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Diameter is a critical parameter for determining the physical properties of a submicrometer optical fiber and requires an accurate measurement. In this study, we proposed, to our knowledge, a novel diameter measurement technique derived from the waveguide theory, utilizing the pitch of a standing-wave near-field light generated by two counter-propagating lights within the submicrometer optical fiber. In a submicrometer optical fiber, the propagating light extends into the surrounding air as near-field light, existing within a range approximately equivalent to one wavelength from the surface of the fiber. By generating the standing-wave near-field light with the incident lights from both ends of the fiber, the pitch of the standing-wave near-field light can be measured by scanning along the fiber's central axis with a scanning near-field optical microscopy probe. The fiber diameter is subsequently acquired by solving the optical fiber eigenvalue equation. Based on the feasibility verification experiment, a high-precision measurement of approximately 0.50â µm was realized for the diameter of the optical fiber.
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The electrochemical nitrate reduction reaction (NO3RR) is a promising alternative synthetic route for sustainable ammonia (NH3) production, because it not only eliminates nitrate (NO3-) from water but also produces NH3 under mild operating conditions. However, owing to the complicated eight-electron reaction and the competition from the hydrogen evolution reaction, developing catalysts with high activities and Faradaic efficiencies (FEs) is highly imperative to improve the reaction performance. In this study, Cu-doped Fe3O4 flakes are fabricated and demonstrated to be excellent catalysts for electrochemical conversion of NO3- to NH3, with a maximum FE of â¼100% and an NH3 yield of 179.55 ± 16.37 mg h-1 mgcat-1 at -0.6 V vs RHE. Theoretical calculations reveal that doping the catalyst surface with Cu results in a more thermodynamically facile reaction. These results highlight the feasibility of promoting the NO3RR activity using heteroatom doping strategies.
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BACKGROUND: Phenolic endocrine-disrupting chemicals (EDCs) are widespread and easily ingested through the food chain. They pose a serious threat to human health. Magnetic solid-phase extraction (MSPE) is an effective sample pre-treatment technology to determine traces of phenolic EDCs. RESULTS: Magnetic covalent organic framework (COF) (Fe3 O4 @COF) nanospheres were prepared and characterized. The efficient and selective extraction of phenolic EDCs relies on a large specific surface and the inherent porosity of COFs and hydrogen bonding, π-π, and hydrophobic interactions between COF shells and phenolic EDCs. Under optimal conditions, the proposed magnetic solid-phase extraction-high-performance liquid chromatography-ultra violet (MSPE-HPLC-UV) based on the metallic covalent organic framework method for phenolic EDCs shows good linearities (0.002-6 µg mL-1 ), with R2 of 0.995 or higher, and low limits of detection (6-1.200 ng mL-1 ). CONCLUSION: Magnetic covalent organic frameworks (Fe3 O4 @COFs) with good MSPE performance for phenolic EDCs were synthesized by the solvothermal method. The magnetic covalent organic framework-based MSPE-HPLC-UV method was applied successfully to determine phenolic EDCs in beverage and water samples with satisfactory recoveries (90.200%-123%) and relative standard deviations (2.100%-12.100%). © 2023 Society of Chemical Industry.
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Disruptores Endócrinos , Estruturas Metalorgânicas , Humanos , Estruturas Metalorgânicas/química , Cromatografia Líquida de Alta Pressão , Bebidas , Extração em Fase Sólida/métodos , Fenóis , Fenômenos Magnéticos , Água/química , Limite de DetecçãoRESUMO
Photocatalytic CO2 reduction into ideal hydrocarbon fuels, such as CH4 , is a sluggish kinetic process involving adsorption of multiple intermediates and multi-electron steps. Achieving high CH4 activity and selectivity therefore remains a great challenge, which largely depends on the efficiency of photogenerated charge separation and transfer as well as the intermediate energy levels in CO2 reduction. Herein, we construct La and Cu dual-atom anchored carbon nitride (LaCu/CN), with La-N4 and Cu-N3 coordination bonds connected by Cu-N-La bridges. The asymmetric Cu-N-La species enables the establishment of an atomic-level donor-acceptor structure, which allows the migration of electrons from La atoms to the reactive Cu atom sites. Simultaneously, intermediates during CO2 reduction on LaCu/CN demonstrate thermodynamically more favorable process for CH4 formation based on theoretical calculations. Eventually, LaCu/CN exhibits a high selectivity (91.6 %) for CH4 formation with a yield of 125.8â µmol g-1 , over ten times of that for pristine CN. This work presents a strategy for designing multi-functional dual-atom based photocatalysts.
