Lithium‐rich disordered rock‐salt oxides have attracted great interest owing to their promising performance as Li‐ion battery cathodes. While experimental and theoretical efforts are critical in advancing this class of materials, a fundamental understanding of key property changes upon Li extraction is largely missing. In the present study, single‐crystal synthesis of a new disordered rock‐salt cathode material, Li1.3Ta0.3Mn0.4O2 (LTMO), and its use as a model compound to investigate Li concentration–driven evolution of local cationic ordering, charge compensation, and chemical distribution are reported. Through the combined use of 2D and 3D X‐ray nanotomography, it is shown that Li removal accompanied by oxygen oxidation is correlated with the development of morphological defects such as particle cracking. Chemical heterogeneity, quantified by subparticle level distribution of Mn valence state, is minimal during Mn redox, which drastically increases upon the formation of cracks during oxygen redox. Density functional theory and bond valence sum mismatch calculations reveal the presence of local short‐range ordering in the pristine oxide, which gradually disappears along with the extraction of Li. The study suggests that with cycling the transformation into true cation–disordered state can be expected, which likely impacts the voltage profile and obtainable energy density of the oxide cathodes. 相似文献
We present a new scheme for visibly-opaque but near-infrared-transmitting filters involving 7 layers based on one-dimensional ternary photonic crystals, with capabilities in reaching nearly 100% transmission efficiency in the near-infrared region. Different decorative reflection colors can be created by adding additional three layers while maintaining the near-infrared transmission performance. In addition, our proposed structural colors show great angular insensitivity up to ±60° for both transverse electric and transverse magnetic polarizations, which are highly desired in various fields. The facile strategy described here involves a simple deposition method for the fabrication, thereby having great potential in diverse applications such as image sensors, anti-counterfeit tag, and optical measurement systems.
The case-based learning (CBL) approach has gained attention in medical education as an alternative to traditional learning methodology. However, current CBL systems do not facilitate and provide computer-based domain knowledge to medical students for solving real-world clinical cases during CBL practice. To automate CBL, clinical documents are beneficial for constructing domain knowledge. In the literature, most systems and methodologies require a knowledge engineer to construct machine-readable knowledge. Keeping in view these facts, we present a knowledge construction methodology (KCM-CD) to construct domain knowledge ontology (i.e., structured declarative knowledge) from unstructured text in a systematic way using artificial intelligence techniques, with minimum intervention from a knowledge engineer. To utilize the strength of humans and computers, and to realize the KCM-CD methodology, an interactive case-based learning system(iCBLS) was developed. Finally, the developed ontological model was evaluated to evaluate the quality of domain knowledge in terms of coherence measure. The results showed that the overall domain model has positive coherence values, indicating that all words in each branch of the domain ontology are correlated with each other and the quality of the developed model is acceptable. 相似文献
This Concept article describes the latest developments in the emerging area of late-stage biocatalytic alkylation. Central to these developments is the ability to efficiently prepare S-adenosyl methionine (SAM) cofactor analogues and couple this with enzymatic alkyl transfer. Recent developments in the enzymatic synthesis of SAM cofactor analogues are summarized first, followed by their application as alkyl transfer agents catalyzed by methyltransferases (MTases). Second, innovative methods to regenerate SAM cofactors by enzymatic cascades is reported. Finally, future opportunities towards establishing a generalized platform for late-stage alkylation are described. 相似文献
While qualitative studies have identified chlorogenic acids in antioxidant extracts, particularly ethyl acetate‐derived extracts, of Taraxacum officinale, quantitative analysis of these phenolic compounds remains largely unreported for this species. In this study, bioactivity‐guided fractionation of an antioxidant crude ethyl acetate extract (DPPH = 295.481 ± 0.955 mg TE g?1 extract) from T. officinale root resulted in a number of reverse‐phase fractions that demonstrated high antioxidant activity (DPPH = 1058.733–1312.136 mg TE g?1 extract), stronger than that of the synthetic antioxidant Trolox®. UPLC‐MS/MS screening of these fractions for the presence of selected mono‐ and di‐caffeoylquinic acids revealed large quantities of 1,5‐dicaffeoylquinic acid present in several fractions (853.052–907.324 μg mg?1), respectively. Due to the antioxidant potency and high levels of 1,5‐dicaffeoylquinic acid observed in these fractions, it was concluded that specifically this chlorogenic acid derivative is a major contributor to the antioxidant efficacy of dandelion root. 相似文献
The purpose of present study was to develop and evaluate methods to assess stimulation responses of the lumbar extensors, as part of a longer‐term goal of detecting fatigue during prolonged sitting. Three stimulation frequencies (2, 5, and 8 Hz) were tested in separate stages, which include 3 stimulation trains and 4 sampling blocks. Repeated measures analyses of variance were used to determine whether any significant differences in mean stimulation responses occurred with respect to stimulation frequency, sampling block, and stimulation train. Reliability of measured stimulation responses was assessed within and between sampling blocks using intraclass correlation coefficients. Stimulation frequencies significantly affected the stimulation responses and time‐to‐potentiation differed between the 3 stimulation frequencies; it was highest for 2 Hz stimulation. All 3 stimulation frequencies resulted in excellent reliability within and between sampling blocks. Use of the current protocol at 2 Hz is recommended as appropriate to measure the lumbar extensors status during prolonged sitting. 相似文献
C-axis textured thin films of gallium-doped indium zinc oxide (GIZO) with a 2% ratio of Ga/Zn, were obtained via RF-magnetron sputtering with high transparency and electrical conductivity. A Box-Behnken response surface design was used to evaluate the effects of the deposition parameters (In2O3 target power, deposition time, and substrate temperature) on the chemical composition, optical, electrical, and structural properties of the GIZO films. The optical constants and the electrical properties were obtained using optical models. The GIZO stoichiometry, and therefore the In/Zn atomic ratio, affected the crystallinity, crystalline parameters, band gap, and charge carrier mobility of the GIZO films. The charge carrier density was related to the change in the crystalline parameters of the hexagonal structure and the In/Zn atomic ratio. The best electrical conductivity values (1.75?×?103 Ω?1 cm?1) were obtained for GIZO films with In/Zn ratio ≥?1. Several figures of merit (FOM) defined for the visible and solar regions were comparatively used to select the optimal In/Zn atomic ratio that provided the best balance between the conductivity and the transparency. The optimal In/Zn ratio was in a range of 0.85–0.90 for the GIZO films. 相似文献