Engineering the adsorption of molecules on active sites is an integral and challenging part for the design of highly efficient transition‐metal‐based catalysts for methanol dehydrogenation. A ...Mott–Schottky catalyst composed of Ni nanoparticles and tailorable nitrogen‐doped carbon‐foam (Ni/NCF) and thus tunable adsorption energy is presented for highly efficient and selective dehydrogenation of gas‐phase methanol to hydrogen and CO even under relatively high weight hourly space velocities (WHSV). Both theoretical and experimental results reveal the key role of the rectifying contact at the Ni/NCF boundaries in tailoring the electron density of Ni species and enhancing the absorption energies of methanol molecules, which leads to a remarkably high turnover frequency (TOF) value (356 mol methanol mol−1 Ni h−1 at 350 °C), outpacing previously reported bench‐marked transition‐metal catalysts 10‐fold.
Active boundaries: The ability of Mott–Schottky‐type nanocatalysts to change the adsorption energy of methanol molecules for highly efficient and selective dehydrogenation of gas‐phase methanol was achieved by constructing a Ni nanoparticle/N‐doped carbon‐foam catalyst. The electron redistribution along the Ni‐N‐doped carbon phase boundaries promotes adsorption and activation of methanol, thus boosting methanol dehydrogenation.
Coordination-driven self-assembly has emerged as a powerful bottom-up approach to construct various supramolecular architectures with increasing complexity and functionality. Tetraphenylethylene ...(TPE) has been incorporated into metallo-supramolecules to build luminescent materials based on aggregation-induced emission. We herein report three generations of ligands with full conjugation of TPE with 2,2':6',2″-terpyridine (TPY) to construct emissive materials. Due to the bulky size of TPY substituents, the intramolecular rotations of ligands are partially restricted even in dilute solution, thus leading to emission in both solution and aggregation states. Furthermore, TPE-TPY ligands are assembled with Cd(II) to introduce additional restriction of intramolecular rotation and immobilize fluorophores into rosette-like metallo-supramolecules ranging from generation 1-3 (G1-G3). More importantly, the fluorescent behavior of TPE-TPY ligands is preserved in these rosettes, which display tunable emissive properties with respect to different generations, particularly, pure white-light emission for G2.
Abstract
Background
Adding radiotherapy (RT) to systemic therapy improves progression-free survival (PFS) and overall survival (OS) in oligometastatic non-small cell lung cancer (NSCLC). Whether ...these findings translate to epidermal growth factor receptor (EGFR)–mutated NSCLC remains unknown. The SINDAS trial (NCT02893332) evaluated first-line tyrosine kinase inhibitor (TKI) therapy for EGFR-mutated synchronous oligometastatic NSCLC and randomized to upfront RT vs no RT; we now report the prespecified interim analysis at 68% accrual.
Methods
Inclusion criteria were biopsy-proven EGFR-mutated adenocarcinoma (per amplification refractory mutation system or next generation sequencing), with synchronous (newly diagnosed, treatment naïve) oligometastatic (≤5 metastases; ≤2 lesions in any one organ) NSCLC without brain metastases. All patients received a first-generation TKI (gefitinib, erlotinib, or icotinib), and randomization was between no RT vs RT (25-40 Gy in 5 fractions depending on tumor size and location) to all metastases and the primary tumor/involved regional lymphatics. The primary endpoint (intention to treat) was PFS. Secondary endpoints included OS and toxicities. All statistical tests were 2-sided.
Results
A total of 133 patients (n = 65 TKI only, n = 68 TKI with RT) were enrolled (2016-2019). The median follow-up was 23.6 months. The respective median PFS was 12.5 months vs 20.2 months (P < .001), and the median OS was 17.4 months vs 25.5 months (P < .001) for TKI only vs TKI with RT. Treatment yielded no grade 5 events and a 6% rate of symptomatic grade 3-4 pneumonitis in the TKI with RT arm. Based on the efficacy results of this prespecified interim analysis, the ethics committee recommended premature cessation of this trial.
Conclusions
As compared with a first-line TKI alone, addition of upfront local therapy using RT statistically significantly improved PFS and OS for EGFR-mutated NSCLC.
Graphene sheet/polymeric carbon nitride nanocomposite (GSCN) functions as a metal-free catalyst to activate O2 for the selective oxidation of secondary C–H bonds of cyclohexane. By fine-tuning the ...weight ratio of graphene and carbon nitride components, GSCN offers good conversion and high selectivity to corresponding ketones. Besides its high stability, this catalyst also exhibits high chemoselectivity for secondary C–H bonds of various saturated alkanes and, therefore, should be useful in overcoming challenges confronted by metal-mediated catalysis.
