Chemically synthesized InP nanocrystals (NCs) are drawing a large interest as a potentially less toxic alternative to CdSebased nanocrystals. With a bulk band gap of 1.35 eV and an exciton Bohr radius of ∼10 nm the emission wavelength of InP NCs can in principle be tuned throughout the whole visible and near-infrared range by changing their size. Furthermore, a few works reported fluorescence quantum yields exceeding 70% after overcoating the core NCs with appropriate shell materials. Therefore, InP NCs are very promising for use in lighting and display applications. On the other hand, a number of challenges remain to be addressed in order to progress from isolated research results to robust and reproducible synthesis methods for high quality InP NCs. First of all, the size distribution of the as-synthesized NCs needs to be reduced, which directly translates into more narrow emission line widths. Next, reliable protocols are required for achieving a given emission wavelength at high reaction yield and for further improving the emission efficiency and chemical and photostability. Advances in these directions have been hampered for a long time by the specific properties of InP, such as the rather covalent nature of binding implying harsh synthesis conditions, high sensitivity toward oxidation, and limited choice of phosphorus precursors. However, in recent years a much better understanding of the precursor conversion kinetics and reaction mechanisms has been achieved, giving this field new impulse. In this review we provide a comprehensive overview from initial synthetic approaches to the most recent developments. First, we highlight the fundamental differences in the syntheses of InPbased NCs with respect to established II−VI and IV−VI semiconductor NCs comparing their nucleation and growth stages. Next, we inspect in detail the influence of the nature of the phosphorus and indium precursors used and of reaction additives, such as zinc carboxylates or alkylamines, on the properties of the NCs. Finally, core/shell systems and doped InP NCs are discussed, and perspectives in this field are given.
The key to fully leveraging the potential of the electrochemical CO2 reduction reaction (CO2RR) to achieve a sustainable solar‐power‐based economy is the development of high‐performance electrocatalysts. The development process relies heavily on trial and error methods due to poor mechanistic understanding of the reaction. Demonstrated here is that ionic liquids (ILs) can be employed as a chemical trapping agent to probe CO2RR mechanistic pathways. This method is implemented by introducing a small amount of an IL ([BMIm][NTf2]) to a copper foam catalyst, on which a wide range of CO2RR products, including formate, CO, alcohols, and hydrocarbons, can be produced. The IL can selectively suppress the formation of ethylene, ethanol and n‐propanol while having little impact on others. Thus, reaction networks leading to various products can be disentangled. The results shed new light on the mechanistic understanding of the CO2RR, and provide guidelines for modulating the CO2RR properties. Chemical trapping using an IL adds to the toolbox to deduce the mechanistic understanding of electrocatalysis and could be applied to other reactions as well.
Through in situ photoelectron spectroscopy, the interface properties of BiVO4/NiO, BiVO4/CoOx and BiVO4/ITO were investigated.
The interface formation and energy-band alignment at interfaces between polycrystalline BiVO 4 and high-work-function RuO 2 and low-work-function Sn-doped In 2 O 3 (indium tin oxide) have been studied using photoelectron spectroscopy with in situ thin-film deposition of the contact materials. The Schottky barrier heights for both contact films differ by 0.85 eV, which is smaller than the difference in work function and the differences observed for other semiconducting oxides, indicating a partial Fermi-level pinning. On the basis of the present results and the comparison with other photoelectrochemically active oxides, the differences of band alignment obtained from solid/ electrolyte and from solid/solid interfaces, which can exhibit substantial differences, are discussed.
CuFeO2 is recognized as a potential photocathode for photo(electro)chemical water splitting. However, photocurrents with CuFeO2‐based systems are rather low so far. In order to optimize charge carrier separation and water reduction kinetics, defined CuFeO2/Pt, CuFeO2/Ag, and CuFeO2/NiOx(OH)y heterostructures are made in this work through a photodeposition procedure based on a 2H CuFeO2 hexagonal nanoplatelet shaped powder. However, water splitting performance tests in a closed batch photoreactor show that these heterostructured powders exhibit limited water reduction efficiencies. To test whether Fermi level pinning intrinsically limits the water reduction capacity of CuFeO2, the Fermi level tunability in CuFeO2 is evaluated by creating CuFeO2/ITO and CuFeO2/H2O interfaces and analyzing the electronic and chemical properties of the interfaces through photoelectron spectroscopy. The results indicate that Fermi level pinning at the Fe3+/Fe2+ electron polaron formation level may intrinsically prohibit CuFeO2 from acquiring enough photovoltage to reach the water reduction potential. This result is complemented with density functional theory calculations as well.
A new strategy affords “non‐nano” carbon materials as dehydrogenation catalysts that perform similarly to nanocarbons. Polymer‐based carbon precursors that combine a soft‐template approach with ion adsorption and catalytic graphitization are key to this synthesis strategy, thus offering control over macroscopic shape, texture, and crystallinity and resulting in a hybrid amorphous/graphitic carbon after pyrolysis. From this intermediate the active carbon catalyst is prepared by removing the amorphous parts of the hybrid carbon materials via selective oxidation. The oxidative dehydrogenation of ethanol was chosen as test reaction, which shows that fine‐tuning the synthesis of the new carbon catalysts allows to obtain a catalytic material with an attractive high selectivity (82 %) similar to a carbon nanotube reference, while achieving 10 times higher space–time yields at 330 °C. This new class of carbon materials is accessible via a technically scalable, reproducible synthetic pathway and exhibits spherical particles with diameters around 100 μm, allowing unproblematic handling similar to classic non‐nano catalysts.
The (photo)electrochemical water-splitting mechanism has not yet been completely resolved on an atomic level, partly because the interaction between water and the (photo)electrocatalytic surface has not yet been completely elucidated. Because of its ability to oxidize water upon light exposure, BiVO4 was chosen in this work as a prototype photocatalytic material to investigate the effects of water on a pristine metal oxide surface. In particular, polycrystalline surface-cleaned BiVO4 samples were exposed to water in controlled experiments at room temperature and at 77 K, analyzing any electronic and chemical changes at the surface by applying photoelectron spectroscopy. The results show that upon water exposure, hydroxide species form, the Fermi level position rises, the amount of oxygen at the surface decreases, and bismuth and vanadium partially reduces. Accordingly, the interaction of water with bismuth vanadate seemingly follows a reductive water dissociation process.
We report a high-speed low dark current near-infrared (NIR) organic photodetector (OPD) on a silicon substrate with amorphous indium gallium zinc oxide (a-IGZO) as the electron transport layer (ETL). In-depth understanding of the origin of dark current is obtained using an elaborate set of characterization techniques, including temperature-dependent current-voltage measurements, current-based deep-level transient spectroscopy (Q-DLTS), and transient photovoltage decay measurements. These characterization results are complemented by energy band structures deduced from ultraviolet photoelectron spectroscopy. The presence of trap states and a strong dependency of activation energy on the applied reverse bias voltage point to a dark current mechanism based on trap-assisted fieldenhanced thermal emission (Poole−Frenkel emission). We significantly reduce this emission by introducing a thin interfacial layer between the donor: acceptor blend and the a-IGZO ETL and obtain a dark current as low as 125 pA/cm 2 at an applied reverse bias of −1 V. Thanks to the use of high-mobility metal-oxide transport layers, a fast photo response time of 639 ns (rise) and 1497 ns (fall) is achieved, which, to the best of our knowledge, is among the fastest reported for NIR OPDs. Finally, we present an imager integrating the NIR OPD on a complementary metal oxide semiconductor read-out circuit, demonstrating the significance of the improved dark current characteristics in capturing high-quality sample images with this technology.
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