Your browser doesn't support javascript.
loading
Mostrar: 20 | 50 | 100
Resultados 1 - 20 de 65
Filtrar
1.
Nat Commun ; 15(1): 4734, 2024 Jun 03.
Artigo em Inglês | MEDLINE | ID: mdl-38830907

RESUMO

Achieving effective manipulation of perpendicular exchange bias effect remains an intricate endeavor, yet it stands a significance for the evolution of ultra-high capacity and energy-efficient magnetic memory and logic devices. A persistent impediment to its practical applications is the reliance on external magnetic fields during the current-induced switching of exchange bias in perpendicularly magnetized structures. This study elucidates the achievement of a full electrical manipulation of the perpendicular exchange bias in the multilayers with an ultrathin antiferromagnetic layer. Owing to the anisotropic epitaxial strain in the 2-nm-thick IrMn3 layer, the considerable exchange bias effect is clearly achieved at room temperature. Concomitantly, a specific global uncompensated magnetization manifests in the IrMn3 layer, facilitating the switching of the irreversible portion of the uncompensated magnetization. Consequently, the perpendicular exchange bias can be manipulated by only applying pulsed current, notably independent of the presence of any external magnetic fields.

2.
ACS Appl Mater Interfaces ; 16(17): 21905-21914, 2024 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-38634487

RESUMO

For acid-water oxidation, pyrochloric ruthenates are thought to be extremely effective electrocatalysts. In this work, through partial B-site replacement with larger M2+ cations, the electronic states of Y2Ru2O7 with strong electron correlations are reasonably managed, by which the inherent performance is tremendously promoted. Based on this, the improved Y2Ru1.9Sr0.1O7 electrocatalyst exhibits an outstanding durability and presents a highly inherent mass activity of 1915.1 A gRu-1 (at 1.53 V vs RHE). The enhanced oxygen-evolving reaction (OER) activity by ionic dopant in YRO pyrochlore can be attributed to two aspects, i.e., the lattice distortion induced inhibition of the grain coarsening, which results in a large surface area for YRO-M and increases the OER active sites, and the weakening of electron correlation via broadening of the Ru 4d bandwidths due to the increase of the average radius of B-site ions, which gives rise to an enhancement of conductivity and a strengthened hybridization between Ru 4d and O 2p orbitals and improves the reaction kinetics. The synergistic effects of lattice distortion and orbital hybridization promote the enhanced OER activity. The results would provide fresh concepts for the design of improved electrocatalysts and underscore the significance of managing the intrinsic performance through the dual modification of microstructure morphology and electronic structure.

3.
Phys Rev Lett ; 132(5): 056702, 2024 Feb 02.
Artigo em Inglês | MEDLINE | ID: mdl-38364119

RESUMO

We report a giant hysteretic spin Seebeck effect (SSE) anomaly with a sign reversal at magnetic fields much stronger than the coercive field in a (001)-oriented Tb_{3}Fe_{5}O_{12} film. The high-field SSE enhancement reaches 4200% at approximately 105 K over its weak-field value and presents a nonmonotonic dependence on temperature. The unexpected high-field hysteresis of SSE is found to be associated with a magnetic transition of double-umbrella spin texture in TbIG. Nearly parallel dispersion curves of magnons and acoustic phonons around this neoteric transition are supported by theoretical calculations, leading to a high density of field-tuned magnon polarons and consequently an extraordinarily large SSE. Our study provides insight into the evolution of magnon dispersions of double-umbrella TbIG and could potentially boost the efficiency of magnon-polarons SSE devices.

