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1.
Nano Lett ; 24(11): 3507-3514, 2024 Mar 20.
Artículo en Inglés | MEDLINE | ID: mdl-38445582

RESUMEN

Layertronics, rooted in the layer Hall effect (LHE), is an emerging fundamental phenomenon in condensed matter physics and spintronics. So far, several theoretical and experimental proposals have been made to realize LHE, but all are based on antiferromagnetic systems. Here, using symmetry and tight-binding model analysis, we propose a general mechanism for engineering layertronics in a two-dimensional ferromagnetic multiferroic lattice. The physics is related to the band geometric properties and multiferroicity, which results in the coupling between Berry curvature and layer degree of freedom, thereby generating the LHE. Using first-principles calculations, we further demonstrate this mechanism in bilayer (BL) TcIrGe2S6. Due to the intrinsic inversion and time-reversal symmetry breakings, BL TcIrGe2S6 exhibits multiferroicity with large Berry curvatures at both the center and corners of the Brillouin zone. These Berry curvatures couple with the layer physics, forming the LHE in BL TcIrGe2S6. Our work opens a new direction for research on layertronics.

2.
Nano Lett ; 24(34): 10490-10495, 2024 Aug 28.
Artículo en Inglés | MEDLINE | ID: mdl-39150250

RESUMEN

Engineering the valley index is essential and highly sought for valley physics, but currently, it is exclusively based on the paradigm of the challenging ferrovalley with spin-orientation reversal under a magnetic field. Here, an alternative strategy, i.e., the so-called ferroelectrovalley, is proposed to tackle the insurmountable spin-orientation reversal, which reverses the valley index with the feasible ferroelectricity. Using symmetry arguments and the tight-binding model, the C2z rotation is unveiled to be able to take the place of time reversal for operating the valley index in two-dimensional multiferroic kagome lattices, which enables a ferroelectricity-engineered valley index, thereby generating the concept of a ferroelectrovalley. Based on first-principles calculations, this concept is further demonstrated in the breathing kagome lattice of single-layer Ti3Br8, wherein ferroelectricity couples with the breathing process. These findings open a new direction for valleytronics and 2D materials research.

3.
Nano Lett ; 24(3): 1009-1014, 2024 Jan 24.
Artículo en Inglés | MEDLINE | ID: mdl-38214894

RESUMEN

In the field of physics and materials science, the discovery of the layer-polarized anomalous Hall effect (LP-AHE) stands as a crucial development. The current research paradigm is rooted in topological or inversion-asymmetric valleytronic systems, making such a phenomenon rather rare. In this work, a universal design principle for achieving the LP-AHE from inversion-symmetric single-layer lattices is proposed. Through tight-binding model analysis, we demonstrate that by stacking into antiferromagnetic van der Waals bilayer lattices, the coupling physics between PT symmetry and vertical external bias can be realized. This coupling reveals the previously neutralized layer-locked Berry curvature, compelling the carriers to move in a specific direction within a given layer, thereby realizing the LP-AHE. Intriguingly, the chirality of the LP-AHE can be effectively switched by modulating the direction of vertical external bias. First-principles calculations validate this mechanism in bilayer T-FeCl2 and MnPSe3. Our results pave the way for new explorations of the LP-AHE.

4.
Nano Lett ; 24(1): 450-457, 2024 Jan 10.
Artículo en Inglés | MEDLINE | ID: mdl-38112315

RESUMEN

We put forward that stacked Chern insulators with opposite chiralities offer a strategy to achieve gapless helical edge states in two dimensions. We employ the square lattice as an example and elucidate that the gapless chiral and helical edge states emerge in the monolayer and antiferromagnetically stacked bilayer, characterized by Chern number C=-1 and spin Chern number CS=-1, respectively. Particularly, for a topological phase transition to the normal insulator in the stacked bilayer, a band gap closing and reopening procedure takes place accompanied by helical edge states disappearing, where the Chern insulating phase in the monolayer vanishes at the same time. Moreover, EuO is revealed as a suitable candidate for material realization. This work is not only valuable to the research of the quantum anomalous Hall effect but also offers a favorable platform to realize magnetic topologically insulating materials for spintronics applications.

