The development of high-performance near-infrared organic light-emitting diodes is hindered by strong non-radiative processes as governed by the energy gap law. Here, we show that exciton ...delocalization, which serves to decouple the exciton band from highly vibrational ladders in the S0 ground state, can bring substantial enhancements in the photoluminescence quantum yield of emitters, bypassing the energy gap law. Experimental proof is provided by the design and synthesis of a series of new Pt(ii) complexes with a delocalization length of 5–9 molecules that emit at 866–960 nm with a photoluminescence quantum yield of 5–12% in solid films. The corresponding near-infrared organic light-emitting diodes emit light with a 930 nm peak wavelength and a high external quantum efficiency up to 2.14% and a radiance of 41.6 W sr−1 m−2. Both theoretical and experimental results confirm the exciton–vibration decoupling strategy, which should be broadly applicable to other well-aligned molecular solids.Pt(ii) complexes allow the fabrication of efficient near-infrared organic light-emitting diodes that operate beyond the 900 nm region.
Deep learning for digital pathology is hindered by the extremely high spatial resolution of whole-slide images (WSIs). Most studies have employed patch-based methods, which often require detailed ...annotation of image patches. This typically involves laborious free-hand contouring on WSIs. To alleviate the burden of such contouring and obtain benefits from scaling up training with numerous WSIs, we develop a method for training neural networks on entire WSIs using only slide-level diagnoses. Our method leverages the unified memory mechanism to overcome the memory constraint of compute accelerators. Experiments conducted on a data set of 9662 lung cancer WSIs reveal that the proposed method achieves areas under the receiver operating characteristic curve of 0.9594 and 0.9414 for adenocarcinoma and squamous cell carcinoma classification on the testing set, respectively. Furthermore, the method demonstrates higher classification performance than multiple-instance learning as well as strong localization results for small lesions through class activation mapping.
Electrochemical reduction of carbon dioxide (CO2RR) into value‐added chemicals is a promising tactic to mitigate global warming. However, this process resists catalyst preparation, low faradaic ...efficiency (FE%) towards multi‐carbon products, and insights into mechanistic understanding. Indeed, it is demonstrated that this Fe single‐atom catalyst (Fe SAC) exists in three oxygen coordination of Fe–(O)3 configuration in Nafion coated functionalized multi‐wall carbon nanotubes (Fe‐n‐f‐CNTs), which is obtained via a simple ionic exchange method under ambient conditions. The electrochemical performance reveals that Fe SACs achieve an FE of 45% and a yield rate of 56.42 µmol cm−2 h−1 at −0.8 VRHE for ethanol. In situ X‐ray analysis reveals that the Fe SACs have variable electronic states and keeps close +3 of the oxidation state at the potential range of CO2RR. The catalytic feature reduces the reaction energy and induces the electrons transferred to the adsorbed products intermediates of *COOH and *OCHO, thus promoting CO. The carboxylic functional group on the CNTs stabilizes the Fe active sites via electrostatic interaction, verified by density functional theory calculations. The yield rate of Fe SACs indicates that the Fe single‐atom site can instantly provide a large CO to help conversion of CO2‐to‐C2 product on the CNTs.
The Fe–(O)3 single‐atom catalyst synthesis via a simple ionic exchange method on Nafion‐coated functionalized multi‐wall carbon nanotubes (Fe‐n‐f‐CNTs). The Fe SACs and functionalized CNTs are dual active sites toward CO2RR with enhanced selectivity of C2 products. During CO2RR, the carboxylic functional group stabilizes the Fe single‐atom active catalytic site via electrostatic interactions.
Near‐infrared organic light‐emitting diodes (NIR OLEDs) enable many unique applications ranging from night‐vision displays and photodynamic therapies. However, the development of efficient NIR OLEDs ...with a low efficiency roll‐off is still challenging. Here, a series of new heteroleptic Pt(II) complexes (1–4) flanked by both pyridyl pyrimidinate and functional azolate chelates are synthesized. The reduced ππ* energy gap of the pyridyl pyrimidinate chelate, and strong intermolecular interaction and high crystallinity in vacuum‐deposited thin films engender strong intermolecular charge transfer transition including metal–metal‐to‐ligand charge transfer; thereby, exhibiting efficient photoluminescence within 776–832 nm and short radiative lifetimes of 0.52–0.79 µs. Consequently, nondoped NIR‐emitting OLEDs based on these Pt(II) complexes are fabricated, to which Pt(II) complexes 2 and 4 give record high maximum external quantum efficiency of 10.61% at 794 nm and 9.58% at 803 nm, respectively. Moreover, low efficiency roll‐off is also observed, among which the device efficiencies of 2 and 4 are at least four times higher than that of the best NIR‐emitting OLEDs recorded at current density of 100 mA cm−2.
