The modulation of electron density is an effective option for efficient alternative electrocatalysts. Here, p‐n junctions are constructed in 3D free‐standing FeNi‐LDH/CoP/carbon cloth (CC) electrode ...(LDH=layered double hydroxide). The positively charged FeNi‐LDH in the space‐charge region can significantly boost oxygen evolution reaction. Therefore, the j at 1.485 V (vs. RHE) of FeNi‐LDH/CoP/CC achieves ca. 10‐fold and ca. 100‐fold increases compared to those of FeNi‐LDH/CC and CoP/CC, respectively. Density functional theory calculation reveals OH− has a stronger trend to adsorb on the surface of FeNi‐LDH side in the p‐n junction compared to individual FeNi‐LDH further verifying the synergistic effect in the p‐n junction. Additionally, it represents excellent activity toward water splitting. The utilization of heterojunctions would open up an entirely new possibility to purposefully regulate the electronic structure of active sites and promote their catalytic activities.
The p‐n junction in FeNi‐LDH/CoP with positively charged FeNi‐LDH in the space‐charge region exhibits superior electro‐catalytical activity for the oxygen evolution reaction (OER). LDH=layered double hydroxide.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
For high-temperature catalytic reaction, it is of significant importance and challenge to construct stable active sites in catalysts. Herein, we report the construction of sufficient and stable ...copper clusters in the copper‒ceria catalyst with high Cu loading (15 wt.%) for the high-temperature reverse water gas shift (RWGS) reaction. Under very harsh working conditions, the ceria nanorods suffered a partial sintering, on which the 2D and 3D copper clusters were formed. This partially sintered catalyst exhibits unmatched activity and excellent durability at high temperature. The interaction between the copper and ceria ensures the copper clusters stably anchored on the surface of ceria. Abundant in situ generated and consumed surface oxygen vacancies form synergistic effect with adjacent copper clusters to promote the reaction process. This work investigates the structure-function relation of the catalyst with sintered and inhomogeneous structure and explores the potential application of the sintered catalyst in C1 chemistry.
The cobalt‐catalyzed alkoxylation of C(sp2)H bonds in aromatic and olefinic carboxamides has been developed. The reaction proceeded under mild conditions in the presence of Co(OAc)2⋅4H2O as the ...catalyst and tolerates a wide range of both alcohols and benzamide substrates, including even olefinic carboxamides. In addition, this reaction is the first example of the direct alkoxylation of alkenes through CH bond activation.
Alcohols in action: A wide range of alcohols and benzamide substrates functionalized with electron‐rich or electron‐poor substituents are tolerated in the title reaction. This practical reaction occurs under mild conditions.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
For the past three decades, the coordination-driven self-assembly of three-dimensional structures has undergone rapid progress; however, parallel efforts to create large discrete two-dimensional ...architectures-as opposed to polymers-have met with limited success. The synthesis of metallo-supramolecular systems with well-defined shapes and sizes in the range of 10-100 nm remains challenging. Here we report the construction of a series of giant supramolecular hexagonal grids, with diameters on the order of 20 nm and molecular weights greater than 65 kDa, through a combination of intra- and intermolecular metal-mediated self-assembly steps. The hexagonal intermediates and the resulting self-assembled grid architectures were imaged at submolecular resolution by scanning tunnelling microscopy. Characterization (including by scanning tunnelling spectroscopy) enabled the unambiguous atomic-scale determination of fourteen hexagonal grid isomers.
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FZAB, GEOZS, IJS, IMTLJ, KILJ, KISLJ, MFDPS, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, SBMB, SBNM, UKNU, UL, UM, UPUK, VKSCE, ZAGLJ
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.
