Three‐dimensionally ordered macroporous (3DOM) structures have been widely utilized to largely enhance a photocatalytic activity. However, the common nanoparticles‐constructed 3DOM photocatalysts ...possess numerous grain boundaries, unavoidably leading to a fast recombination of photogenerated electrons and holes. Herein, for the first time, a hierarchically two‐dimensional (2D) meso‐microporous perovskite nanosheet‐constructed 3DOM CaTiO3 to significantly reduce the grain boundaries is designed and fabricated. Using carbon quantum dots (CQDs) as a metal‐free co‐catalyst, the 3DOM CQDs‐CaTiO3 exhibits an outstanding photocatalytic activity for hydrogen generation of 0.13 mmol h−1 (20 mg photocatalyst) with remarkable apparent quantum efficiency (QAY) of 14.55% at 365 nm monochromatic light. This unprecedented performance is endowed by the synergy of a macro‐meso‐microporosity architecture, a large surface area, enhanced light harvesting, and improved charge carriers separation and transport. Density functional theory calculations and finite difference time‐domain simulations further reveal the mechanism behind the enhanced separation of photogenerated electrons and holes. The present work demonstrates a trial on rationally designing meso‐microporous nanosheet‐constructed 3DOM perovskites for solar driven hydrogen production.
A perovskite meso‐microporous nanosheet‐constructed 3DOM CaTiO3 decorated with CQDs is designed for remarkable photocatalytic hydrogen production in a noble‐metal free system. The as‐synthesized composite exhibits extremely enhanced photocatalytic activity owing to the easy mass transfer by the synergistic effect of macro‐meso‐microporosity, large surface area, enhanced light harvesting, and improved separation of charge carriers.
Cognitive dysfunction is a common postoperative neurological complication in patients undergoing valve replacement surgery. This study aimed to compare the effects of sevoflurane versus ...propofol‐based total intravenous anesthesia on the incidence of cognitive dysfunction following valve replacement surgery. This multicenter, randomized, controlled double‐blinded study was conducted in three teaching hospitals in China. Patients receiving on‐pump valve replacement surgery were enrolled. Stratified block randomization was used to randomly assign patients 1:1 to receive sevoflurane (1.0–1.5 MAC) or propofol (2.0–3.0 mg/kg/h) for anesthesia maintenance. The primary outcome was the incidence of cognitive dysfunction assessed by four cognitive tests before, as well as 7–14 days after surgery. Patients were randomly assigned to receive sevoflurane anesthesia (n = 144) or propofol‐based total intravenous anesthesia (n = 145). The incidence of postoperative cognitive dysfunction in the sevoflurane anesthesia group (31.9%) was significantly lower than that in the total intravenous anesthesia group (43.4%; relative risk 0.61, 95% confidence interval CI: 0.38–0.97, p = 0.044). There was no difference in the incidence of delirium between patients receiving sevoflurane and total intravenous anesthesia (27.8% 35/144 vs. 25.9% 35/145, 1.10, 95% CI: 0.64 to 1.90, p = 0.736). There was a significant difference in the Katz Index on day 3 after surgery (3 0.9) vs. 3 (1.0, 0.095, 95% CI: 0.05 to 0.43, p = 0.012). No difference was observed in other outcomes between the two groups. For patients undergoing on‐pump valve replacement surgery, sevoflurane anesthesia had a smaller effect on cognitive function and independence in daily life activities compared with propofol anesthesia.
Transmission electron microscopy (TEM) is a powerful tool for unveiling the structural, compositional, and electronic properties of organic–inorganic hybrid perovskites (OIHPs) at the atomic to ...micrometer length scales. However, the structural and compositional instability of OIHPs under electron beam radiation results in misunderstandings of the microscopic structure–property–performance relationship in OIHP devices. Here, ultralow dose TEM is utilized to identify the mechanism of the electron‐beam‐induced changes in OHIPs and clarify the cumulative electron dose thresholds (critical dose) of different commercially interesting state‐of‐the‐art OIHPs, including methylammonium lead iodide (MAPbI3), formamidinium lead iodide (FAPbI3), FA0.83Cs0.17PbI3, FA0.15Cs0.85PbI3, and MAPb0.5Sn0.5I3. The critical dose is related to the composition of the OIHPs, with FA0.15Cs0.85PbI3 having the highest critical dose of ≈84 e Å−2 and FA0.83Cs0.17PbI3 having the lowest critical dose of ≈4.2 e Å−2. The electron beam irradiation results in the formation of a superstructure with ordered I and FA vacancies along c, as identified from the three major crystal axes in cubic FAPbI3, c, c, and c. The intragrain planar defects in FAPbI3 are stable, while an obvious modification is observed in FA0.83Cs0.17PbI3 under continuous electron beam exposure. This information can serve as a guide for ensuring a reliable understanding of the microstructure of OIHP optoelectronic devices by TEM.