Nondoped near‐infrared organic light‐emitting diodes based on pyrimidinate‐pyrazolate Pt(II) metal complexes 2 and 4 are fabricated, yielding a record high maximum external quantum efficiency of 10.61% at 794 nm and 9.58% at 803 nm, respectively.
Oxygen evolution reaction (OER) plays a key role in proton exchange membrane water electrolysis (PEMWE), yet the electrocatalysts still suffer from the disadvantages of low activity and poor ...stability in acidic conditions. Here, a new class of CdRu2IrOx nanoframes with distorted structure for acidic OER is successfully fabricated. Impressively, CdRu2IrOx displays an ultralow overpotential of 189 mV and an ultralong stability of 1500 h at 10 mA cm⁻2 toward OER in 0.5 M H2SO4. Moreover, a PEMWE using the distorted CdRu2IrOx can be steadily operated at 0.1 A cm⁻2 for 90 h. Microstructural analyses and X‐ray absorption spectroscopy (XAS) demonstrate that the synergy between Ru and Ir in CdRu2IrOx induces the distortion of Ru−O, Ir−O, and Ru−M (M = Ru, Ir) bonds. In situ XAS indicates that the applied potential leads to the deformation octahedral structure of RuOx/IrOx and the formation of stable Ru5+ species for OER. Theoretical calculations also reveal that the distorted structures can reduce the energy barrier of rate‐limiting step during OER. This work provides an efficient strategy for constructing structural distortion to achieve significant enhancement on the activity and stability of OER catalysts.
Structurally‐distorted CdRu2IrOx nanoframes with twisted Ru−O, Ir−O, and Ru–M (M = Ru, Ir) are successfully constructed via cation exchange and sequential thermal treatment, which can be used as ultra‐active and ultra‐stable acidic OER catalyst due to the strong synergy between Ru and Ir.
MicroRNAs (miRNAs) are small non-coding RNAs of approximately 22 nucleotides, which negatively regulate the gene expression at the post-transcriptional level. This study describes an update of the ...miRTarBase (http://miRTarBase.mbc.nctu.edu.tw/) that provides information about experimentally validated miRNA-target interactions (MTIs). The latest update of the miRTarBase expanded it to identify systematically Argonaute-miRNA-RNA interactions from 138 crosslinking and immunoprecipitation sequencing (CLIP-seq) data sets that were generated by 21 independent studies. The database contains 4966 articles, 7439 strongly validated MTIs (using reporter assays or western blots) and 348 007 MTIs from CLIP-seq. The number of MTIs in the miRTarBase has increased around 7-fold since the 2014 miRTarBase update. The miRNA and gene expression profiles from The Cancer Genome Atlas (TCGA) are integrated to provide an effective overview of this exponential growth in the miRNA experimental data. These improvements make the miRTarBase one of the more comprehensively annotated, experimentally validated miRNA-target interactions databases and motivate additional miRNA research efforts.
Despite the unique advantages of single‐atom catalysts, molecular dual‐active sites facilitate the C‐C coupling reaction for C2 products toward the CO2 reduction reaction (CO2RR). The Ni/Cu proximal ...dual‐active site catalyst (Ni/Cu‐PASC) is developed, which is a harmonic catalyst with dual‐active sites, by simply mixing commercial Ni‐phthalocyanine (Ni‐Pc) and Cu‐phthalocyanine (Cu‐Pc) molecules physically. According to scanning transmission electron microscopy (STEM) and transmission electron microscopy (TEM) energy dispersive spectroscopy (EDS) data, Ni and Cu atoms are separated, creating dual‐active sites for the CO2RR. The Ni/Cu‐PASC generates ethanol with an FE of 55%. Conversely, Ni‐Pc and Cu‐Pc have only detected single‐carbon products like CO and HCOO−. In situ X‐ray absorption spectroscopy (XAS) indicates that CO generation is caused by the stable Ni active site's balanced electronic state. The CO production from Ni‐Pc consistently increased the CO concentration over Cu sites attributed to subsequent reduction reaction through a C‐C coupling on nearby Cu. The CO bound (HCOO−) peak, which can be found on Cu‐Pc, vanishes on Ni/Cu‐PASC, as shown by in situ fourier transformation infrared (FTIR). The characteristic intermediate of *CHO instead of HCOO− proves to be the prerequisite for multi‐carbon products by electrochemical CO2RR. The work demonstrates that the harmonic dual‐active sites in Ni/Cu‐PASC can be readily available by the cascading proximal active Ni‐ and Cu‐Pc sites.
