Using Mn-doped CsPbCl3 nanocrystals (Mn:CsPbCl3 NCs) to improve perovskite’s
properties is becoming an important
strategy. Here, we demonstrate a modified supersaturated recrystallization
route to synthesize high-quality Mn:CsPbCl3 NCs at room
temperature. Unprecedentedly, sulfonate ligands with various concentrations
are shown to successfully tune the dual-color emission of Mn:CsPbCl3 NCs. Ultrafast transient absorption studies reveal that the
host-to-dopant internal energy-transfer process involves the mediated
traps. Interestingly, the dual-color emission is tuned via stabilizing
mediated traps with a small amount of ligand (band edge (BE) emission
reduces and Mn2+ emission increases), passivating the deep
traps with a large amount of ligand (Mn2+ emission increases),
and destroying Mn:CsPbCl3 NCs with too much ligand (both
BE and Mn2+ emission is quenched). Furthermore, the ligand
tuning Mn2+ emission exhibits quenching for Cu2+ with high sensitivity and selectivity. Our work provides a new strategy
to tune the optical properties of Mn:CsPbCl3 NCs and presents
its potential application in an optical detector.
Doping metal ions into lead halide perovskite nanocrystals is one of the most efficient strategies to control their photoelectric properties. Here, we develop a simple and low-cost route to synthesize the high-quality alkaline-earth metal ion (AE 2+ )-doped CsPbBr 3 nanocrystals at room temperature. The almost 100% promoted photoluminescence quantum yield behavior of AE 2+ -doped CsPbBr 3 nanocrystals is demonstrated by an ultrafast dynamics study and theoretical calculations on the dopant defect formation energies and electronic properties. The AE 2+ dopants can promote the radiation recombination of carriers by essentially reducing the carriers trapped into intraband and interband defect states and promote the intraband coupling. Furthermore, Br − and Pb 2+ vacancies can be eliminated to enhance the short-range order of the CsPbBr 3 lattice and enrich the conduction band edge states, leading to the photoluminescence enhancement of CsPbBr 3 nanocrystals. Our studies provide new insights into the mechanism of AE 2+ -doped effects and present guiding strategies for improving the optical performance of doped perovskite nanocrystals.
Sluggish sulfur redox reaction (SROR) kinetics accompanying lithium polysulfides (LiPSs) shuttle effect becomes a stumbling block for commercial application of LiS battery. High‐efficient single atom catalysts (SACs) are desired to improve the SROR conversion capability; however, the sparse active sites as well as partial sites encapsulated in bulk‐phase are fatal to the catalytic performance. Herein, high loading (5.02 wt.%) atomically dispersed manganese sites (MnSA) on hollow nitrogen‐doped carbonaceous support (HNC) are realized for the MnSA@HNC SAC by a facile transmetalation synthetic strategy. The thin‐walled hollow structure (≈12 nm) anchoring the unique trans‐MnN2O2 sites of MnSA@HNC provides a shuttle buffer zone and catalytic conversion site for LiPSs. Both electrochemical measurement and theoretical calculation indicate that the MnSA@HNC with abundant trans‐MnN2O2 sites have extremely high bidirectional SROR catalytic activity. The assembled LiS battery based on the MnSA@HNC modified separator can deliver a large specific capacity of 1422 mAh g−1 at 0.1 C and stable cycling over 1400 cycles with an ultralow decay rate of 0.033% per cycle at 1 C. More impressively, a flexible pouch cell on account of the MnSA@HNC modified separator may release a high initial specific capacity of 1192 mAh g−1 at 0.1 C and uninterruptedly work after the bending‐unbending processes.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.