5.
Nano Lett ; 2024 Apr 15.
Artículo en Inglés | MEDLINE | ID: mdl-38619844

RESUMEN

Recent advances in the manipulation of the orbital angular momentum (OAM) within the paradigm of orbitronics presents a promising avenue for the design of future electronic devices. In this context, the recently observed orbital Hall effect (OHE) occupies a special place. Here, focusing on both the second-order topological and quantum anomalous Hall insulators in two-dimensional ferromagnets, we demonstrate that topological phase transitions present an efficient and straightforward way to engineer the OHE, where the OAM distribution can be controlled by the nature of the band inversion. Using first-principles calculations, we identify Janus RuBrCl and three septuple layers of MnBi2Te4 as experimentally feasible examples of the proposed mechanism of OHE engineering by topology. With our work, we open up new possibilities for innovative applications in topological spintronics and orbitronics.

6.
Small ; 20(22): e2309256, 2024 May.
Artículo en Inglés | MEDLINE | ID: mdl-38133479

RESUMEN

Although 2D π-d conjugated metal-organic frameworks (MOFs) exhibit high in-plane conductivity, the closely stacked layers result in low specific surface area and difficulty in mass transfer and diffusion. Hence, a conductive 3D MOF Fe3(HITP)2/bpm@Co (HITP = 2,3,6,7,10,11-hexaiminotriphenylene) is reported through inserting bpm (4,4'-bipyrimidine) ligands and Co2+ into the interlayers of 2D MOF Fe3(HITP)2. Compared to 2D Fe3(HITP)2 (37.23 m2 g-1), 3D Fe3(HITP)2/bpm@Co displays a huge improvement in the specific surface area (373.82 m2 g-1). Furthermore, the combined experimental and density functional theory (DFT) theoretical calculations demonstrate the metallic behavior of Fe3(HITP)2/bpm@Co, which will benefit to the electrocatalytic activity of it. Impressively, Fe3(HITP)2/bpm@Co exhibits prominent and stable oxygen evolution reaction (OER) performance (an overpotential of 299 mV vs RHE at a current density of 10 mA cm-2 and a Tafel slope of 37.14 mV dec-1), which is superior to 2D Fe3(HITP)2 and comparable to commercial IrO2. DFT theoretical calculation reveals that the combined action of the Fe and Co sites in Fe3(HITP)2/bpm@Co is responsible for the enhanced electrocatalytic activity. This work provides an alternative approach to develop conductive 3D MOFs as efficient electrocatalysts.

7.
Hepatology ; 78(1): 72-87, 2023 07 01.
Artículo en Inglés | MEDLINE | ID: mdl-36626624

RESUMEN

BACKGROUND AND AIMS: The innate-like mucosa-associated invariant T (MAIT) cells are enriched in human liver and have been linked to human HCC. However, their contributions to the progression of HCC are controversial due to the heterogeneity of MAIT cells, and new MAIT cell subsets remain to be explored. APPROACH AND RESULTS: Combining single cell RNA sequencing (scRNA-seq) and flow cytometry analysis, we performed phenotypic and functional studies and found that FOXP3 + CXCR3 + MAIT cells in HCC patients were regulatory MAIT cells (MAITregs) with high immunosuppressive potential. These MAITregs were induced under Treg-inducing condition and predominantly from FOXP3 - CXCR3 + MAIT cells, which displayed mild Treg-related features and represented a pre-MAITreg reservoir. In addition, the induction and function of MAITregs were promoted by ß1 adrenergic receptor signaling in pre-MAITregs and MAITregs, respectively. In HCC patients, high proportion of the intratumoral MAITregs inhibited antitumor immune responses and was associated with poor clinical outcomes. CONCLUSIONS: Together, we reveal an immunosuppressive subset of MAIT cells in HCC patients that contributes to HCC progression, and propose a control through neuroimmune crosstalk.


