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1.
Nano Lett ; 24(20): 6183-6191, 2024 May 22.
Artigo em Inglês | MEDLINE | ID: mdl-38728596

RESUMO

Two-dimensional (2D) materials are promising candidates for spintronic applications. Maintaining their atomically smooth interfaces during integration of ferromagnetic (FM) electrodes is crucial since conventional metal deposition tends to induce defects at the interfaces. Meanwhile, the difficulties in picking up FM metals with strong adhesion and in achieving conductance match between FM electrodes and spin transport channels make it challenging to fabricate high-quality 2D spintronic devices using metal transfer techniques. Here, we report a solvent-free magnetic electrode transfer technique that employs a graphene layer to assist in the transfer of FM metals. It also serves as part of the FM electrode after transfer for optimizing spin injection, which enables the realization of spin valves with excellent performance based on various 2D materials. In addition to two-terminal devices, we demonstrate that the technique is applicable for four-terminal spin valves with nonlocal geometry. Our results provide a promising future of realizing 2D spintronic applications using the developed magnetic electrode transfer technique.

2.
Small ; 20(26): e2310926, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38239093

RESUMO

Activation of small molecules is considered to be a central concern in the theoretical investigation of environment- and energy-related catalytic conversions. Sub-nanostructured frustrated Lewis pairs (FLPs) have been an emerging research hotspot in recent years due to their advantages in small molecule activation. Although the progress of catalytic applications of FLPs is increasingly reported, the fundamental theories related to the structural formation, site regulation, and catalytic mechanism of FLPs have not yet been fully developed. Given this, it is attempted to demonstrate the underlying theory of FLPs formation, corresponding regulation methods, and its activation mechanism on small molecules using CeO2 as the representative metal oxide. Specifically, this paper presents three fundamental principles for constructing FLPs on CeO2 surfaces, and feasible engineering methods for the regulation of FLPs sites are presented. Furthermore, cases where typical small molecules (e.g., hydrogen, carbon dioxide, methane oxygen, etc.) are activated over FLPs are analyzed. Meanwhile, corresponding future challenges for the development of FLPs-centered theory are presented. The insights presented in this paper may contribute to the theories of FLPs, which can potentially provide inspiration for the development of broader environment- and energy-related catalysis involving small molecule activation.

3.
Chemphyschem ; : e202400335, 2024 May 28.
Artigo em Inglês | MEDLINE | ID: mdl-38807346

RESUMO

Vibrational-mode-selective modulation of electronic excitation is conducted with a synchronized femtosecond (fs) visible (vis) pulse and a picosecond (ps) infrared (IR) pulse. The mechanism of modulation of vibrational and vibronic relaxation behavior of excited state is investigated with ultrafast vis/IR, IR/IR, and vis-IR/IR transient spectroscopy, optical gating experiments and theoretical calculations. An organic molecule, 4'-(N,N-dimethylamino)-3-methoxyflavone (DMA3MHF) is chosen as the model system. Upon 1608 cm-1 excitation, the skeleton stretching vibration of DMA3MHF is energized, which can significantly change the shape of the absorption, facilitate the radiative decay and promote emission from vibrational excited states. As results, a remarkable enhancement and a slight blueshift in fluorescence are observed. The mode-selective modulation of electronic excitation is not limited in luminescence or photophysics. It is expected to be widely applicable in tuning many photochemical processes.

4.
Langmuir ; 40(20): 10776-10791, 2024 May 21.
Artigo em Inglês | MEDLINE | ID: mdl-38728176

RESUMO

Fractured reservoirs are an important source of oil and gas energy. After depletion of production, the production capacity of this reservoir decreases rapidly. Effective profile control is needed to improve the sweep efficiency and reservoir heterogeneity. Foam can solve such problems, but its profile control mechanism is not fully understood. Based on this, this paper uses the level set method to study the microscale control mechanism of foam in fractured media. The results show that artificial fractures and high-permeability microfractures are tighter than natural fractures, the Jamin effect of foam is stronger, and the secondary foaming ability is better. Therefore, the plugging ability of foam to natural fractures is far less than that of foam to artificial fractures and high-permeability microfractures. The larger the fracture opening, the larger the foam volume and the smaller the flow rate. As the opening ratio increases gradually, the generated foam flows more to the natural fractures with a large opening, and the effect of foam blocking large fractures becomes worse. The diversion rate curves of different opening ratios show that the foam has a good profile control effect when the opening ratios are 4:1 and 2:1, and even the diversion rate overturns, while the profile control diversion effect is poor when the opening ratio is 10:1, so it cannot play an effective role in profile control. The foam shows the profile control process of preferentially plugging the high-permeability area and allowing more subsequent fluids to enter the low-permeability area. The research reveals the profile control mechanism of foam on fractured reservoirs from the micro level, which is the supplement and verification of relevant macro research and provides a theoretical basis for the efficient development of fractured reservoirs.

