Angew Chem Int Ed Engl
December 2024
Crystal structural rearrangements unavoidably introduce defects into materials, where even these small changes in local lattice structure could arouse a prominent impact on the overall nature of crystals. Contrary to the traditional notion that defects obstruct carrier transport, herein, we report a promoted transport mechanism of nonluminescent carriers in single-crystalline CHNHPbI nanowires (1345.2 cm V s, about a 14-fold improvement), enabled by the phase transition induced defects (PTIDs).
View Article and Find Full Text PDFNative mass spectrometry (MS), ion mobility (IM), and collision-induced unfolding (CIU) have all been widely used to study the binding of small molecules to proteins and their complexes. Despite many successes in detecting subtle gas-phase stability differences in smaller systems dominated by single-domain subunits, studies targeting complexes comprised of large, multidomain subunits still face many challenges. For example, polyketide synthases (PKSs) are multiprotein enzymes that use their modular architecture to produce polyketide natural products and form the basis for nearly one-third of pharmaceuticals.
View Article and Find Full Text PDFThe type 1 polyketide synthase (PKS) assembly line uses its modular structure to produce polyketide natural products that form the basis of many pharmaceuticals. Currently, several cryoelectron microscopy (cryo-EM) structures of a multidomain PKS module have been constructed, but much remains to be learned. Here we utilize ion-mobility mass spectrometry (IM-MS) to record size and shape information and detect different conformational states of a 207 kDa didomain dimer comprised of ketosynthase (KS) and acyl transferase (AT), excised from full-length module.
View Article and Find Full Text PDFBased on their excellent stability, high carrier mobility, and wide photoresponse range, composites formed by embedding perovskite quantum dots (PQDs) into metal-organic frameworks (PQDs@MOF) show great development potential in the field of photocatalysis, including the toxic hexavalent chromium (Cr) degradation, CO reduction, H production, etc. However, the rapid recombination of photogenerated carriers is still a major obstacle to the improvement of photocatalytic performance, and the internal mechanism of photocatalysis is still unclear. In this work, we construct a novel double heterojunction photocatalyst by encapsulating CsPbBr PQDs in Zr-based metal-organic frameworks (UiO-67) and loading additional hole-acceptor pentylenetetrazol (PTZ).
View Article and Find Full Text PDFBackground: Traditional Chinese medicine (TCM) comprising herbal formulas has been used for millennia to treat various diseases, such as insomnia, based on distinct syndrome types. Although TCM has been proposed to be effective in insomnia through gut microbiota modulation in animal models, human studies remain limited. Therefore, this study employs machine learning and integrative network techniques to elucidate the role of the gut microbiome in the efficacies of two TCM formulas - center-supplementing and qi-boosting decoction (CSQBD) and spleen-tonifying and yin heat-clearing decoction (STYHCD) - in treating insomnia patients diagnosed with spleen qi deficiency and spleen qi deficiency with stomach heat.
View Article and Find Full Text PDFAs opposed to natural photosynthesis, a significant challenge in a semiconductor-based photocatalyst is the limited hole extraction efficiency, which adversely affects solar-to-fuel efficiency. Recent studies have demonstrated that photocatalysts featuring spatially isolated dual catalytic oxidation/reduction sites can yield enhanced hole extraction efficiencies. However, the decay dynamics of excited states in such photocatalysts have not been explored.
View Article and Find Full Text PDFLong noncoding RNAs (lncRNAs) are revealed to be involved in the tumorigenesis and progression of human malignancies mediated by microRNA (miRNA) via the competing endogenous RNA (ceRNA) mechanism, a newly proposed "RNA language." However, the lncRNA-associated competing triplet (lncACT) network among ceRNA transcripts in clear cell renal cell carcinoma (ccRCC) is currently lacking. We carried out differential expression analysis to identify aberrantly expressed lncRNAs, miRNAs, and mRNAs by analyzing the RNA-seq data of 420 ccRCC tissues and 71 noncancerous kidney tissues obtained from The Cancer Genome Atlas (TCGA).