Asunto(s)
Carcinoma Hepatocelular , Neoplasias Hepáticas , Células T Invariantes Asociadas a Mucosa , Humanos , Carcinoma Hepatocelular/patología , Neoplasias Hepáticas/patología , Membrana Mucosa , Factores de Transcripción Forkhead , Receptores Adrenérgicos
8.
Chemistry ; : e202401380, 2024 Jul 10.
Artículo en Inglés | MEDLINE | ID: mdl-38987889

RESUMEN

Photocatalytic ozonation is considered to be a promising approach for the treatment of refractory organic pollutants, but the design of efficient catalyst remains a challenge. Surface modification provides a potential strategy to improve the activity of photocatalytic ozonation. In this work, density functional theory (DFT) calculations were first performed to check the interaction between O3 and TiO2-OH (surface hydroxylated TiO2) or TiO2-F (surface fluorinated TiO2), and the results suggest that TiO2-OH displays better O3 adsorption and activation than does TiO2-F, which is confirmed by experimental results. The surface hydroxyl groups greatly promote the O3 activation, which is beneficial for the generation of reactive oxygen species (ROS). Importantly, TiO2-OH displays better performance towards pollutants (such as berberine hydrochloride) removal than does TiO2-F and most reported ozonation photocatalysts. The total organic carbon (TOC) removal efficiency reaches 84.4 % within two hours. This work highlights the effect of surface hydroxylation on photocatalytic ozonation and provides ideas for the design of efficient photocatalytic ozonation catalysts.

9.
Eur J Neurol ; : e16458, 2024 Sep 10.
Artículo en Inglés | MEDLINE | ID: mdl-39254065

RESUMEN

BACKGROUND AND PURPOSE: The benefit of remote ischaemic conditioning (RIC) in acute moderate ischaemic stroke has been demonstrated by the Remote Ischaemic Conditioning for Acute Moderate Ischaemic Stroke (RICAMIS) study. This prespecified exploratory analysis aimed to determine whether there was a difference of RIC efficacy in anterior versus posterior circulation stroke based on RICAMIS data. METHODS: In this analysis, eligible patients presenting within 48 h of stroke onset were divided into two groups: anterior circulation stroke (ACS) and posterior circulation stroke (PCS) groups. The primary endpoint was an excellent functional outcome, defined as a modified Rankin Scale (mRS) score 0-1 at 90 days. RESULTS: In all, 1013 patients were included in the final analysis, including 642 with ACS and 371 with PCS. Compared with the control group, RIC was significantly associated with an increased proportion of mRS scores 0-1 within 90 days in the PCS group (unadjusted odds ratio 1.6, 95% confidence interval 1.0-2.4, p = 0.04; adjusted odds ratio 2.0, 95% confidence interval 1.2-3.3, p = 0.005), but not in the ACS group (p = 0.29). Similar results were found regarding secondary outcomes including mRS score 0-2 at 90 days, mRS distribution at 90 days and change in National Institutes of Health Stroke Scale score at day 12 from baseline. However, there was no significant interaction effect between stroke location and intervention on the primary outcome (pinteraction = 0.21). CONCLUSION: Amongst patients with acute PCS who are not candidates for reperfusion treatment, RIC may be associated with a higher probability of improved functional outcomes. These findings need to be validated in prospective trials.

10.
Br J Clin Pharmacol ; 90(2): 452-462, 2024 02.
Artículo en Inglés | MEDLINE | ID: mdl-37749762

RESUMEN

AIMS: This study aims to establish a population pharmacokinetic (PK) model of teicoplanin in Chinese adult patients to evaluate the dosing regimen in the label sheet and optimize it. METHODS: Nonlinear mixed-effects modelling was used to estimate PK parameters. Monte Carlo simulations were used to evaluate the attainment of various dosing regimens in achieving the target trough concentrations in patients with normal or decreased renal function. RESULTS: A total of 115 patients were enrolled in this retrospective study. Creatinine clearance (CrCL) and albumin (ALB) were identified as covariates on the clearance of teicoplanin. For the treatment of non-complicated methicillin-resistant Staphylococcus aureus (MRSA) infections in patients with normal renal function and serum ALB concentration, the recommended dosing regimen was 600 mg q12h with five administrations as the loading dose followed by 600 mg qd as the maintenance dose; for the treatment of serious and/or complicated MRSA infections, the recommended dosing regimen was 800 mg q12h with five administrations as the loading dose followed by 800 mg qd as the maintenance dose. It is worth noting that both the loading and maintenance doses ought to be modified based on the patient's renal function and serum ALB concentration. In addition, trough concentrations of teicoplanin were significantly increased every other week. CONCLUSIONS: Both loading dosing and maintenance dosing regimens were recommended to be adjusted according to patient's renal function and serum ALB concentration. In addition, it is necessary to perform follow-up therapeutic drug monitoring of teicoplanin at least once every week.