4.
Nat Commun ; 15(1): 1767, 2024 Feb 26.
Artigo em Inglês | MEDLINE | ID: mdl-38409177

RESUMO

Developing efficient and economical electrocatalysts for acidic oxygen evolution reaction (OER) is essential for proton exchange membrane water electrolyzers (PEMWE). Cobalt oxides are considered promising non-precious OER catalysts due to their high activities. However, the severe dissolution of Co atoms in acid media leads to the collapse of crystal structure, which impedes their application in PEMWE. Here, we report that introducing acid-resistant Ir single atoms into the lattice of spinel cobalt oxides can significantly suppress the Co dissolution and keep them highly stable during the acidic OER process. Combining theoretical and experimental studies, we reveal that the stabilizing effect induced by Ir heteroatoms exhibits a strong dependence on the distance of adjacent Ir single atoms, where the OER stability of cobalt oxides continuously improves with decreasing the distance. When the distance reduces to about 0.6 nm, the spinel cobalt oxides present no obvious degradation over a 60-h stability test for acidic OER, suggesting potential for practical applications.

5.
J Am Chem Soc ; 146(10): 6536-6543, 2024 Mar 13.
Artigo em Inglês | MEDLINE | ID: mdl-38412553

RESUMO

The past decade has witnessed substantial progress in understanding nontrivial band topology and discovering exotic topological materials in condensed-matter physics. Recently, topological physics has been further extended to the chemistry discipline, leading to the emergence of topological catalysis. In principle, the topological effect is detectable in catalytic reactions, but no conclusive evidence has been reported yet. Herein, by precisely manipulating the topological surface state (TSS) of Bi2Se3 nanosheets through thickness control and the application of a magnetic field, we provide direct experimental evidence to illustrate topological catalysis for CO2 electroreduction. With and without the cooperation of TSS, CO2 is mainly reduced into liquid fuels (HCOOH and H2C2O4) and CO, exhibiting high (up to 90% at -1.1 V versus reversible hydrogen electrode) and low Faradaic efficiency (FE), respectively. Theoretically, the product and FE difference can be attributed to the TSS-regulated adsorption of key intermediates and the reduced barrier of the potential-determining step. Our work demonstrates the inherent correlation between band topology and electrocatalysis, paving a new avenue for designing high-performance catalysts.

6.
Nat Commun ; 15(1): 559, 2024 Jan 16.
Artigo em Inglês | MEDLINE | ID: mdl-38228626

RESUMO

The metal-support interactions (MSI) could greatly determine the electronic properties of single-atom catalysts, thus affecting the catalytic performance. However, the typical approach to regulating MSI usually suffers from interference of the variation of supports or sacrificing the stability of catalysts. Here, we effectively regulate the site-specific MSI of Ir single atoms anchored on Ni layered double hydroxide through an electrochemical deposition strategy. Cathodic deposition drives Ir atoms to locate at three-fold facial center cubic hollow sites with strong MSI, while anodic deposition drives Ir atoms to deposit onto oxygen vacancy sites with weak MSI. The mass activity and intrinsic activity of Ir single-atom catalysts with strong MSI towards oxygen evolution reaction are 19.5 and 5.2 times that with weak MSI, respectively. Mechanism study reveals that the strong MSI between Ir atoms and the support stimulates the activity of Ir sites by inducing the switch of active sites from Ni sites to Ir sites and optimizes the adsorption strength of intermediates, thereby enhancing the activity.

7.
Nano Lett ; 23(8): 3309-3316, 2023 Apr 26.
Artigo em Inglês | MEDLINE | ID: mdl-36946560

RESUMO

Integrating single atoms and clusters into one system is a novel strategy to achieve desired catalytic performances. Compared with homogeneous single-atom cluster catalysts, heterogeneous ones combine the merits of different species and therefore show greater potential. However, it is still challenging to construct single-atom cluster systems of heterogeneous species, and the underlying mechanism for activity improvement remains unclear. In this work, we developed a heterogeneous single-atom cluster catalyst (ConIr1/N-C) for efficient oxygen evolution. The Ir single atoms worked in synergy with the Co clusters at a distance of about 8 Å, which optimized the configuration of the key intermediates. Consequently, the oxygen evolution activity was significantly improved on ConIr1/N-C relative to the Co cluster catalyst (Con/N-C), exhibiting an overpotential lower by 107 mV than that of Con/N-C at 10 mA cm-2 and a turnover frequency 50.9 times as much as that of Con/N-C at an overpotential of 300 mV.