A three-dimensional (3-D) printed W -band slotted waveguide array antenna (SWAA) is proposed. The proposed SWAA consists of three different sections (two horizontal ones and a vertical one) such as a ...radiating waveguide array with 10 × 10 slots array with an aperture size of 31 mm × 31.4 mm, a coupling waveguide to feed the radiating waveguide array, and a vertical waveguide to feed the coupling waveguide. Machine learning technique based on artificial neural network algorithm is used to optimize the design. The optimized SWAA is fabricated using stereolithography apparatus (SLA) 3-D printing and then is metallized with silver on the inner and outer surfaces by jet metal spraying method. To metallize the inner and outer surfaces of the monolithic structure, nonradiating slots are added on the surface of the designed SWAA. The surface roughness is taken into account by employing the Huray-model methodology in simulation. The SWAA has a 22.5 dBi far-field gain, a −13.5 dB sidelobe level, and 10° half-power beamwidth (HPBW) at 78.7 GHz in measurement.
Photoactive, condensed carbon nitride nanorods (CNRs) can be obtained via confined thermal condensation of cyanamide inside the nanochannels of an anodic alumni oxide (AAO) membrane template. The ...promotion of a more condensed network of CNRs with lowered HOMO in water splitting (including both H2 and O2 revolution) and photocurrent output was demonstrated.
•A linear source infiltrability measurement system was applied to capture the complete infiltration processes.•Grasses promote soil physical properties and infiltrability better than shrubs in ...heavy-textured soil.•The effects of plant roots on soil infiltrability are mediated via soil aggregate stability and soil porosity.•Species mixtures require inclusion of high fine root length density grasses to mitigate overland flow and erosion.
Soil degradation impairs ecosystem functions, and vegetation restoration is a major eco-engineering method that is used to restore soils globally. Despite the fundamental role that plants play in enhancing soil functions and ecosystem services, little is known about the relationships among root traits, soil physical properties, and water infiltration. The objectives of this study were to therefore evaluate changes in soil infiltrability due to different vegetation types and identify soil properties and root trait predictors of variation in soil infiltrability. The influences of four plant species (two gramineous grasses and two leguminous shrubs) on physical properties of soil and water infiltration in heavy-textured soils with 43 % clay content following five years of restoration after surface soil removal were investigated. These data were subsequently incorporated into a conceptual path model to quantify the direct and indirect effects of root traits and root-induced soil properties on infiltration. Soil organic matter, aggregate stability, soil total porosity, and non-capillary porosity were significantly higher in planted soil than in bare soil (p < 0.05), following the order of grass-planted > shrub-planted > bare soils. The infiltration rates during the initial and steady states were 63 % and 38 % higher in grass-planted soils than in shrub-planted soils, respectively. Among all evaluated root traits, fine root length density was the best predictor of these changes. Furthermore, the conceptual path model explained 82 % of the variance in water infiltration and confirmed the important role of roots in soil infiltration. Modeling indicated that this might not be a direct effect, but is rather mediated via soil physical properties like soil aggregate stability and soil porosity. These observations have important implications for designing efficient strategies in restoration of human-induced disturbed soils to mitigate overland flows and erosion.
Pd nanoparticles were successfully encapsulated inside mesoporous silicalite‐1 nanocrystals (Pd@mnc‐S1) by a one‐pot method. The as‐synthesized Pd@mnc‐S1 with excellent stability functioned as an ...active and reusable heterogeneous catalyst. The unique porosity and nanostructure of silicalite‐1 crystals endowed the Pd@mnc‐S1 material general shape‐selectivity for various catalytic reactions, including selective hydrogenation, oxidation, and carbon–carbon coupling reactions.
Shape‐selective reactions over a palladium nanoparticle (Pd NP) based catalyst were achieved by integrating Pd NPs inside mesoporous silicalite‐1 nanocrystals. The unique micro‐ and mesoporous structure of the zeolite nanocrystals endowed Pd NPs both high stability and excellent shape selectivity for organic synthesis.
The visionary idea that RNA adopts nonbiological roles in today's nanomaterial world has been nothing short of phenomenal. These RNA molecules have ample chemical functionality and self‐assemble to ...form distinct nanostructures in response to external stimuli. They may be combined with inorganic materials to produce nanomachines that carry cargo to a target site in a controlled manner and respond dynamically to environmental changes. Comparable to biological cells, programmed RNA nanomachines have the potential to replicate bone healing in vitro. Here, an RNA–biomineral nanomachine is developed, which accomplishes intrafibrillar and extrafibrillar mineralization of collagen scaffolds to mimic bone formation in vitro. Molecular dynamics simulation indicates that noncovalent hydrogen bonding provides the energy source that initiates self‐assembly of these nanomachines. Incorporation of the RNA–biomineral nanomachines into collagen scaffolds in vivo creates an osteoinductive microenvironment within a bone defect that is conducive to rapid biomineralization and osteogenesis. Addition of RNA‐degrading enzymes into RNA–biomineral nanomachines further creates a stop signal that inhibits unwarranted bone formation in tissues. The potential of RNA in building functional nanostructures has been underestimated in the past. The concept of RNA–biomineral nanomachines participating in physiological processes may transform the nanoscopic world of life science.
An RNA–amorphous calcium phosphate nanomachine that induces extrafibrillar and intrafibrillar mineralization of collagen fibrils and regenerates new bone in a dynamic and programmable manner is developed. This multifunctional nanomachinery is comparable to the function of osteoblasts. The RNA–biomineral nanomachines that simulate physiological processes brings new opportunities and challenges to bone tissue engineering.
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