Transmission‐electron‐microscopy‐based characterization techniques are expected to play a significant role in revealing the structural, compositional, and electronic properties of organic–inorganic hybrid perovskite materials and optoelectronic devices. However, perovskites are unstable and highly sensitive to electron beam radiation. This paper has outlined key guidelines for imaging the intrinsic structure of organic–inorganic hybrid perovskite materials.
Upregulation of histone methyltransferase SETDB1 is associated with poor prognosis in cancer patients. However, the mechanism of oncogenicity of SETDB1 in cancer is hitherto unknown. Here, we show ...that SETDB1 is upregulated in human colorectal cancer (CRC) where its level correlates with poor clinical outcome. Ectopic SETDB1 promotes CRC cell proliferation, whereas SETDB1 attenuation inhibits this process. Flow cytometry reveals that SETDB1 promotes proliferation by driving the CRC cell cycle from G0/G1 phase to S phase. Mechanistically, SETDB1 binds directly to the STAT1 promoter region resulting in increased STAT1 expression. Functional characterization reveals that STAT1-CCND1/CDK6 axis is a downstream effector of SETDB1-mediated CRC cell proliferation. Furthermore, SETDB1 upregulation is sufficient to accelerate in vivo proliferation in xenograft animal model. Taken together, our results provide insight into the upregulation of SETDB1 within CRC and can lead to novel treatment strategies targeting this cell proliferation-promoting gene.
Aqueous zinc ion batteries (AZIBs) have recently sparked an enormous surge of research attention, due to their environmental benignity, natural abundance, negligible safety issue, and exceptional ...electrochemical performance. Despite the rapid progress in designing a kind of exceptional cathode material with high compatibility to the aqueous electrolyte, the potential issues on the zinc anode side should not be underestimated, including dendrite growth, Zn corrosion, and hydrogen evolution. Herein, the origin of the above problems is outlined from the perspective of thermodynamics, and the optimization strategies of Zn are accordingly discussed and summarized in two aspects: the anode and the electrolyte. Finally, some general guidance and suggested future research directions for high-performance Zn anodes are proposed, aiming to further prolong cycling lifespan and promote commercialization of AZIBs.
Aqueous zinc ion batteries (AZIBs) have recently sparked an enormous surge of research attention, due to their environmental benignity, natural abundance, negligible safety issue, and exceptional electrochemical performance.
Current chemodynamic therapy (CDT) primarily relies on the delivery of transition metal ions with Fenton activity to trigger hydroxyl radical production from hydrogen peroxide. However, ...administration of an excess amount of exogenous Fenton-type heavy metals may cause potential adverse effects to human health, including acute and chronic damages. Here, we present a new CDT strategy that uses intracellular labile iron pool (LIP) as the endogenous source of Fenton-reactive metals for eliciting free radical generation, and the discovery of hydroperoxides (R′OOH) as an optimal LIP-mediated chemodynamic agent against cancer. By simulating the metabolic fates of peroxo compounds within cells, R′OOH was found to have excellent free radical-producing ability in the presence of labile iron(II) and to suffer only moderate elimination by glutathione/glutathione peroxidase, which contributes to its superior chemodynamic efficacy. The LIP-initiated nontoxic-to-toxic transition of R′OOH, together with increased LIP levels in tumor cells, enabled efficient and specific CDT of cancer. Moreover, pH/labile iron(II) cascade-responsive nanomedicines comprising encapsulated methyl linoleate hydroperoxide and LIP-increasing agent in pH-sensitive polymer particles were fabricated to realize enhanced CDT. This work not only paves the way to using endogenous Fenton-type metals for cancer therapy but also offers a paradigm for the exploration of high-performance chemodynamic agents activated by intracellular LIP.