8.
Angew Chem Int Ed Engl ; 62(15): e202216837, 2023 Apr 03.
Artigo em Inglês | MEDLINE | ID: mdl-36598399

RESUMO

Developing efficient and stable transition metal oxides catalysts for energy conversion processes such as oxygen evolution reaction and oxygen reduction reaction is one of the key measures to solve the problem of energy shortage. The spin state of transition metal oxides is strongly correlated with their catalytic activities. In an octahedral structure of transition metal oxides, the spin state of active centers could be regulated by adjusting the splitting energy and the electron pairing energy. Regulating spin state of active centers could directly modulate the d orbitals occupancy, which influence the strength of metal-ligand bonds and the adsorption behavior of the intermediates. In this review, we clarified the significance of regulating spin state of the active centers. Subsequently, we discussed several characterization technologies for spin state and some recent strategies to regulate the spin state of the active centers. Finally, we put forward some views on the future research direction of this vital field.

9.
Adv Sci (Weinh) ; 10(6): e2205903, 2023 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-36596707

RESUMO

Coherent optical control of the magnetization in ferromagnetic (FM) mediums using ultrafast nonthermal effect paves a promising avenue to improve the speed and repetition rate of the magnetization manipulation. Whereas previously, only heat-induced or helicity-dependent magnetization dynamics are demonstrated in metallic ferromagnets. Here, the linearly-polarized light control of magnetization is demonstrated in FM Co coupled with ferroelectric (FE) BiFeO3 by tuning the light polarization direction. It is revealed that in the Co/BiFeO3 heterostructure excited by femtosecond laser pulses, the magnetization precession amplitude follows a sinusoidal dependence on the laser polarization direction. This nonthermal control of coherent magnetization rotation is attributed to the optical rectification effect in the BiFeO3 layer, which yields a FE polarization depending on the light polarization, and the subsequent modulation of magnetic energy in Co by the electrostriction-induced strain. This work demonstrates an effective route to nonthermally manipulate the ultrafast magnetization dynamics in metallic ferromagnets.

10.
Nat Commun ; 13(1): 4447, 2022 Aug 01.
Artigo em Inglês | MEDLINE | ID: mdl-35915121

RESUMO

Current induced spin-orbit torques driven by the conventional spin Hall effect are widely used to manipulate the magnetization. This approach, however, is nondeterministic and inefficient for the switching of magnets with perpendicular magnetic anisotropy that are demanded by the high-density magnetic storage and memory devices. Here, we demonstrate that this limitation can be overcome by exploiting a magnetic spin Hall effect in noncollinear antiferromagnets, such as Mn3Sn. The magnetic group symmetry of Mn3Sn allows generation of the out-of-plane spin current carrying spin polarization collinear to its direction induced by an in-plane charge current. This spin current drives an out-of-plane anti-damping torque providing the deterministic switching of the perpendicular magnetization of an adjacent Ni/Co multilayer. Due to being odd with respect to time reversal symmetry, the observed magnetic spin Hall effect and the resulting spin-orbit torque can be reversed with reversal of the antiferromagnetic order. Contrary to the conventional spin-orbit torque devices, the demonstrated magnetization switching does not need an external magnetic field and requires much lower current density which is useful for low-power spintronics.

11.
ACS Macro Lett ; 11(1): 26-32, 2022 01 18.
Artigo em Inglês | MEDLINE | ID: mdl-35574802

RESUMO

Here, we report a distinct approach for regulating the substrate specificity of enzymes immobilized in microgels by a phase transition in polymer networks. The finding is demonstrated on glucose oxidase that is immobilized in thermoresponsive poly(N-isopropylacrylamide)-based microgels. Laser light scattering and enzymatic oxidation tests indicate that the broadened specificity appears at low temperatures, at which the gel matrix is in the relatively swollen state relative to its state at microgel synthesis temperature; upon heating to the relative higher temperatures, the gel matrix is not able to shrink further that offers a tight space in which the enzyme resides to retain high glucose specificity. It is proposed that polymer phase transition in the gel matrix mainly alter protein gates that control passage of substrates into active sites, making them open or close to a certain extent that enable reversible regulating the substrate specificity. The finding is also observed on bulk gels under a rational design, making it of potential interest in enzymatic biofuel cell applications.


