductor/QD monolayer/hole conductor junctions with high optical absorbance. Herein we focus on recent developments in the field of mono‐ and polydisperse QDSCs. Stability issues are adressed, coating methods are presented, performance is reviewed and special emphasis is given to the importance of energy‐level alignment to increase the light to electric power conversion efficiency.
The investigation of nickel phosphide (Ni5 P4 ) as a catalyst for the hydrogen (HER) and oxygen evolution reaction (OER) in strong acidic and alkaline environment is described. The catalyst can be grown in a 3D hierarchical structure directly on a nickel substrate, thus making it an ideal candidate for practical water splitting devices. The activity of the catalyst towards the HER, together with its high stability especially in acidic solution, makes it one of the best non-noble materials described to date. Furthermore, Ni5 P4 was investigated in the OER and showed activity superior to pristine nickel or platinum. The practical relevance of Ni5 P4 as a bifunctional catalyst for the overall water splitting reaction was demonstrated, with 10 mA cm(-2) achieved below 1.7 V.
Semiconductor Quantum Dots (QDs) currently receive widespread attention for the development of photovoltaic devices due to the possibility of tailoring their optoelectronic properties by the control of size and composition. Here we show that it is possible to design both injection and recombination in QD sensitized solar cells (QDSCs) by the appropriate use of molecular dipoles and conformal coatings. QDSCs have been manufactured using mesoporous TiO(2) electrodes coated with "in situ" grown CdSe semiconductor nanocrystals by chemical bath deposition (CBD). Surface modification of the CdSe sensitized electrodes by conformal ZnS coating and grafting of molecular dipoles (DT) has been explored to both increase the injection from QDs into the TiO(2) matrix and reduce the recombination of the QD sensitized electrodes. Different sequences of both treatments have been tested aiming at boosting the energy conversion efficiency of the devices. The obtained results showed that the most favorable sequence of the surface treatment (DT+ZnS) led to a dramatic 600% increase of photovoltaic performance compared to the reference electrode (without modification): V(oc) = 0.488 V, j(sc) = 9.74 mA/cm(2), FF = 0.34, and efficiency = 1.60% under full 1 sun illumination. The measured photovoltaic performance was correlated to the relative position of the CdSe conduction band (characterized by surface photovoltage measurements) and TiO(2) conduction band (characterized by the chemical capacitance, C(mu)) together with recombination resistance, R(rec).
Efficient, robust and low-cost nickel nitride electrocatalyst on nickel foam demonstrates high performance in water splitting and oxygen reduction reactions.
The synthesis of vertically aligned functional graphitic carbon nanosheets (CNS) is challenging. Herein, we demonstrate a general approach for the fabrication of vertically aligned CNS and metal carbide@CNS composites via a facile salt templating induced self-assembly. The resulting vertically aligned CNS and metal carbide@CNS structures possess ultrathin walls, good electrical conductivity, strong adhesion, excellent structural robustness, and small particle size. In electrochemical energy conversion and storage such unique features are favorable for providing efficient mass transport as well as a large and accessible electroactive surface. The materials were tested as electrodes in a lithium ion battery and in electrochemical water splitting. The vertically aligned nanosheets exhibit remarkable lithium ion storage properties and, concurrently, excellent properties as electrocatalysts for hydrogen evolution.
ARTICLE systems for comparison. A CdSe QD-sensitized photoelectrode was used in conjunction with an aqueous polysulfide electrolyte and the PbS-CE to record IÀV measurements under illumination and to compare the solar cell performance to a cell with a Pt-CE. Our results show that the PbS-CE reported here provides better performance while bypassing contamination problems known from alternative materials.
Quantum dot sensitized solar cells (QDSSC) may benefit from the ability to tune the quantum dot optical properties and band gap through the manipulation of their size and composition. Moreover, the inorganic nanocrystals may provide increased stability compared to organic sensitizers. We report the facile fabrication of QDSSC by electrophoretic deposition of CdSe QDs onto conducting electrodes coated with mesoporous TiO(2). Unlike prior chemical linker-based methods, no pretreatment of the TiO(2) was needed, and deposition times as short as 2 h were sufficient for effective coating. Cross-sectional chemical analysis shows that the Cd content is nearly constant across the entire TiO(2) layer. The dependence of the deposition on size was studied and successfully applied to CdSe dots with diameters between 2.5 and 5.5 nm as well as larger CdSe quantum rods. The photovoltaic characteristics of the devices are greatly improved compared with those achieved for cells prepared with a linker approach, reaching efficiencies as high as 1.7%, under 1 sun illumination conditions, after treating the coated electrodes with ZnS. Notably, the absorbed photon to electron conversion efficiencies did not show a clear size-dependence indicating efficient electron injection even for the larger QD sizes. The electrophoretic deposition method can be easily expanded and applied for preparations of QDSSCs using diverse colloidal quantum dot and quantum rod materials for sensitization.
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