View Article and Find Full Text PDFBackground: Cancer-associated fibroblasts (CAFs) are vital components of gastric cancer (GC) microenvironments, which impact the aggressive characteristics of GC cells. The objective of this study is to evaluate the influence of High Mobility Group Box (HMGB) on CAF-related GC.
Methods: The tissues of 10 GC patients who underwent surgery the Sanya Central Hospital of Hainan Province from July 2018 to July 2019 were collected for the clinical study.
Two-dimensional (2D) and quasi-2D Ruddlesden-Popper (RP) phase organolead halide perovskites are promising materials for both photovoltaic and optoelectronic devices. Although they are known to be more stable when exposed to moisture than their 3D counterpart, chemical degradation of these materials under moisture, which not only leads to a significant drop in device performance but also leads to lead leakage, yet remains one of the most serious hurdles for their practical applications. To gain insight into the degradation mechanism of 2D/quasi-2D perovskites under moisture conditions, the degradation pathway of 2D/quasi-2D (PEA)(MA) PbI (PEA = CHCHNH , MA = CHNH , and is the number of perovskite layers between adjacent organic spacer layers) perovskite single crystals (SCs) and thin film are explored.
View Article and Find Full Text PDFBackground And Objectives: Cementoblasts can communicate with osteoclasts by synthesis and secretion of cytokines, such as RANKL, OPG, and M-CSF. Previously, we reported that irisin promotes the differentiation of cementoblasts, while the effect of irisin on cementoblast-mediated osteoclastogenesis remains inconclusive. This study aimed to explore the effect of irisin on the expression of osteoclastogenesis-related cytokines in cementoblasts.
View Article and Find Full Text PDFThe temperature-induced phase transition in two-dimensional (2D) layered perovskites was recently found to be incomplete even if the temperature dropped to tens of kelvin. However, its intrinsic cause still remains unclear, and the information on the phase transition in individual single crystals (SCs) is also limited. Herein, we study the phase transition process in individual (-CHNH)PbI SCs using a home-built photoluminescence (PL)-scanned image microscope.
View Article and Find Full Text PDFLayered two-dimensional (2D) lead halide perovskites are a class of quantum well (QW) materials, holding dramatic potentials for optical and optoelectronic applications. However, the thermally activated exciton dissociation into free carriers in 2D perovskites, a key property that determines their optoelectronic performance, was predicted to be weak due to large exciton binding energy (, about 100-400 meV). Herein, in contrast to the theoretical prediction, we discover an ultrafast (<1.
View Article and Find Full Text PDFJ Phys Chem Lett
February 2021
Doping with a transition metal is an effective way to tune the optical properties of semiconductor nanocrystals (NCs). The excitation of transition-metal dopants in NCs is through an internal energy transfer from a host exciton, by which the short-lived exciton energy can be "stored" at the dopant for a significantly longer lifetime. Herein, using Mn-doped CsPbCl perovskite NCs as an example, we report that the long-lived excited state at Mn dopants can be efficiently extracted from the NCs through an external energy transfer (EET) to rhodamine B (RhB) molecules adsorbed on the NC surface.
View Article and Find Full Text PDFFerulic acid decarboxylase catalyzes the decarboxylation of various substituted phenylacrylic acids to their corresponding styrene derivatives and CO using the recently discovered cofactor prenylated FMN (prFMN). The mechanism involves an unusual 1,3-dipolar cycloaddition reaction between prFMN and the substrate to generate a cycloadduct capable of undergoing decarboxylation. Using native mass spectrometry, we show the enzyme forms a stable prFMN-styrene cycloadduct that accumulates on the enzyme during turnover.