Asunto(s)
Staphylococcus aureus Resistente a Meticilina , Infecciones Estafilocócicas , Adulto , Humanos , Teicoplanina/uso terapéutico , Antibacterianos , Estudios Retrospectivos , Monitoreo de Drogas , Albúmina Sérica , Infecciones Estafilocócicas/tratamiento farmacológico
11.
BMC Psychiatry ; 24(1): 514, 2024 Jul 19.
Artículo en Inglés | MEDLINE | ID: mdl-39030516

RESUMEN

BACKGROUND: In this prospective cohort study, we determined the phenotypic characteristics of children with regressive autism spectrum disorder (ASD) and explored the effects of rehabilitation. METHODS: We recruited 370 children with ASD aged 1.5-7 years. Based on the Regression Supplement Form, the children were assigned to two groups: regressive and non-regressive. The core symptoms and neurodevelopmental levels of ASD were assessed before and after 1 year of behavioral intervention using the Autism Diagnostic Observation Schedule (ADOS), Social Response Scale (SRS), Children Autism Rating Scale (CARS), and Gesell Developmental Scale (GDS). RESULTS: Among the 370 children with ASD, 28.38% (105/370) experienced regression. Regression was primarily observed in social communication and language skills. Children with regressive ASD exhibited higher SRS and CARS scores and lower GDS scores than those with non-regressive ASD. After 1 year of behavioral intervention, the symptom scale scores significantly decreased for all children with ASD; however, a lesser degree of improvement was observed in children with regressive ASD than in those with non-regressive ASD. In addition, the symptom scores of children with regressive ASD below 4 years old significantly decreased, whereas the scores of those over 4 years old did not significantly improve. Children with regressive ASD showed higher core symptom scores and lower neurodevelopmental levels. Nevertheless, after behavioral intervention, some symptoms exhibited significant improvements in children with regressive ASD under 4 years of age. CONCLUSION: Early intervention should be considered for children with ASD, particularly for those with regressive ASD.


Asunto(s)
Trastorno del Espectro Autista , Fenotipo , Humanos , Trastorno del Espectro Autista/rehabilitación , Trastorno del Espectro Autista/complicaciones , Preescolar , Masculino , Femenino , Niño , Estudios Prospectivos , Lactante , Terapia Conductista/métodos
12.
BMC Womens Health ; 24(1): 38, 2024 01 13.
Artículo en Inglés | MEDLINE | ID: mdl-38218823

RESUMEN

BACKGROUND: Immune checkpoint inhibitors (ICIs) can improve survivals of metastatic triple negative breast cancer (mTNBC); however, we still seek circulating blood biomarkers to predict the efficacy of ICIs. MATERIALS AND METHODS: In this study, we analyzed the data of ICIs treated mTNBC collected in Anhui Medical University affiliated hospitals from 2018 to 2023. The counts of lymphocytes, monocytes, platelets, and ratio indexes (NLR, MLR, PLR) in peripheral blood were investigated via the Kaplan-Meier curves and the Cox proportional-hazards model. RESULTS: The total of 50 mTNBC patients were treated with ICIs. High level of peripheral lymphocytes and low level of NLR and MLR at baseline and post the first cycle of ICIs play the predictable role of immunotherapies. Lymphocytes counts (HR = 0.280; 95% CI: 0.095-0.823; p = 0.021) and NLR (HR = 1.150; 95% CI: 1.052-1.257; p = 0.002) are significantly correlated with overall survival. High NLR also increases the risk of disease progression (HR = 2.189; 95% CI:1.085-4.414; p = 0.029). When NLR at baseline ≥ 2.75, the hazard of death (HR = 2.575; 95% CI:1.217-5.447; p = 0.013) and disease progression (HR = 2.189; 95% CI: 1.085-4.414; p = 0.029) significantly rise. HER-2 expression and anti-tumor therapy lines are statistically correlated with survivals. CONCLUSIONS: Before the initiation of ICIs, enriched peripheral lymphocytes and poor neutrophils and NLR contribute to the prediction of survivals.