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Catalysts involving post-transition metals have shown almost invincible performance on generating formate in electrochemical CO2 reduction reaction (CO2 RR). Conversely, Cu without post-transition metals has struggled to achieve comparable activity. In this study, a sulfur (S)-doped-copper (Cu)-based catalyst is developed, exhibiting excellent performance in formate generation with a maximum Faradaic efficiency of 92 % and a partial current density of 321â mA cm-2 . Ex situ structural elucidations reveal the presence of abundant grain boundaries and high retention of S-S bonds from the covellite phase during CO2 RR. Furthermore, thermodynamic calculations demonstrate that S-S bonds can moderate the binding energies with various intermediates, further improving the activity of the formate pathway. This work is significant in modifying a low-cost catalyst (Cu) with a non-metallic element (S) to achieve comparable performance to mainstream catalysts for formate generation in industrial grade.
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There is a lack of effective programmed cell death protein 1 (PD-1)-targeted immunotherapy with good tolerability in patients with advanced hepatocellular carcinoma (HCC) and severely compromised liver function. We assessed patient outcomes after combined camrelizumab and molecular targeted therapy in a multicenter cohort study in China. The study included 99 patients with advanced HCC (58 Child-Pugh A and 41 Child-Pugh B), 84 of them received camrelizumab combined with molecular targeted therapy from January 10, 2019, to March 31, 2021. Overall survival (OS), progression-free survival (PFS), objective response rate (ORR), disease control rate (DCR), and adverse events (AEs) were assessed. The median follow-up was 12.1 months. For patients with Child-Pugh B, the OS probability at 12-months, ORR and DCR were 49.7%, 31.7% and 65.9%, respectively, and the median PFS was 5.1 months [95% confidence interval (CI) 3.0-7.1], which were comparable with Child-Pugh A patients, although median OS was shorter in Child-Pugh B patients (20.5 vs.13.4 months, P = 0.12). In multivariate analysis, macrovascular infiltration (MVI), but not sex, age, hepatitis B virus etiology, extrahepatic metastasis, Child-Pugh B, or AFP > 400 ng/ml, was associated with 12-months OS [hazard ratio (HR) 2.970, 95% CI 1.276-6.917, P = 0.012] and ORR (HR 2.906, 95% CI 1.18-7.16, P = 0.020). Grade 3/4 immune-related AEs occurred in 26.8% of Child-Pugh B patients, including one potentially treatment-related death. In both groups, the most common AEs were immune thrombocytopenia and hepatotoxicity. Camrelizumab combined with targeted therapy showed favorable effectiveness and tolerability with manageable toxicities in Chinese HCC patients, regardless of Child-Pugh A/B liver function. MVI was associated with suboptimal immunotherapy response and poor prognosis.
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Carcinoma Hepatocelular , Neoplasias Hepáticas , Humanos , Carcinoma Hepatocelular/patologia , Neoplasias Hepáticas/patologia , Terapia de Alvo Molecular , Estudos de CoortesRESUMO
Although increasing efforts have been devoted to the development of non-invasive wearable or stretchable electrochemical sweat sensors for monitoring physiological and metabolic information, most of them still suffer from poor stability and specificity over time and fluctuating temperatures. This study reports the design and fabrication of a long-term stable and highly sensitive flexible electrochemical sensor based on nanocomposite-modified porous graphene by simple and facile laser treatment for detecting biomarkers such as glucose in sweat. The laser-reduced and patterned stable conductive nanocomposite on the porous graphene electrode provides the resulting glucose sensor with an excellent sensitivity of 1317.69 µAmM-1cm-2 with an ultra-low limit of detection (LOD) of 0.079 µM. The sensor can also detect pH and exhibit extraordinary stability to maintain more than 91% sensitivity over 21 days in ambient conditions. Taken together with a temperature sensor based on the same material system, the dual glucose and pH sensor integrated with a flexible microfluidic sweat sampling network further results in accurate continuous on-body glucose detection calibrated by the simultaneously measured pH and temperature. The low-cost, highly sensitive, and long-term stable platform could facilitate and pave the way for the early identification and continuous monitoring of different biomarkers for non-invasive disease diagnosis and treatment evaluation.