Assuntos
Microgéis , Géis/química , Transição de Fase , Polímeros/química , Especificidade por Substrato
12.
J Am Chem Soc ; 144(21): 9271-9279, 2022 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-35549330

RESUMO

The two-dimensional surface or one-dimensional interface of heterogeneous catalysts is essential to determine the adsorption strengths and configurations of the reaction intermediates for desired activities. Recently, the development of single-atom catalysts has enabled an atomic-level understanding of catalytic processes. However, it remains obscure whether the conventional concept and mechanism of one-dimensional interface are applicable to zero-dimensional single atoms. In this work, we arranged the locations of single atoms to explore their interfacial interactions for improved oxygen evolution. When iridium single atoms were confined into the lattice of CoOOH, efficient electron transfer between Ir and Co tuned the adsorption strength of oxygenated intermediates. In contrast, atomic iridium species anchored on the surface of CoOOH induced inappreciable modification in electronic structures, whereas steric interactions with key intermediates at its Ir-OH-Co interface played a primary role in reducing its energy barrier toward oxygen evolution.

13.
ACS Omega ; 7(16): 14148-14159, 2022 Apr 26.
Artigo em Inglês | MEDLINE | ID: mdl-35559179

RESUMO

Under the condition of heavy oil thermal recovery, the cement sheath is easy to crack in the high temperature environment, resulting in the decrease of cement paste strength, which may further cause sealing failure and oil and gas production safety accidents. In this paper, the influence of graphite on the mechanical properties of cement paste under the simulated thermal recovery of heavy oil was studied, and its mechanism is explored by testing and analyzing the microstructure. The phase composition and microstructure of graphite-cement composites were determined by X-ray diffraction analysis (XRD) and scanning electron microscope (SEM), and the thermogravimetric analyzer (TG/DTG) was used to analyze the heat resistance of the graphite-cement composites. The results show that the addition of graphite significantly improved the strength and deformation resistance of the Class G oil well cement at high temperature (300, 400, and 500 °C) and low temperature (50 °C), and the optimal addition amount is 0.07%. The microscopic analysis shows that the incorporation of graphite promoted the formation of hydration products, and played a role in filling pores and reducing microcracks in cement pastes. At the same time, due to the better thermal conductivity of graphite, it can balance the internal thermal stress of the cement pastes and inhibit the strength decline of cement pastes under high temperature environments. The integrity of cement pastes was guaranteed through the mechanism of "crack deflection" and "crack bridging". The research results of this paper have presented a certain theoretical basis and new ideas for the development of cementing slurry systems in heavy oil thermal recovery wells.

14.
Nat Commun ; 13(1): 2473, 2022 May 05.
Artigo em Inglês | MEDLINE | ID: mdl-35513390

RESUMO

The homogeneity of single-atom catalysts is only to the first-order approximation when all isolated metal centers interact identically with the support. Since the realistic support with various topologies or defects offers diverse coordination environments, realizing real homogeneity requires precise control over the anchoring sites. In this work, we selectively anchor Ir single atoms onto the three-fold hollow sites (Ir1/TO-CoOOH) and oxygen vacancies (Ir1/VO-CoOOH) on defective CoOOH surface to investigate how the anchoring sites modulate catalytic performance. The oxygen evolution activities of Ir1/TO-CoOOH and Ir1/VO-CoOOH are improved relative to CoOOH through different mechanisms. For Ir1/TO-CoOOH, the strong electronic interaction between single-atom Ir and the support modifies the electronic structure of the active center for stronger electronic affinity to intermediates. For Ir1/VO-CoOOH, a hydrogen bonding is formed between the coordinated oxygen of single-atom Ir center and the oxygenated intermediates, which stabilizes the intermediates and lowers the energy barrier of the rate-determining step.

