RESUMEN
Nitrogen-doped carbon dots (NCDs) featuring primary pyrrolic N and pyridinic N dominated configurations were prepared using hydrothermal (H-NCDs) and microwave (M-NCDs) methods, respectively. These H-NCDs and M-NCDs were subsequently applied to decorate CsPbBr3 nanocrystals (CPB NCs) individually, using a ligand-assisted reprecipitation process. Both CPB/M-NCDs and CPB/H-NCDs nanoheterostructures (NHSs) exhibited S-scheme charge transfer behavior, which enhanced their performance in photocatalytic CO2 reduction and selectivity of CO2-to-CH4 conversion, compared to pristine CPB NCs. The presence of pyrrolic N configuration at the heterojunction of CPB/H-NCDs facilitated efficient S-scheme charge transfer, leading to a remarkable 43-fold increase in photoactivity. In contrast, CPB/M-NCDs showed only a modest 3-fold enhancement in photoactivity, which was attributed to electron trapping by pyridinic N at the heterojunction. The study offers crucial insights into charge carrier dynamics within perovskite/carbon NHSs at the molecular level to advance the understanding of solar fuel generation.
RESUMEN
InP/ZnSexS1-x core/shell quantum dots (QDs) with varying Cu concentrations were synthesized by a one-pot hot-injection method. X-ray diffraction and high-resolution transmission electron microscopy results indicate that Cu doping did not alter the crystal structure or particle size of the QDs. The optical shifts in UV-visible absorption and photoluminescence (PL) suggest changes in the electronic structure and induction of lattice disorder due to Cu doping. Ultrafast transient absorption spectroscopy (TAS) reveled that a higher Cu-doping level leads to faster charge carrier recombination, likely due to increased nonradiative decay from defect states. Time-resolved PL (TRPL) studies show longer average lifetimes of charge carriers with increased Cu doping. These findings informed the development of a kinetic model to better understand how Cu-induced disorder affects charge carrier dynamics in the QDs, which is important for emerging applications of Cu-doped InP/ZnSexS1-x QDs in optoelectronics.
RESUMEN
The photon energy-dependent selectivity of photocatalytic CO2-to-CO conversion by CsPbBr3 nanocrystals (NCs) and CsPbBr3/g-C3N4 nanoheterostructures (NHSs) was demonstrated for the first time. The surficial capping ligands of CsPbBr3 NCs would adsorb CO2, resulting in the carboxyl intermediate to process the CO2-to-CO conversion via carbene pathways. The type-II energy band structure at the heterojunction of CsPbBr3/g-C3N4 NHSs would separate the charge carriers, promoting the efficiency in photocatalytic CO2-to-CO conversion. The electron consumption rate of CO2-to-CO conversion for CsPbBr3/g-C3N4 NHSs was found to intensively depend on the rate constant of interfacial hole transfer from CsPbBr3 to g-C3N4. An in situ transient absorption spectroscopy investigation revealed that the half-life time of photoexcited electrons in optimized CsPbBr3/g-C3N4 NHS was extended two times more than that in the CsPbBr3 NCs, resulting in the higher probability of charge carriers to carry out the CO2-to-CO conversion. The current work presents important and novel insights of semiconductor NHSs for solar energy-driven CO2 conversion.
RESUMEN
Ferroelectric photoelectrodes, other than conventional semiconductors, are alternative photo-absorbers in the process of water splitting. However, the capture of photons and efficient transfer of photo-excited carriers remain as two critical issues in ferroelectric photoelectrodes. In this work, we overcome the aforementioned issues by decorating the ferroelectric BiFeO3 (BFO) surface with Au nanocrystals, and thus improving the photoelectrochemical (PEC) performance of BFO film. We demonstrate that the internal field induced by the spontaneous polarization of BFO can (1) tune the efficiency of the photo-excited carriers' separation and charge transfer characteristics in bare BFO photoelectrodes, and (2) modulate an extra optical absorption within the visible light region, created by the surface plasmon resonance excitation of Au nanocrystals to capture more photons in the Au/BFO heterostructure. This study provides key insights for understanding the tunable features of PEC performance, composed of the heterostructure of noble metals and ferroelectric materials.
RESUMEN
Hybrid nanoparticles (NPs) composed of multiple components offer new opportunities for next-generation materials. In this study, a paradigm for the noble metal/ternary complex oxide hybrid NPs is reported by adopting pulsed laser ablation in liquids. As model hybrids, gold-spinel heterodimer (Au-CoFe2O4) and gold-pervoskite heterodimer (Au-SrTiO3) NPs are investigated. This work has demonstrated the diverse playgroup of NP conjugation enlarged by complex oxides.