Mesenchymal stem cell (MSC)-derived exosomes have shown comprehensive application prospects over the years. Despite performing similar functions, exosomes from different origins present heterogeneous ...characteristics and components; however, the relative study remains scarce. Lacking of a valuable reference, researchers select source cells for exosome studies mainly based on accessibility and personal preference.
In this study, exosomes secreted by MSCs derived from different tissues were isolated, by ultracentrifugation, and proteomics analysis was performed. A total of 1014 proteins were detected using a label-free method.
Bioinformatics analysis revealed their shared function in the extracellular matrix receptor. Bone marrow MSC-derived exosomes showed superior regeneration ability, and adipose tissue MSC-derived exosomes played a significant role in immune regulation, whereas umbilical cord MSC-derived exosomes were more prominent in tissue damage repair.
This study systematically and comprehensively analyzes the human MSC-derived exosomes via proteomics, which reveals their potential applications in different fields, so as to provide a reference for researchers to select optimal source cells in future exosome-related studies.
Although long-read single-cell RNA isoform sequencing (scISO-Seq) can reveal alternative RNA splicing in individual cells, it suffers from a low read throughput. Here, we introduce HIT-scISOseq, a ...method that removes most artifact cDNAs and concatenates multiple cDNAs for PacBio circular consensus sequencing (CCS) to achieve high-throughput and high-accuracy single-cell RNA isoform sequencing. HIT-scISOseq can yield >10 million high-accuracy long-reads in a single PacBio Sequel II SMRT Cell 8M. We also report the development of scISA-Tools that demultiplex HIT-scISOseq concatenated reads into single-cell cDNA reads with >99.99% accuracy and specificity. We apply HIT-scISOseq to characterize the transcriptomes of 3375 corneal limbus cells and reveal cell-type-specific isoform expression in them. HIT-scISOseq is a high-throughput, high-accuracy, technically accessible method and it can accelerate the burgeoning field of long-read single-cell transcriptomics.
A robust polyimide film was facilely fabricated on the ITO-glass substrate from the electrolyte solution of a bis(triphenylamine) perylene diimide by electrochemical polymerization. The cyclic ...voltammogram of the electrodeposited polyimide film shows ambipolar redox processes, with a reversible redox couple with a half wave potential (E1/2) of +0.99V during the anodic scanning and two pairs of redox waves at E1/2=−0.41V and −0.65V during cathodic scanning. The electroactive film did not delaminate from the electrode upon cycling electrochemically between its oxidized/reduced and neutral states. The polyimide film exhibits stable anodic and cathodic coloring, with high optical contrast, high coloration efficiency, and good cycling stability.
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•A redox-active polyimide film was electropolymerized from a bis(triphenylamine) perylene diimide.•The polyimide film showed stable ambipolar redox and electrochromic properties.•The polyimide film exhibited high optical contrast, coloration efficiency, and cycling stability.
Desalination is a sustainable process that removes sodium and chloride ions from seawater. Herein, we demonstrate a faradaic mechanism to promote the capacity of capacitive deionization in highly ...concentrated salt water via an electrochemical deionization device. In this system, ion removal is achieved by the faradaic mechanism via a constant current operation mode, which is improved based on the constant voltage operation mode used in the conventional CDI operation. Benefiting from the high capacity and excellent rate performance of Prussian blue as an active electrochemical reaction material, the designed unit has revealed a superior removal capacity with an ultrafast ion removal rate. A high removal capacity of 101.7 mg g
has been obtained with proper flow rate and current density. To further improve the performance of the EDI, a reduced graphene oxide with nanopores and Prussian blue composite has been synthesized. The PB@NPG has demonstrated a high salt removal capacity of 120.0 mg g
at 1 C with an energy consumption of 6.76 kT per ion removed, which is much lower than most CDI methods. A particularly high rate performance of 0.5430 mg g
s
has been achieved at 40 C. The faradaic mechanism promoted EDI has provided a new insight into the design and selection of host materials for highly concentrated salt water desalination.
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