Asunto(s)
Neoplasias de la Mama Triple Negativas , Humanos , Neoplasias de la Mama Triple Negativas/tratamiento farmacológico , Pronóstico , Biomarcadores , Linfocitos/patología , Progresión de la Enfermedad , Estudios Retrospectivos , Biomarcadores de Tumor
13.
Artículo en Inglés | MEDLINE | ID: mdl-39277560

RESUMEN

PURPOSE: Childhood lead exposure is linked to poorer neurobehavioral function in adolescence, but the relationship between lead and adolescent sleep health remains inconsistent. This study aimed to investigate concurrent and longitudinal associations between lead exposure and multiple sleep health domains in adolescents. METHODS: A total of 972 adolescents from China Jintan Child Cohort were included in analyses. The Blood lead levels (BLLs) were assessed in two Waves, at ages 3-5 years (mean 6.50 ± 2.76 µg/dL) and 11-13 years (mean 3.12 ± 1.17 µg/dL). Sleep problems at age 11-13 were parent-reported via the Child Sleep Health Questionnaire (CSHQ) and self-reported by adolescents using the Pittsburgh Sleep Quality Index (PSQI). RESULTS: Both early and later BLLs were associated positively with parental reported sleep problems, including sleep onset delay, night waking, short duration, parasomnias, and disordered breathing. Sex-stratified analyzes showed that most adjusted associations between two-Wave BLLs and sleep outcomes (CSHQ and PSQI) remained statistically significant in males, with a minor increase in the magnitude of these associations. The association between Wave II BLLs and shorter self-reported sleep duration was only statistically significant in female adolescents. Compared to children with consistently low BLLs at both ages, those with persistently high BLLs at both ages had significantly shorter parental-reported sleep duration and worse sleep onset delay. CONCLUSION: Findings suggest that both early and later childhood lead exposures link to more adolescent sleep problems, with recent BLLs showing stronger associations with poor adolescent sleep health reported by their parents.

14.
Nano Lett ; 23(1): 91-97, 2023 Jan 11.
Artículo en Inglés | MEDLINE | ID: mdl-36326600

RESUMEN

Magnetic topological states have attracted great attention that provide exciting platforms for exploring prominent physical phenomena and applications of topological spintronics. Here, using a tight-binding model and first-principles calculations, we put forward that, in contrast to previously reported magnetic second-order topological insulators (SOTIs), robust SOTIs can emerge in two-dimensional ferromagnets regardless of magnetization directions. Remarkably, we identify intrinsic ferromagnetic 2H-RuCl2 and Janus VSSe monolayers as experimentally feasible candidates of predicted robust SOTIs with the emergence of nontrivial corner states along different magnetization directions. Moreover, under out-of-plane magnetization, we unexpectedly point out that the valley polarization of SOTIs can be huge and much larger than that of the known ferrovalley materials, opening up a technological avenue to bridge the valleytronics and higher-order topology with high possibility of innovative applications in topological spintronics and valleytronics.