15.
Adv Mater ; 34(30): e2202677, 2022 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-35612001

RESUMO

Controlling lattice vibrations to obtain intrinsic low thermal conductivity play a critical role in thermal management of electronic and photonic devices, energy converters, and thermal insulation, which necessitates exploring new compounds and a thorough understanding of their chemical structure, bonding, and lattice dynamics. Herein, a new chalcogenide, Ga6 Cr5 Se16 , shows intrinsic low lattice thermal conductivity κlat , which crystallizes in the monoclinic phase (C2/m) with the stacked inverse GaSe4 layers (g'), close-packed Cr3+ Se6 layers (c), GaSe4 layers (g) and loosely-stacked Cr2+ Se6 layers (c') along the c-axis. In this structure, a wide variety of chemical bonding is arranged in each layer, such as covalent Ga-Se, covalent Cr3+ -Se, and weaker Cr2+ -Se bonding, which endow it with a large phonon symphony by strong coupling of soft acoustic and low-lying optical phonons. As a result, Ga6 Cr5 Se16 realizes an intrinsic low κlat of 0.79 W m- 1  K- 1 at 323 K, which is almost four times, or twice lower than that of Cr3 Se4 (2.95 W m- 1  K- 1 ), or Cr2 Se3 (1.56 W m- 1  K- 1 ), Ga2 Se3 (1.36 W m- 1 K- 1 ) at 323 K, respectively. These insights will offer comprehensive understanding of the phonon propagation in complex layered chalcogenides, and also shed useful light on future design of low-κlat solids.

16.
Small ; 18(16): e2105129, 2022 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-35253963

RESUMO

Single-atom catalysts (SACs) can achieve excellent catalytic efficiency at ultralow catalyst consumptions. Herein, platinum (Pt) atoms are fixed on the wall of atomic layer deposition (ALD)-made molybdenum disulfide nanotube arrays (MoS2 -NTA) for efficient hydrogen evolution reaction (HER). More concretely, MoS2 -NTA with different nanotube diameters and wall thicknesses are fabricated by a sacrificial strategy of anodic aluminum oxide (AAO) template via ALD; then Pt atoms are fixed on the wall of Ti3 C2 -supported MoS2 -NTA as a catalytic system. The MoS2 -NTA/Ti3 C2 decorated with 0.13 wt.% of Pt results in a low overpotential of 32 mV to deliver a current density of 10 mA cm-2 , which is superior to 20 wt.% commercial Pt/C (41 mV). Ordered MoS2 -NTA instead of 2D MoS2 prevents Pt atoms from aggregating and then exerts catalytic activities. The density functional theory calculations suggest that the Pt atoms are more likely to occupy the sites on the tubular MoS2 than the planar MoS2 , and the Pt atoms accumulated at the Mo site of MoS2 -NT have a moderate Gibbs free energy (close to zero).

17.
Nano Lett ; 21(11): 4795-4801, 2021 Jun 09.
Artigo em Inglês | MEDLINE | ID: mdl-34018755

RESUMO

Oxygen evolution reaction (OER) plays an important role in renewable energy supplies as the anodic reaction for electrochemical transformation of various chemicals. Iron-based OER catalysts are potential candidates due to their abundance but suffer from poor activity. Here we demonstrate that a single-atom iron catalyst with in-situ generated Fe4+ centers is highly active toward OER. Only an overpotential of 320 mV was needed to reach 10 mA cm-2. The catalyst exhibited an ultrahigh turnover frequency of 0.62 s-1 at an overpotential of 0.35 V, which is comparable to currently reported transitional-metal based OER catalysts. Experimental and theoretical studies revealed that the valence state of the metal center transferred from Fe3+ to highly active Fe4+ prior to the OER process. This transformation was originated from the strong interaction between atomic Fe and carbon support via C-O-Fe bonding, leading to a lower energy barrier of the rate-limiting *OOH formation.