View Article and Find Full Text PDFJ Phys Chem Lett
November 2020
The encapsulation of perovskite quantum dots (PQDs) in metal organic frameworks (MOFs) is a promising strategy for fabricating stable and functional perovskite solid composites (denoted as PQDs@MOF), which have exhibited great potential for optoelectronics, catalysis, and luminesce applications. However, the exciton diffusion distance, one of the key factors determining the performance of PQDs@MOF in these applications, remains unknown. Herein, by using time-resolved and photoluminescence-scanned imaging microscopy, we report the observation of long-distance exciton transport (278 ± 12.
View Article and Find Full Text PDFJ Am Chem Soc
September 2020
Layered two-dimensional (2D) hybrid perovskites are naturally formed multiple quantum well (QW) materials with promising applications in quantum and optoelectronic devices. In principle, the transport of excitons in 2D perovskites is limited by their short lifetime and small mobility to a distance within a few hundred nanometers. Herein, we report an observation of long-distance carrier transport over 2 to 5 μm in 2D perovskites with various well thicknesses.
View Article and Find Full Text PDFDivalent manganese cation (Mn) doped perovskite materials are of great interest for their unique optical, magnetic, and electric properties. Herein, we report an excitation-dependent emission color tuning from an individual Mn-doped CsPbCl microcrystal (MC) with a wide color tuning range, reversible and continuous color change, and high photostability. We demonstrate that the Mn-doped CsPbCl MCs exhibit dual-color emission from both host excitons (blue) and Mn-dopants (orange) through an internal energy transfer (IET) process.
View Article and Find Full Text PDFTwo-dimensional (2D) hybrid perovskites have emerged as promising materials for optoelectronic devices owing to their improved stability. The crystal edges of layered 2D perovskites were found to play an important role in device performance by providing a pathway to dissociate bound excitons into long-lived free charge carriers. However, their formation mechanism and whether they are controllable remain unclear.
View Article and Find Full Text PDFMetal-halide perovskites are promising optical gain materials because of their excellent photophysical properties. Recently, large perovskite single crystals with phase purity, less defects, and over millimeter dimensions have been successfully synthesized. However, the optical gain effect from these large-size single crystals has not yet been realized.
View Article and Find Full Text PDFLighting accounts for one-fifth of global electricity consumption. Single materials with efficient and stable white-light emission are ideal for lighting applications, but photon emission covering the entire visible spectrum is difficult to achieve using a single material. Metal halide perovskites have outstanding emission properties; however, the best-performing materials of this type contain lead and have unsatisfactory stability.
View Article and Find Full Text PDFThe excellent charge carrier transportation in organolead halide perovskites is one major contributor to the high performance of many perovskite-based devices. There still exists a possibility for further enhancement of carrier transportation through nanoscale engineering, owing to the versatile wet-chemistry synthesis and processing of perovskites. Here we report the successful synthesis of bromide-gradient CHNHPbBrI single-crystalline nanowires (NWs) by a solid-to-solid ion exchange reaction starting from one end of pure CHNHPbI NWs, which was confirmed by local photoluminescence (PL) and energy dispersive X-ray spectroscopy (EDS) measurements.
View Article and Find Full Text PDFActa Pharm Sin B
November 2016
The purpose of this study was to investigate the effect of isopropyl myristate (IPM), a penetration enhancer, on the viscoelasticity and drug release of a drug-in-adhesive transdermal patch containing blonanserin. The patches were prepared with DURO-TAK 87-2287 as a pressure-sensitive adhesive (PSA) containing 5% (/) of blonanserin and different concentrations of IPM. An release experiment was performed and the adhesive performance of the drug-in-adhesive patches with different concentrations of IPM was evaluated by a rolling ball tack test and a shear-adhesion test.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
October 2016
Although the power conversion efficiency of perovskite solar cells has improved rapidly, a rational path for further improvement remains unclear. The effect of large morphological heterogeneity of polycrystalline perovskite films on their device performance by photoluminescence (PL) microscopy has now been studied. Contrary to the common belief on the deleterious effect of morphological heterogeneity on carrier lifetimes and diffusivities, in neat CH NH PbI (Cl) polycrystalline perovskite films, the local (intra-grain) carrier diffusivities in different grains are all surprisingly high (1.
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