5.
J Phys Chem A ; 128(15): 2912-2922, 2024 Apr 18.
Artigo em Inglês | MEDLINE | ID: mdl-38572812

RESUMO

Mode-selective vibrational excitations to modify the electronic states of fluorescein dianion in methanol solutions are carried out with a femtosecond visible pulse synchronized with a tunable high-power, narrow-band picosecond infrared (IR) pulse. In this work, simultaneous intensity enhancement, peak blueshift, and line width broadening of fluorescence are observed in the visible/IR double resonance experiments. Comprehensive investigations on the modulation mechanism with scanning the vibrational excitation frequencies, tuning the time delay between the two excitation pulses, theoretical calculations, and nonlinear and linear spectroscopic measurements suggest that the fluorescence intensity enhancement is caused by the increase of the Franck-Condon factor induced by the vibrational excitations at the electronic ground state. Various enhancement effects are observed as vibrations initially excited by the IR photons relax to populate the vibrational modes of lower frequencies. The peak blueshift and line width broadening are caused by both increasing the Franck-Condon factors among different subensembles because of IR pre-excitation and the long-lived processes induced by the initial IR excitation. The results demonstrate that the fluorescence from the visible/IR double resonance experiments is not a simple sum frequency effect, and vibrational relaxations can produce profound effects modifying luminescence.

6.
Sheng Wu Yi Xue Gong Cheng Xue Za Zhi ; 41(2): 342-350, 2024 Apr 25.
Artigo em Chinês | MEDLINE | ID: mdl-38686416

RESUMO

Temporal interference (TI) as a new neuromodulation technique can be applied to non-invasive deep brain stimulation. In order to verify its effectiveness in the regulation of motor behavior in animals, this paper uses the TI method to focus the envelope electric field to the ventral posterior lateral nucleus (VPL) of the thalamus in the deep brain of mouse to regulate left- and right-turning motor behavior. The focusability of TI in the mouse VPL was analyzed by finite element method, and the focus area and volume were obtained by numerical calculation. A stimulator was used to generate TI current to stimulate the mouse VPL to verify the effectiveness of the TI stimulation method, and the accuracy of the focus location was further determined by c-Fos immunofluorescence experiments. The results showed that the electric field generated by TI stimulation was able to focus on the VPL nuclei when the stimulation current reached 800 µA; the mouse were able to make corresponding left and right turns according to the stimulation position; and the c-Fos positive cell markers in the VPL nuclei increased significantly after stimulation. This study confirms the feasibility of TI in regulating animal motor behavior and provides a non-invasive stimulation method for brain tissue for animal robots.


Assuntos
Estimulação Encefálica Profunda , Atividade Motora , Proteínas Proto-Oncogênicas c-fos , Animais , Camundongos , Estimulação Encefálica Profunda/métodos , Atividade Motora/fisiologia , Proteínas Proto-Oncogênicas c-fos/metabolismo , Comportamento Animal , Núcleos Ventrais do Tálamo/fisiologia , Análise de Elementos Finitos
7.
Angew Chem Int Ed Engl ; 63(13): e202318030, 2024 Mar 22.
Artigo em Inglês | MEDLINE | ID: mdl-38308534

RESUMO

The specific states of aggregation of metal atoms in sub-nanometer-sized gold clusters are related to the different quantum confinement volumes of electrons, leading to novel optical and electronic properties. These volumes can be tuned by changing the relative positions of the gold atoms to generate isomers. Studying the isomeric gold core and the electron coupling between the basic units is fundamentally important for nanoelectronic devices and luminescence; however, appropriate cases are lacking. In this study, the structure of the first staggered di-superatomic Au25 -S was solved using single-crystal X-ray diffraction. The optical properties of Au25 -S were studied by comparing with eclipsed Au25 -E. From Au25 -E to Au25 -S, changes in the electronic structures occurred, resulting in significantly different optical absorptions originating from the coupling between the two Au13 modules. Au25 -S shows a longer electron decay lifetime of 307.7 ps before populating the lowest triplet emissive state, compared to 1.29 ps for Au25 -E. The experimental and theoretical results show that variations in the geometric isomerism lead to distinct photophysical processes owing to isomerism-dependent electronic coupling. This study offers new insights into the connection between the geometric isomerism of nanosized building blocks and the optical properties of their assemblies, opening new possibilities for constructing function-specific nanomaterials.