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Phase (composition) is known to play a key role in determining the electronic and optical properties of amorphous oxide semiconductors. In this work, modulating the ultrafast nonlinear optical (NLO) response of SnO2 and SnO thin films by tuning oxygen partial pressure during film sputtering is explored. Femtosecond Z-scan results demonstrate that intermediate phases have no profound impact on the two-photon absorption (TPA) response of SnO2 and SnO films. Interestingly, the magnitude of the effective nonlinear absorption coefficient (ßeff) of both intermediate SnO2-x and SnOx are enhanced after the change of Sn2+/Sn4+ composition ratio, as measured by picosecond Z-scan technique. Femtosecond degenerate pump-probe measurements show that intermediate phases accelerate the carrier trapping and improve the defect-related carrier absorption in SnOx (SnO-rich) film, while intermediate phase suppress the TPA response of SnO2-x (SnO2-rich) films, therefore carrier-induced absorption dominates the NLO behavior of SnO2-x film on picosecond regime. Our results indicate a simple and effective way to modulate the NLO response of transparent conductive oxide SnO2 and SnO.
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Optical multiplexing is a pivotal technique for augmenting the capacity of optical data storage (ODS) and increasing the security of anti-counterfeiting. However, due to the dearth of appropriate storage media, optical multiplexing is generally restricted to a single dimension, thus curtailing the encoding capacity. Herein, the co-multiplexing spectral and temporal dimensions are proposed for optical encoding based on photoluminescence (PL) and persistent-luminescence (PersL) at four different wavelengths. Each emission color comprises four luminescence modes. The further multiplexing of four wavelengths leads to the maximum encoding capacity of 8 bits at each pixel. The wavelength difference between adjacent peaks is larger than 50â nm. The well-separated emission wavelengths significantly lower the requirements for high-resolution spectrometers. Moreover, the information is unable to be decoded until both PL and PersL spectra are collected, suggesting a substantial improvement in information security and the security level of anti-counterfeiting.
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We have designed a metal-semiconductor-metal (MSM) solar-blind ultraviolet (UV) photodetector (PD) by utilizing Al0.55Ga0.45N/Al0.4Ga0.6N/Al0.65Ga0.35N heterostructures. The interdigital Ni/Au metal stack is deposited on the Al0.55Ga0.45N layer to form Schottky contacts. The AlGaN hetero-epilayers with varying Al content contribute to the formation of a two-dimensional electron gas (2DEG) conduction channel and the enhancement of the built-in electric field in the Al0.4Ga0.6N absorption layer. This strong electric field facilitates the efficient separation of photogenerated electron-hole pairs. Consequently, the fabricated PD exhibits an ultra-low dark current of 1.6 × 10-11 A and a broad spectral response ranging from 220 to 280â nm, with a peak responsivity of 14.08 A/W at -20â V. Besides, the PD demonstrates an ultrahigh detectivity of 2.28 × 1013 Jones at -5â V. Furthermore, to investigate the underlying physical mechanism of the designed solar-blind UV PD, we have conducted comprehensive two-dimensional device simulations.
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Compounds with ordered and interconnected channels have versatile multifunctional applications in technological fields. In this work, we report the intrinsic- and Eu3+-activated luminescence in NbAlO4 with a wide channel structure. NbAlO4 is an n-type semiconductor with an indirect allowed transition and a band-gap energy of 3.26 eV. The conduction band and valence band are composed of Nb 3d and O 2p states, respectively. Unlike the common niobate oxide Nb2O5, NbAlO4 exhibits efficient self-activated luminescence with good thermal stability even at room temperature. The AlO4 tetrahedron effectively blocks the transfer/dispersion of excitation energy between NbO6 chains in NbAlO4, allowing for effective self-activated luminescence from NbO6 activation centers. Moreover, Eu3+-doped NbAlO4 displayed a bright red luminescence of 5D0 â 7F2 transition at 610 nm. The site-selective excitation and luminescence of Eu3+ ions in a spectroscopic probe were utilized to investigate the doping mechanism. It is evidenced that Eu3+ is doped in the structure channel in NbAlO4 lattices, not in the normal cation sites of Nb5+ or Al3+. The experimental findings are valuable in developing new luminescent materials and improving the understanding of the material's channel structure.
