RESUMO
In the emerging Sb2S3-based solar energy conversion devices, a CdS buffer layer prepared by chemical bath deposition is commonly used to improve the separation of photogenerated electron-hole pairs. However, the cation diffusion at the Sb2S3/CdS interface induces detrimental defects but is often overlooked. Designing a stable interface in the Sb2S3/CdS heterojunction is essential to achieve high solar energy conversion efficiency. As a proof of concept, this study reports that the modification of the Sb2S3/CdS heterojunction with an ultrathin Al2O3 interlayer effectively suppresses the interfacial defects by preventing the diffusion of Cd2+ cations into the Sb2S3 layer. As a result, a water-splitting photocathode based on Ag:Sb2S3/Al2O3/CdS heterojunction achieves a significantly improved half-cell solar-to-hydrogen efficiency of 2.78% in a neutral electrolyte, as compared to 1.66% for the control Ag:Sb2S3/CdS device. This work demonstrates the importance of designing atomic interfaces and may provide a guideline for the fabrication of high-performance stibnite-type semiconductor-based solar energy conversion devices.
RESUMO
Interface engineering is a proven strategy to improve the efficiency of thin film semiconductor based solar energy conversion devices. Ta3N5 thin film photoanode is a promising candidate for photoelectrochemical (PEC) water splitting. Yet, a concerted effort to engineer both the bottom and top interfaces of Ta3N5 thin film photoanode is still lacking. Here, we employ n-type In:GaN and p-type Mg:GaN to modify the bottom and top interfaces of Ta3N5 thin film photoanode, respectively. The obtained In:GaN/Ta3N5/Mg:GaN heterojunction photoanode shows enhanced bulk carrier separation capability and better injection efficiency at photoanode/electrolyte interface, which lead to a record-high applied bias photon-to-current efficiency of 3.46% for Ta3N5-based photoanode. Furthermore, the roles of the In:GaN and Mg:GaN layers are distinguished through mechanistic studies. While the In:GaN layer contributes mainly to the enhanced bulk charge separation efficiency, the Mg:GaN layer improves the surface charge inject efficiency. This work demonstrates the crucial role of proper interface engineering for thin film-based photoanode in achieving efficient PEC water splitting.
RESUMO
This paper describes a study on the charge transport in a composite of liquid-exfoliated graphene nanoparticles (GNPs) and a polythiophene semiconducting polymer. While the former component is highly conducting, although it consists of isolated nanostructures, the latter offers an efficient charge transport path between the individual GNPs within the film, overall yielding enhanced charge transport properties of the resulting bi-component system. The electrical characteristics of the composite layers were investigated by means of measurements of time-of-flight photoconductivity and transconductance in field-effect transistors. In order to analyze both phenomena separately, charge density and charge mobility contributions to the conductivity were singled out. With the increasing GNP concentration, the charge mobility was found to increase, thereby reducing the time spent by the carriers on the polymer chains. In addition, for GNP loading above 0.2 % (wt.), an increase of free charge density was observed that highlights an additional key role played by doping. Variable-range hopping model of a mixed two- and three-dimensional transport is explained using temperature dependence of mobility and free charge density. The temperature variation of free charge density was related to the electron transfer from polythiophene to GNP, with an energy barrier of 24â meV.