Ethanol is produced by a Ni/Cu dual active site in the Ni/Cu‐PASC catalyst. Because of the CO that has migrated from the Ni atom, a harmonious Ni/Cu dual atom site modifies the coordination bind site, converting the Cu‐*OCHO intermediate site to Cu‐*CHO. Ethanol is eventually produced when the Ni/Cu dual site facilitates the C‐C coupling via Cu‐*CHO‐CO
.
Solar fuel generation using seawater as the proton source is fascinating but challenging due to the detrimental chlorochemistry, the lack of active and stable oxygen evolution catalysts operating at ...seawater pH (∼8) and high turnover conditions. In the present study, iron phosphate modified calcium iron oxide (CaFeO
x
|FePO
4
) modified FTO electrodes were prepared, and their electrocatalytic properties towards the oxygen evolution reaction in both synthetic and natural seawater solutions were investigated. CaFeO
x
|FePO
4
was prepared by electrodepositing FePO
4
onto CaFeO
x
, prepared by spin-coating and a follow-up annealing process, under a constant applied current for different durations. Mg
2+
-induced fouling significantly reduces the activity of CaFeO
x
and slows down the activation process of CaFeO
x
, but can be mitigated by surface-modification of CaFeO
x
with FePO
4
. In addition, the presence of additional electrodeposited iron phosphate on the surface of CaFeO
x
attenuates the production of corrosive hypochlorite from chloride oxidation. With these unique properties of FePO
4
, the activated CaFeO
x
|FePO
4
electrode shows high activity and stability under high turnover conditions, reaching 10 mA cm
−2
at an overpotential of ∼710 mV, with a moderate increase in
η
(∼70 mV), mainly due to the change in solution pH, over 10 h of electrolysis in phosphate-buffered (0.5 M, pH 7) seawater solution.
CaFeO
x
modified with electrodeposited FePO
4
exhibits high activity and stability in natural seawater splitting.
Retinoic acid‐induced 1 (RAI1) encodes a transcriptional regulator critical for brain development and function. RAI1 haploinsufficiency in humans causes a syndromic autism spectrum disorder known as ...Smith−Magenis syndrome (SMS). The neuroanatomical distribution of RAI1 has not been quantitatively analyzed during the development of the prefrontal cortex, a brain region critical for cognitive function and social behaviors and commonly implicated in autism spectrum disorders, including SMS. Here, we performed comparative analyses to uncover the evolutionarily convergent and divergent expression profiles of RAI1 in major cell types during prefrontal cortex maturation in common marmoset monkeys (Callithrix jacchus) and mice (Mus musculus). We found that while RAI1 in both species is enriched in neurons, the percentage of excitatory neurons that express RAI1 is higher in newborn mice than in newborn marmosets. By contrast, RAI1 shows similar neural distribution in adult marmosets and adult mice. In marmosets, RAI1 is expressed in several primate‐specific cell types, including intralaminar astrocytes and MEIS2‐expressing prefrontal GABAergic neurons. At the molecular level, we discovered that RAI1 forms a protein complex with transcription factor 20 (TCF20), PHD finger protein 14 (PHF14), and high mobility group 20A (HMG20A) in the marmoset brain. In vitro assays in human cells revealed that TCF20 regulates RAI1 protein abundance. This work demonstrates that RAI1 expression and protein interactions are largely conserved but with some unique expression in primate‐specific cells. The results also suggest that altered RAI1 abundance could contribute to disease features in disorders caused by TCF20 dosage imbalance.
The SMS protein RAI1 shows primate‐specific expression patterns in newborn marmoset cortices. RAI1 forms an evolutionarily stable protein complex with TCF20, HMG20A, and PHF14 in the cortices of marmoset monkeys and mice. The protein stability of RAI1 is regulated by a paralogous protein TCF20.
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