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Photovoltaic device is highly dependent on the weather, which is completely ineffective on rainy days. Therefore, it is very significant to design an all-weather power generation system that can utilize a variety of natural energy. This work develops a water droplet friction power generation (WDFG)/solar-thermal power generation (STG) hybrid system. The WDFG consists of two metal electrodes and a candle soot/polymer composite film, which also can be regarded as a capacitor. Thus, the capacitor coupled power generation (C-WDFG) device can achieve a sustainable and stable direct-current (DC) output under continuous dripping without external conversion circuits. A single device can produce an open-circuit voltage of ca.0.52 V and a short-circuit current of ca.0.06 mA, which can be further scaled up through series or parallel connection to drive commercial electronics. Moreover, we demonstrate that the C-WDFG is highly compatible with the thermoelectric device. The excellent photothermal performance of soot/polymer composite film can efficiently convert solar into heat, which is then converted to electricity by the thermoelectric device. Therefore, this C-WDFG/STG hybrid system can work in both rainy and sunny days.
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The discovery of two-dimensional (2D) magnetic materials makes it possible to realize in-plane magnetic tunnel junctions. In this study, the transport characteristics of an in-plane double barrier magnetic tunnel junction (IDB-MTJ) based on Cr2C have been studied by density functional theory combined with the nonequilibrium Green's function method. The results showed its maximum tunneling magnetoresistance ratio (TMR) value reached 6.58 × 1010. Its minimum TMR value (3.86 × 106) was also comparable to those of conventional field effect transistors (FETs). Due to its giant TMR and unique structural characteristics, the IDB-MTJ based on Cr2C has great potential applications in magnetic random access memory (MRAM) and logic computing.
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The conventional industrial production of nitrogen-containing fertilizers, such as urea and ammonia, relies heavily on energy-intensive processes, accounting for approximately 3 % of global annual CO2 emissions. Herein, we report a sustainable electrocatalytic approach that realizes direct and selective synthesis of urea and ammonia from co-reduction of CO2 and nitrates under ambient conditions. With the assistance of a copper (Cu)-based salphen organic catalyst, outstanding urea (3.64â mg h-1 mgcat -1 ) and ammonia (9.73â mg h-1 mgcat -1 ) yield rates are achieved, in addition to a remarkable Faradaic efficiency of 57.9±3 % for the former. This work proposes an appealing sustainable route to converting greenhouse gas and waste nitrates by renewable energies into value-added fertilizers.
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Our recent work has demonstrated that the spin-dependent photogalvanic effect (PGE) is an ideal way to induce pure spin current in certain centrosymmetric systems (X. Tao, P. Jiang, H. Hao, X. Zheng, L. Zhang and Z. Zeng, Phys. Rev. B, 2020, 102, 081402), and thus the search for appropriate materials or structures is the key to realize it. Here, we theoretically propose a spin optoelectric device with α-phase carbon phosphide nanoribbons (α-CPNRs) to generate pure spin current by PGE using density functional theory simulation. By designing an α-CPNR based device with a centrosymmetric structure, due to the structural inversion symmetry and real space spin polarization antisymmetry of the system, the PGE induced pure spin current without any accompanying charge current can be always obtained, independent of polarization type and polarization angle of the photons. Furthermore, the magnitude of pure spin current can be greatly increased (nearly by an order of magnitude) by applying antiparallel electrical fields in the two leads to tune the spin density and band structure. Furthermore, by applying parallel electrical fields, a fully spin-polarized photocurrent can be produced in this system, suggesting a fantastic scheme to achieve half-metallic transport, another important goal in spintronics. These investigations suggest that the optoelectric devices constructed by α-CPNRs will have great potential in spintronics.