15.
Nano Lett ; 23(1): 312-318, 2023 Jan 11.
Artículo en Inglés | MEDLINE | ID: mdl-36576995

RESUMEN

Topological magnetism in low-dimensional systems is of fundamental and practical importance in condensed-matter physics and material science. Here, using first-principles and Monte Carlo simulations, we present that multiple topological magnetism (i.e., skyrmion and bimeron) can survive in van der Waals heterostructure MnTe2/ZrS2. Arising from interlayer coupling, MnTe2/ZrS2 can harbor a large Dzyaloshinskii-Moriya interaction. This, combined with exchange interaction, yields an intriguing skyrmion phase under a tiny magnetic field of 75 mT. Meanwhile, upon harnessing a small electric field, magnetic bimeron can be observed in MnTe2/ZrS2, suggesting the existence of multiple topological magnetism. Through interlayer sliding, both topological magnetisms can be switched on-off. In addition, the impacts of d∥ and Keff on these spin textures are revealed, and a dimensionless parameter κ is utilized to describe their joint effect. These explored phenomena and insights not only are useful for fundamental research in topological magnetism but also enable novel applications in nanodevices.

16.
Nano Lett ; 23(11): 5367-5372, 2023 Jun 14.
Artículo en Inglés | MEDLINE | ID: mdl-37232533

RESUMEN

The layer Hall effect (LHE) is of fundamental and practical importance in condensed-matter physics and material science; however, it was rarely observed and usually based on the paradigms of persistent electric field and sliding ferroelectricity. Here, a new mechanism of LHE is proposed by coupling layer physics with multiferroics using symmetry analysis and a low-energy k·p model. Due to time-reversal symmetry breaking and valley physics, the Bloch electrons on one valley will be subject to a large Berry curvature. This combined with inversion symmetry breaking gives rise to layer-polarized Berry curvature and can force the electrons to deflect in one direction of a given layer, thereby generating the LHE. We demonstrate that the resulting LHE is ferroelectrically controllable and reversible. Using first-principles calculations, this mechanism and predicted phenomena are verified in the multiferroic material of bilayer Co2CF2. Our finding opens a new direction for LHE and 2D materials research.

17.
Nano Lett ; 23(4): 1244-1251, 2023 Feb 22.
Artículo en Inglés | MEDLINE | ID: mdl-36757119

RESUMEN

Oxygen vacancies (OVs) on specific sites/facets can strengthen the interaction between reactants and oxide surfaces, facilitating interfacial charge transfer. However, precise monitoring of the spatial distribution of OVs remains a grand challenge. We report here that a single-particle spectroscopy technique addresses this challenge by establishing a positive correlation relationship between defects and bound exciton luminescence across different facets. Taking monoclinic BiVO4 as an example, on the basis of theoretical guidance, by in situ tracking the PL lifetimes and PL spectra of different facets on single particles before and after hydrogen treatment, we provide evidence that the PL emission originates from the OV state and determine that OVs is more inclined to be generated at the {010} facets. This anisotropic defect engineering significantly prolongs the lifetime of carriers and accelerates the activation of molecular oxygen. These findings not only verify preference rules of OVs in metal oxides but also provide a time-space-resolved monitoring method.

18.
Zhongguo Zhong Yao Za Zhi ; 49(9): 2376-2384, 2024 May.
Artículo en Zh | MEDLINE | ID: mdl-38812138

RESUMEN

The abnormal activation of the mammalian target of rapamycin(mTOR) signaling pathway in non-small cell lung cancer(NSCLC) is closely associated with distant metastasis, drug resistance, tumor immune escape, and low overall survival. The present study reported that betulinic acid(BA), a potent inhibitor of mTOR signaling pathway, exhibited an inhibitory activity against NSCLC in vitro and in vivo. CCK-8 and colony formation results demonstrated that BA significantly inhibited the viability and clonogenic ability of H1299, A549, and LLC cells. Additionally, the treatment with BA induced mitochondrion-mediated apoptosis of H1299 and LLC cells. Furthermore, BA inhibited the mobility and invasion of H1299 and LLC cells by down-regulating the expression level of matrix metalloproteinase 2(MMP2) and impairing epithelial-mesenchymal transition. The results demonstrated that the inhibition of mTOR signaling pathway by BA decreased the proportion of M2 phenotype(CD206 positive) cells in total macrophages. Furthermore, a mouse model of subcutaneous tumor was established with LLC cells to evaluate the anti-tumor efficiency of BA in vivo. The results revealed that the administration of BA dramatically retarded the tumor growth and inhibited the proliferation of tumor cells. More importantly, BA increased the ratio of M1/M2 macrophages in the tumor tissue, which implied the enhancement of anti-tumor immunity. In conclusion, BA demonstrated the inhibitory effect on NSCLC by repolarizing tumor-associated macrophages via the mTOR signaling pathway.