8.
SSM Popul Health ; 25: 101584, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38125277

RESUMO

Background: This study focuses on the heterogeneity, interaction, and imbalance in the concurrent development of physical and mental health trajectories among Chinese elderly. Methods: The data used in this study are from four waves of the China Health and Retirement Longitudinal Study (CHRLS) conducted between 2011 and 2018. A multidimensional growth mixture model (MGMM) was employed to analyze the patterns and characteristics of co-occurring physical and mental health development. Additionally, multinomial logistic regression analysis was conducted to systematically investigate the factors that predict the conjoint trajectories of physical and mental health. Results: The study findings reveal the presence of four distinct latent classes of conjoint trajectories for physical and mental health. These classes are categorized as follows: 'physical and mental health deteriorating', 'physical disease increasing & low mental vulnerability maintaining', 'low physical & mental vulnerability maintaining', and 'high physical disease increased & mental health moderate-stable'. Furthermore, demographic characteristics, socioeconomic status, family-society relations, health behaviors, and institutional factors were found to significantly predict these latent classes. Conclusion: The study emphasizes the diversity and complexity of physical and mental co-occurring developmental health issues in the elderly population in China. These findings have significant implications for the development of targeted intervention strategies that take into account the unique health changes experienced by older adults. Additionally, they can serve as evidence for the establishment of a comprehensive long-term care system.

10.
Trop Med Infect Dis ; 9(2)2024 Feb 04.
Artigo em Inglês | MEDLINE | ID: mdl-38393131

RESUMO

We established a mouse model of Schistosoma japonicum infection in order to study the effects of the infection on hepatocyte autophagy and apoptosis. We also stimulated HepG2 cells with soluble egg antigens (SEA) in vitro. At two, four, and six weeks post-infection, quantitative real-time PCR and Western blot (WB) were used to detect liver expression levels of autophagy and apoptosis-related proteins. HepG2 cells were treated with different concentrations of SEA. The changes in the levels of autophagy-related proteins and HepG2 cell apoptosis were detected. The Lc3b, Beclin1, Atg7, and Atg12 mRNA levels were significantly lower at four and six weeks after infection than those in the uninfected group. At four and six weeks following infection, the levels of Beclin1, LC3BII/I, Atg7, and p62 proteins were considerably lower than those in the uninfected group. The protein levels of pro-apoptotic Bax and cleaved caspase 3 and fibrosis-related proteins α-SMA and collagen 3 in the liver post-infection were significantly higher than those in uninfected mice. HepG2 cells stimulated with SEA showed decreased levels of Beclin1, p62, and Atg7 proteins and significantly increased apoptosis rates. The findings demonstrated that following infection with S. japonicum, mice's liver fibrosis worsened, hepatic autophagy was suppressed, and hepatocyte apoptosis was encouraged.

11.
ChemSusChem ; 17(10): e202301687, 2024 May 21.
Artigo em Inglês | MEDLINE | ID: mdl-38221143

RESUMO

Developing inexpensive and efficient catalysts for biomass hydrogenation or hydrodeoxygenation (HDO) is essential for efficient energy conversion. Transition metal phosphides (TMPs), with the merits of abundant active sites, unique physicochemical properties, tunable component structures, and excellent catalytic activities, are recognized as promising biomass hydrogenation or HDO catalytic materials. Nevertheless, the biomass hydrogenation or HDO catalytic applications of TMPs are still limited by various complexities and inherent performance bottlenecks, and thus their future development and utilization remain to be systematically sorted out and further explored. This review summarizes the current popular strategies for the preparation of TMPs. Subsequently, based on the structural and electronic properties of TMPs, the catalytic activity origins of TMPs in biomass hydrogenation or HDO is elucidated. Additionally, the application of TMPs in efficient biomass hydrogenation or HDO catalysis, as well as highly targeted multiscale strategies to enhance the catalytic performance of TMPs, are comprehensively described. Finally, large-scale amplification synthesis, rational construction of TMP-based catalysts and in-depth study of the catalytic mechanism are also mentioned as challenges and future directions in this research field. Expectedly, this review can provide professional and targeted guidance for the rational design and practical application of TMPs biomass hydrogenation or HDO catalysts.