18.
Medicine (Baltimore) ; 100(13): e25239, 2021 Apr 02.
Artigo em Inglês | MEDLINE | ID: mdl-33787607

RESUMO

BACKGROUND: There is no systematic review to compare the efficacy of acupuncture and acupotomy in patients with cervical spondylotic radiculopathy. It is worthy to critically review the evidence of the comparison of these 2 therapies to inform clinical practice. Therefore, the purpose of this study was to compare the efficacy and safety of acupuncture and acupotomy in the treatment of cervical spondylotic radiculopathy and to provide evidence for clinical practice. METHODS: Seven electronic databases including Web of Science, Embase, PubMed, Wanfang Data, Scopus, Science Direct, Cochrane Library were searched in March 2021 by 2 independent reviewers. Data extraction was performed independently, and any conflict was resolved before final analysis. Only randomized clinical trials were included in this study. Outcomes included pain intensity, symptom score, neck disability index, total effective rate, and curative rate. The Cochrane risk of bias tool is used to evaluate the risk of bias of included randomized controlled trials by 2 independent reviewers. RESULTS: We hypothesized that these 2 methods would provide similar therapeutic benefits. The results of this research will be delivered in a peer-reviewed journal. CONCLUSION: This study expects to provide credible and scientific clinical evidence for the efficacy and safety of acupuncture and acupotomy in the treatment of cervical spondylotic radiculopathy. OSF REGISTRATION NUMBER: 10.17605/OSF.IO/U7T6A.


Assuntos
Terapia por Acupuntura/métodos , Radiculopatia/terapia , Espondilose/terapia , Humanos , Metanálise como Assunto , Ensaios Clínicos Controlados Aleatórios como Assunto , Projetos de Pesquisa , Revisões Sistemáticas como Assunto , Resultado do Tratamento
19.
Phys Rev Lett ; 127(27): 277203, 2021 Dec 31.
Artigo em Inglês | MEDLINE | ID: mdl-35061405

RESUMO

The spin Seebeck effect (SSE) signal of magnon polarons in bulk-Y_{3}Fe_{5}O_{12} (YIG)/Pt heterostructures is found to drastically change as a function of temperature. It appears as a dip in the total SSE signal at low temperatures, but as the temperature increases, the dip gradually decreases before turning to a peak. We attribute the observed dip-to-peak transition to the rapid rise of the four-magnon scattering rate. Our analysis provides important insights into the microscopic origin of the hybridized excitations and the overall temperature dependence of the SSE anomalies.

20.
Chem Biol Drug Des ; 96(5): 1272-1279, 2020 11.
Artigo em Inglês | MEDLINE | ID: mdl-32491272

RESUMO

BACKGROUND: Gambogenic acid (GNA) is one of the main active components of Gamboge, and its anticancer role has been reported in some cancers. The study was to investigate the inhibitory effects of GNA on the proliferation and metastasis of bladder cancer (BC) cells and its potential regulatory mechanisms. MATERIALS AND METHODS: BC cell lines (BIU-87 cells, T24 cells, and J82 cells) were treated with different doses of GNA for different time, and then the effects of GNA on BC cell were examined in vitro using CCK-8 assay, apoptosis assays, and Transwell tests. NF-κB signaling activity was detected by the NF-κB p65 luciferase reporter assay. Western blot was used to detect the expressions of cIAP2, XIAP, Survivin, and p65. RESULTS: GNA inhibited the viability of BC cells in vitro in a dose- and time-dependent manner and facilitated apoptosis of BC cells. Moreover, GNA could remarkably impede the migration and invasion abilities of BC cells. In terms of mechanism, GNA administration reduced the activity of NF-κB signaling and down-regulated the expressions of p65, survivin, XIAP, and cIAP2. CONCLUSION: GNA blocks the growth and metastasis of BC cells via inhibiting the NF-κB signal transduction pathway.


Assuntos
Proliferação de Células/efeitos dos fármacos , NF-kappa B/metabolismo , Metástase Neoplásica/prevenção & controle , Transdução de Sinais/efeitos dos fármacos , Neoplasias da Bexiga Urinária/prevenção & controle , Xantenos/farmacologia , Linhagem Celular Tumoral , Humanos , Neoplasias da Bexiga Urinária/metabolismo , Neoplasias da Bexiga Urinária/patologia
SELEÇÃO DE REFERÊNCIAS
DETALHE DA PESQUISA