Asunto(s)
Ácido Betulínico , Carcinoma de Pulmón de Células no Pequeñas , Neoplasias Pulmonares , Triterpenos Pentacíclicos , Transducción de Señal , Serina-Treonina Quinasas TOR , Macrófagos Asociados a Tumores , Serina-Treonina Quinasas TOR/metabolismo , Serina-Treonina Quinasas TOR/genética , Animales , Ratones , Transducción de Señal/efectos de los fármacos , Humanos , Carcinoma de Pulmón de Células no Pequeñas/tratamiento farmacológico , Carcinoma de Pulmón de Células no Pequeñas/genética , Carcinoma de Pulmón de Células no Pequeñas/inmunología , Carcinoma de Pulmón de Células no Pequeñas/metabolismo , Neoplasias Pulmonares/tratamiento farmacológico , Neoplasias Pulmonares/inmunología , Neoplasias Pulmonares/genética , Neoplasias Pulmonares/metabolismo , Triterpenos Pentacíclicos/farmacología , Macrófagos Asociados a Tumores/efectos de los fármacos , Macrófagos Asociados a Tumores/inmunología , Línea Celular Tumoral , Triterpenos/farmacología , Proliferación Celular/efectos de los fármacos , Apoptosis/efectos de los fármacos , Transición Epitelial-Mesenquimal/efectos de los fármacos
19.
Angew Chem Int Ed Engl ; : e202410596, 2024 Jul 19.
Artículo en Inglés | MEDLINE | ID: mdl-39031951

RESUMEN

Selective CO2 photoreduction to value-added multi-carbon (C2+) feedstocks, such as C2H4, holds great promise in direct solar-to-chemical conversion for a carbon-neutral future. Nevertheless, the performance is largely inhibited by the high energy barrier of C-C coupling process, thereby leading to C2+ products with low selectivity. Here we report that through facile surface immobilization of a 1-ethyl-3-methylimidazolium tetrafluoroborate (EMIM-BF4) ionic liquid, plasmonic Cu nanowires could enable highly selective CO2 photoreduction to C2H4 product. At an optimal condition, the resultant plasmonic photocatalyst exhibits C2H4 production with selectivity up to 96.7% under 450 nm monochromatic light irradiation, greatly surpassing its pristine Cu counterpart. Combined in situ spectroscopies and computational calculations unravel that the addition of EMIM-BF4 ionic liquid modulates the local electronic structure of Cu, resulting in its enhanced adsorption strength of *CO intermediate and significantly reduced energy barrier of C-C coupling process. This work paves new path for Cu surface plasmons in selective artificial photosynthesis to targeted products.

20.
Angew Chem Int Ed Engl ; 63(15): e202400965, 2024 Apr 08.
Artículo en Inglés | MEDLINE | ID: mdl-38363034

RESUMEN

Recently, amorphous materials have gained great attention as an emerging kind of functional material, and their characteristics such as isotropy, absence of grain boundaries, and abundant defects are very likely to outrun the disadvantages of crystalline counterparts, such as low conductivity, and ultimately lead to improved charge transfer efficiency. Herein, we investigated the effect of amorphization on the charge transfer process and photocatalytic performance with a phosphonate-based metal-organic framework (FePPA) as the research object. Comprehensive experimental results suggest that compared to crystalline FePPA, amorphous FePPA has more distorted metal nodes, which affects the electron distribution and consequently improves the photogenerated charge separation efficiency. Meanwhile, the distorted metal nodes in amorphous FePPA also greatly promote the adsorption and activation of O2. Hence, amorphous FePPA exhibits a better performance of photocatalytic C(sp3)-H bond activation for selective oxidation of toluene to benzaldehyde. This work illustrates the advantages of amorphous MOFs in the charge transfer process, which is conducive to the further development of high performance MOFs-based photocatalysts.

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