Morphology control represents an important strategy for the development of functional nanomaterials and has yet to be achieved in the case of promising lead-free double perovskite materials so far. In this work, high-quality Cs 2 AgBiX 6 (X = Cl, Br, I) two-dimensional nanoplatelets were synthesized through a newly developed synthetic procedure. By analyzing the optical, morphological, and structural evolutions of the samples during synthesis, we elucidated that the growth mechanism of lead-free double perovskite nanoplatelets followed a lateral growth process from mono-octahedral-layer (half-unit-cell in thickness) cluster-based nanosheets to multilayer (three to four unit cells in thickness) nanoplatelets. Furthermore, we demonstrated that Cs 2 AgBiBr 6 nanoplatelets possess a better performance in photocatalytic CO 2 reduction compared with their nanocube counterpart. Our work demonstrates the first example with two-dimensional morphology of this important class of lead-free perovskite materials, shedding light on the synthetic manipulation and the application integration of such promising materials.
Doping metal ions into lead halide perovskite nanocrystals (NCs) has attracted great attention over the past few years due to the emergence of novel properties relevant to optoelectronic applications. Here, the synthesis of Mn2+/Yb3+ codoped CsPbCl3 NCs through a hot‐injection technique is reported. The resulting NCs show a unique triple‐wavelength emission covering ultraviolet/blue, visible, and near‐infrared regions. By optimizing the dopant concentrations, the total photoluminescence quantum yield (PL QY) of the codoped NCs can reach ≈125.3% due to quantum cutting effects. Mechanism studies reveal the efficient energy transfer processes from host NCs to Mn2+ and Yb3+ dopant ions, as well as a possible inter‐dopant energy transfer from Mn2+ to Yb3+ ion centers. Owing to the high PL QYs and minimal reabsorption loss, the codoped perovskite NCs are demonstrated to be used as efficient emitters in luminescent solar concentrators, with greatly enhanced external optical efficiency compared to that of using solely Mn2+ doped CsPbCl3 NCs. This study presents a new model system for enriching doping chemistry studies and future applications of perovskite NCs.
The coordination of the organ-specific responses regulating systemic energy distribution to replenish lipid stores in acutely activated brown adipose tissue (BAT) remains elusive. Here, we show that short-term cold exposure or acute β3-adrenergic receptor (β3AR) stimulation results in secretion of the anabolic hormone insulin. This process is diminished in adipocyte-specific Atgl mice, indicating that lipolysis in white adipose tissue (WAT) promotes insulin secretion. Inhibition of pancreatic β cells abolished uptake of lipids delivered by triglyceride-rich lipoproteins into activated BAT. Both increased lipid uptake into BAT and whole-body energy expenditure in response to β3AR stimulation were blunted in mice treated with the insulin receptor antagonist S961 or lacking the insulin receptor in brown adipocytes. In conclusion, we introduce the concept that acute cold and β3AR stimulation trigger a systemic response involving WAT, β cells, and BAT, which is essential for insulin-dependent fuel uptake and adaptive thermogenesis.
Heterostructural
core–shell quantum dots (hetero-QDs) have
garnered a copious amount of research effort for not only scientific
advances but also a range of technological applications. Particularly,
controlling the heteroshell deposition, which in turn determines the
particle morphology, is vital in regulating the photophysical properties
and the application potential of the hetero-QDs. In this work, we
present the first report on a synthesis of pyramidal shaped (i.e.,
hexagonal pyramid, HP, and hexagonal bipyramid, HBP) CdSe-CdS hetero-QDs
with high morphological uniformity and epitaxial crystallinity through
a two-step shell growth method. The stabilization of the exposed (0002)
and {101̅1} facets by octadecylphosphonic acid and oleic acid
ligands, respectively, is the key for the formation of pyramidal particle
shapes. High photoluminescence quantum yield (94%, HP-QDs and 73%,
HBP-QDs), minimal inhomogeneous PL line width broadening, and significantly
suppressed single-QD blinking are observed. Specifically, the “giant”
HBP-QDs showed an average “On” time fraction of 96%
with more than 50% of measured particles completely nonblinking. Additionally,
high multiexciton emission, prolonged ensemble and single-QD PL lifetimes
as compared to their spherical counterparts are also reported. Finally,
the HBP-QDs have been successfully transferred into an aqueous solution
without aggregation. High cellular uptakes associated with low cytotoxicity
render these water-soluble HBP-QDs an excellent candidate for intracellular
imaging and labeling.
Semiconductor quantum dots (QDs) have attracted tremendous attention in the field of photocatalysis, owing to their superior optoelectronic properties for photocatalytic reactions, including high absorption coefficients and long photogenerated carrier lifetimes. Herein, by choosing 2‐(3,4‐dimethoxyphenyl)‐3‐oxobutanenitrile as a model substrate, we demonstrate that the stereoselective (>99 %) C−C oxidative coupling reaction can be realized with a high product yield (99 %) using zwitterionic ligand capped CsPbBr3 perovskite QDs under visible light illumination. The reaction can be generalized to different starting materials with various substituents on the phenyl ring and varied functional moieties, producing stereoselective dl‐isomers. A radical mediated reaction pathway has been proposed. Our study provides a new way of stereoselective C−C oxidative coupling via a photocatalytic means using specially designed perovskite QDs.
The reaction of phenyliodine bis(trifluoroacetate) (PIFA) with a series of anilides 1 (E = CO(2)Et) in CF(3)CH(2)OH was found to give 3-hydroxy-2-oxindole derivatives 2, while that with various anilides 1' (E = CON(R(4))Ar) afforded the C(2)-symmetric or unsymmetric spirooxindoles 3. These processes feature a metal-free oxidative C(sp(2))-C(sp(3)) bond formation, followed by oxidative hydroxylation or spirocyclization.
Fabrication
of quantum dots (QDs) with emission covering a wide
spectral region has been persistently intriguing because of their
potentials in a range of practical applications such as biological
labeling and imaging, solar cells, light-emitting diodes, and next-generation
displays. In this work, we report the synthesis of CdZnSe–CdZnS
core–shell alloy QDs through a Cu-catalyzed solid solution
alloying strategy starting from CdSe–CdS core–shell
QDs. The resulting CdZnSe–CdZnS alloy QDs exhibit emission
profiles covering a wide wavelength range of 470–650 nm while
maintaining high photoluminescence quantum yields. In addition, high
morphological uniformity of the starting CdSe–CdS QDs can be
largely retained in the final alloy QDs. We attribute this alloying
process to the high mobility nature of Cu cations in Cd-chalcogenide
crystals at elevated reaction temperatures, which allows Cu cations
to act as transporting agents to transfer a Zn component into the
CdSe–CdS QDs while maintaining the particle integrity. We show
that this unique alloying strategy is independent of the shape of
the starting QDs and can also be applied to the synthesis of CdZnSe–CdZnS
nanorods. We anticipate that our study will instigate the synthesis
of various high-quality alloy QDs and other alloy nanocrystals beyond
what can be achieved currently.
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