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Magnetic tunnel junctions (MTJs) have attained new opportunities due to the emergence of two-dimensional (2D) magnetic materials after they were proposed more than forty years ago. Here, an in-plane double barrier magnetic tunnel junction (IDB-MTJ) based on B vacancy h-NB nanoribbons has been proposed firstly, and the transport properties have been studied using density functional theory combined with the nonequilibrium Green's function method. Due to its unique structural characteristics, the tunneling magnetoresistance (TMR) ratio can be tuned and the maximum TMR can reach 1.86 × 105. The potential applications of the IDB-MTJ in magnetic random-access memories and logical computation have also been discussed. We find that the IDB-MTJs have great potential in magnetic random-access memories and logical computation applications.
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The high carrier mobility, appropriate band gap and good environmental stability of two-dimensional (2D) MoSi2N4 enable it to be an appropriate channel material for transistors with excellent performance. Therefore, we predict the performance of double-gate (DG) metal-oxide-semiconductor field-effect transistors (MOSFETs) based on monolayer (ML) MoSi2N4 by ab initio quantum-transport calculations. The results show that the on-state current of the p-type device is remarkable when the gate length is greater than 4 nm, which can meet the high performance requirements of the International Technology Roadmap for Semiconductors (ITRS), 2013 version. Moreover, the gate length can be reduced to 3 nm when an underlap (UL) structure is employed in the MOSFET, and the sub-threshold swing, intrinsic delay time and power consumption also perform well. The calculation results reveal that ML MoSi2N4 will be a promising alternative for transistor channel materials in the post-silicon era.
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Staphylococcus aureus (S. aureus) is a pathogen closely associated with foodborne diseases. We prepared a reliable colorimetric sensor to detect S. aureus using click chemical reaction and immunomagnetic separation. Aptamer-functionalized and ALP-labeled Fe3O4 NPs act as separation and signal transduction elements. Under the optimized conditions, the Cu+ generated by signal transduction triggers a click chemistry reaction, which causes the aggregation of azides and alkyne-AuNPs and a color change. The net extinction ratio of Δ(A530/A760) was linearly correlated with the S. aureus concentration from 10 to 106 cfu mL-1, and the limit detection was 2.4 cfu mL-1. The recoveries were 91.15 ~ 106.36% for the analysis of spiked food and water samples without pre-enrichment. Therefore, we believe that the detection platform can be easily and accurately used for S. aureus detection, providing a broad prospect for on-site visual detection.
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Técnicas Biossensoriais , Colorimetria , Ouro/química , Separação Imunomagnética , Nanopartículas Metálicas/química , Staphylococcus aureus/isolamento & purificação , HumanosRESUMO
Covalent organic framework (COF)-decorated magnetic nanoparticles (Fe3O4@DhaTab) with core-shell structure have been synthesized by one-pot method. The prepared Fe3O4@DhaTab was well characterized, and parameters of magnetic solid-phase extraction (MSPE) for parabens were also investigated in detail. Under optimized conditions, the adsorbent dosage was only 3 mg and extraction time was 10 min. The developed Fe3O4@DhaTab-based MSPE-HPLC analysis method offered good linearity (0.01-20 µg mL-1) with R2 (0.999) and low limits of detection (3.3-6.5 µg L-1) using UV detector at 254 nm. The proposed method was applied to determine four parabens in environmental water samples with recoveries in the range 64.0-105% and relative standard deviations of 0.16-7.8%. The adsorption mechanism was explored and indicated that porous DhaTab shell provided π-π, hydrophobic, and hydrogen bonding interactions in the MSPE process. The results revealed the potential of magnetic-functionalized COFs in determination of environmental contaminants.
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Estruturas Metalorgânicas , Cromatografia Líquida de Alta Pressão , Fenômenos Magnéticos , Magnetismo/métodos , Estruturas Metalorgânicas/química , ParabenosRESUMO
A metal electrode modification process for AlGaN-based metal-semiconductor-metal (MSM) photodetectors have been introduced to enhance the response of solar-blind ultraviolet (UV) light detection. The hexadecanethiol organic molecules are chemically adsorbed on the electrodes of high-Al-content Al0.6Ga0.4N MSM solar-blind UV photodetectors, which can reduce the work function of the metal electrode and change the height of the Schottky barrier. This modification process significantly increases the photocurrent and responsivity of the device compared with the referential photodetector without modification. Additionally, the adverse effects caused by the surface state and polarization of the AlGaN materials are effectively reduced, which can be beneficial for improving the electrical performances of III-nitride-based UV photodetectors.