A highly efficient cobalt(II)‐catalyzed alkynylation/annulation of terminal alkynes assisted by an N,O‐bidentate directing group is described. This protocol is characterized by wide substrate scope ...utilizing cheap cobalt catalysts, and offers a new approach to 3‐methyleneisoindolin‐1‐one, which can be converted into an oxadiazine salt in one step. Moreover, the directing group could be removed in three steps.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
Using the near-detailed-balance distribution function obtained in our recent work, we present a set of covariant gravito-thermal transport equations (i.e. the flow of various charges as linear ...response to thermodynamical forces) for neutral relativistic gases in a generic stationary spacetime. All relevant tensorial transport coefficients are worked out and are presented using some particular integration functions in (α,ζ), where α=−βμ and ζ=βm is the relativistic coldness, with β being the inverse temperature and μ being the chemical potential. It is shown that the Onsager reciprocal relation holds in the gravito-thermal transport phenomena, and that the heat conductivity and the gravito-conductivity tensors are proportional to each other, with the coefficient of proportionality given by the product of the so-called Lorenz number with the temperature, thus proving a gravitational variant of the Wiedemann-Franz law. It is remarkable that, for strongly degenerate Fermi gases, the Lorenz number takes a universal constant value L=π2/3, which extends the Wiedemann-Franz law into the Wiedemann-Franz-Lorenz law.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
Control of solar transmission through windows promises to reduce building energy consumption. However, the ability of current chromogenic technologies to regulate solar gain with the tunable ...extinction of phase-change materials is still far from optimum. We report a strategy for optimizing the transmittance modulation range of temperature-responsive hydrogel particles by means of tuning the light-scattering behaviors through controlling particle size and internal structure. An emerging thermochromic material, poly(N-isopropylacrylamide)-2-aminoethylmethacrylate hydrochloride (pNIPAm-AEMA) microparticles, was synthesized to demonstrate this strategy. The average size of pNIPAm-AEMA microparticles varies from 1,388 nm at 25°C to 546 nm at 35°C, contributing to an unprecedented infrared transmittance modulation of 75.6%. A high luminous transmittance of 87.2% at 25°C had also been accomplished. An investigation of the tunable scattering behaviors of pNIPAm-AEMA particles provided mechanistic insight into light management by this class of materials, the application field of which is beyond energy-saving smart windows.
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•Full solar spectrum transmission modulation by pNIPAm-AEMA hydrogel microparticles•Methodical tuning of scattering with prescribed particle size and internal structure•Unprecedented IR transmission modulation by extending the scattering range•Outstanding stability and scalability of thermochromic hydrogel device
Intelligent control of solar irradiance through windows is promising to reduce building energy consumption by at least 1.055 × 1015 kJ/year in the United States. Light management with thermochromic smart windows holds practical significance due to their autonomous system and simplicity of the device. However, the conventional thermochromic material (VO2) faces scientific challenges with a high phase-transition temperature (68°C) and poor thermochromic performance. Temperature-responsive hydrogel emerges as a promising alternative, whereby light management could be pursued by maneuvering the light-scattering behaviors. This work reports the strategy to explore the thermochromic performance of co-polymerized hydrogel microparticles with the aid of tailoring particle size and internal structure. The solar modulation was effectively extended into the infrared region, and an unprecedented solar transmittance modulation of 81.3% was achieved at ∼32°C by our hydrogel thermochromic device with great scalability and stability.
This article reports the intelligent control of solar gain through windows based on the tunable scattering behaviors of temperature-responsive hydrogel particles. High luminous transmittance and broadband solar transmittance modulation including unprecedented IR modulation are simultaneously achieved for the first time using co-polymerized pNIPA-AEMA microparticles with prescribed particle size and internal structure. The design strategy to maneuver the real part of refractive index is applicable for broader fields beyond energy-saving smart windows.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
The separation attitude of air-to-air missile to fighter should be adjusted adaptively in wide range to meet the missile-aircraft separation requirements under different flight states, but current ...ejection separation mechanism with fixed separation attitude could not meet the requirements. To solve this problem, a metamorphic ejection separation mechanism is proposed. Metamorphic PR-R kinematic pair is used to replace traditional hinge kinematic pair in the key hinge of ejection separation mechanism, the ejection forces of the front and rear push arm to missile are changed in real time, then missile ejection separation attitude could be adjusted adaptively in wide range. Multi-body dynamics model of metamorphic ejection separation mechanism is established, and the dynamics simulation analysis is carried out. Simulation results shows that the proposed metamorphic ejection separation mechanism could adjust separation attitude in wide range, which lays a foundation for the further realization of real-time intell
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