12.
J Chromatogr A ; 1715: 464601, 2024 Jan 25.
Artigo em Inglês | MEDLINE | ID: mdl-38160583

RESUMO

In the present work, parallel reaction monitoring (PRM) and data-independent acquisition (DIA) methods were developed for the accurate quantitation of amino acids, alkaloids nucleosides and nucleotides in tea. The quality peaks were significantly enhanced by optimizing the LC elution procedure, HCD voltage, MS resolution, and scanning event. Both methods were validated with good liner linearity (0.004-200 µg/mL), LODs (0.001-0.309 µg/mL for PRM and 0.001-0.564 µg/mL for DIA). Applied to white tea sample, the contents of these hydrophilic compounds were range from 34,655.39 to 70,586.14 mg/kg, and caffeine (32,529.02 mg/kg) and theanine (5483.46 mg/kg) were determined as the most abundant ones. Based on the quantitation data set, the white tea samples from Puer, Lincang and Xishuangbanna were clearly discriminated using multivariate data analysis. The results of the present works show that PRM and DIA have great potential in quantitative analysis of multiple hydrophilic compounds in food samples.


Assuntos
Alcaloides , Cafeína , Nucleosídeos , Nucleotídeos , Chá/química
13.
J Colloid Interface Sci ; 659: 799-810, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38218084

RESUMO

The catalytic activity improvement of Fe-based active sites derived from metal organic frameworks toward oxygen reduction reaction (ORR) and methanol oxidation reaction (MOR) remains a major challenge. In this study, the growth of strontium decorated 2-methylimidazole zinc salt (Sr/ZIF-8) is prepared as a carrier to vapor deposited iron formation Sr doped Fe-based nitrogen-doped carbon framework (named as Sr/FeNC). After high-temperature pyrolysis and vapor deposition, strontium carbonate nanocrystals are evenly dispersed on the shrunk dodecahedron carbon frame and multitudinous Fe-based active catalytic sites are embedded in carbon skeleton. The optimal Sr/FeNC-2 catalyst demonstrates the outstanding ORR performance in terms of a half-wave potential of 0.851 V and an onset potential of 0.90 V, while Sr/FeNC-2 exhibits a high current density of 18.2 mA cm-2 and a lower Tafel slope of 21 mV dec-1 in MOR. The exceptional catalytic activity could be ascribed to the synergistic coupling effect of strontium compounds with Fe-based catalytic sites (Fe-Nx, Fe, and iron oxide). In particular, the formation of SrCO3 affects the bonding configuration of the iron species sites, leading to an optimization of the electronic structure within the multihole carbon matrix. The synthetic approach presents a prospective strategy for future endeavors in developing innovative and advanced bifunctional catalysts for ORR and MOR.

14.
Nanomaterials (Basel) ; 14(14)2024 Jul 12.
Artigo em Inglês | MEDLINE | ID: mdl-39057872

RESUMO

Brain-inspired flexible neuromorphic devices are of great significance for next-generation high-efficiency wearable sensing and computing systems. In this paper, we propose a flexible organic electrochemical transistor using poly[(bithiophene)-alternate-(2,5-di(2-octyldodecyl)- 3,6-di(thienyl)-pyrrolyl pyrrolidone)] (DPPT-TT) as the organic semiconductor and poly(methyl methacrylate) (PMMA)/LiClO4 solid-state electrolyte as the gate dielectric layer. Under gate voltage modulation, an electric double layer (EDL) forms between the dielectric layer and the channel, allowing the device to operate at low voltages. Furthermore, by leveraging the double layer effect and electrochemical doping within the device, we successfully mimic various synaptic behaviors, including excitatory post-synaptic currents (EPSC), paired-pulse facilitation (PPF), high-pass filtering characteristics, transitions from short-term plasticity (STP) to long-term plasticity (LTP), and demonstrate its image recognition and storage capabilities in a 3 × 3 array. Importantly, the device's electrical performance remains stable even after bending, achieving ultra-low-power consumption of 2.08 fJ per synaptic event at -0.001 V. This research may contribute to the development of ultra-low-power neuromorphic computing, biomimetic robotics, and artificial intelligence.

15.
Patterns (N Y) ; 4(12): 100892, 2023 Dec 08.
Artigo em Inglês | MEDLINE | ID: mdl-38106617

RESUMO

The study aims to develop AICare, an interpretable mortality prediction model, using electronic medical records (EMR) from follow-up visits for end-stage renal disease (ESRD) patients. AICare includes a multichannel feature extraction module and an adaptive feature importance recalibration module. It integrates dynamic records and static features to perform personalized health context representation learning. The dataset encompasses 13,091 visits and demographic data of 656 peritoneal dialysis (PD) patients spanning 12 years. An additional public dataset of 4,789 visits from 1,363 hemodialysis (HD) patients is also considered. AICare outperforms traditional deep learning models in mortality prediction while retaining interpretability. It uncovers mortality-feature relationships and variations in feature importance and provides reference values. An AI-doctor interaction system is developed for visualizing patients' health trajectories and risk indicators.

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