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1.
J Biol Chem ; 300(8): 107556, 2024 Jul 11.
Artigo em Inglês | MEDLINE | ID: mdl-39002683

RESUMO

Diversity, a hallmark of G protein-coupled receptor (GPCR) signaling, partly stems from alternative splicing of a single gene generating more than one isoform for a receptor. Additionally, receptor responses to ligands can be attenuated by desensitization upon prolonged or repeated ligand exposure. Both phenomena have been demonstrated and exemplified by the deuterostome tachykinin signaling system, although the role of phosphorylation in desensitization remains a subject of debate. Here, we describe the signaling system for tachykinin-related peptides (TKRPs) in a protostome, mollusk Aplysia. We cloned the Aplysia TKRP precursor, which encodes three TKRPs (apTKRP-1, apTKRP-2a, and apTKRP-2b) containing the FXGXR-amide motif. In situ hybridization and immunohistochemistry showed predominant expression of TKRP mRNA and peptide in the cerebral ganglia. TKRPs and their posttranslational modifications were observed in extracts of central nervous system ganglia using mass spectrometry. We identified two Aplysia TKRP receptors (apTKRPRs), named apTKRPR-A and apTKRPR-B. These receptors are two isoforms generated through alternative splicing of the same gene and differ only in their intracellular C termini. Structure-activity relationship analysis of apTKRP-2b revealed that both C-terminal amidation and conserved residues of the ligand are critical for receptor activation. C-terminal truncates and mutants of apTKRPRs suggested that there is a C-terminal phosphorylation-independent desensitization for both receptors. Moreover, apTKRPR-B also exhibits phosphorylation-dependent desensitization through the phosphorylation of C-terminal Ser/Thr residues. This comprehensive characterization of the Aplysia TKRP signaling system underscores the evolutionary conservation of the TKRP and TK signaling systems, while highlighting the intricacies of receptor regulation through alternative splicing and differential desensitization mechanisms.

2.
J Am Chem Soc ; 146(25): 17103-17113, 2024 Jun 26.
Artigo em Inglês | MEDLINE | ID: mdl-38869216

RESUMO

Understanding the interfacial hydrogen evolution reaction (HER) is crucial to regulate the electrochemical behavior in aqueous zinc batteries. However, the mechanism of HER related to solvation chemistry remains elusive, especially the time-dependent dynamic evolution of the hydrogen bond (H-bond) under an electric field. Herein, we combine in situ spectroscopy with molecular dynamics simulation to unravel the dynamic evolution of the interfacial solvation structure. We find two critical change processes involving Zn-electroplating/stripping, including the initial electric double layer establishment to form an H2O-rich interface (abrupt change) and the subsequent dynamic evolution of an H-bond (gradual change). Moreover, the number of H-bonds increases, and their strength weakens in comparison with the bulk electrolyte under bias potential during Zn2+ desolvation, forming a diluted interface, resulting in massive hydrogen production. On the contrary, a concentrated interface (H-bond number decreases and strength enhances) is formed and produces a small amount of hydrogen during Zn2+ solvation. The insights on the above results contribute to deciphering the H-bond evolution with competition/corrosion HER during Zn-electroplating/stripping and clarifying the essence of electrochemical window widened and HER suppression by high concentration. This work presents a new strategy for aqueous electrolyte regulation by benchmarking the abrupt change of the interfacial state under an electric field as a zinc performance-enhancement criterion.

3.
Materials (Basel) ; 17(11)2024 May 28.
Artigo em Inglês | MEDLINE | ID: mdl-38893854

RESUMO

The thermal properties, microstructure, and mechanical properties of Fe-18Mn-3Ti (wt%) were investigated, focusing on the effects of different heat-treatment processes. Results revealed that the 450 °C warm-rolling sample (450 WR) exhibited promising mechanical properties. Specifically, this sample displayed a yield strength of 988 MPa, an ultimate tensile strength of 1052 MPa, and total elongation of 15.49%. Consequently, a favorable strength-ductility balance was achieved. The strain-hardening ability surpassed that of the cold rolling sample (CR). Microstructure analysis indicated the simultaneous occurrence of dynamic equilibrium between grain deformation and re-crystallization because of the co-influence of thermal and strain in the warm rolling process. This desirable mechanical property was attributed to the presence of a multi-phase (α-martensite, austenite, and ε-martensite) and heterogeneous microstructure. The improvement of ultimate tensile strength was based on grain refinement, grain co-deformation, and the transformation-induced plasticity (TRIP) effect in the early stage of plastic deformation (stage Ⅰ). The improvement of ultimate elongation (TEL) was ascribed to the TRIP effect in the middle stage of plastic deformation (stage Ⅱ).

4.
Adv Mater ; 36(13): e2312159, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38117030

RESUMO

Developing sacrificial cathode prelithiation technology to compensate for active lithium loss is vital for improving the energy density of lithium-ion battery full-cells. Li2CO3 owns high theoretical specific capacity, superior air stability, but poor conductivity as an insulator, acting as a promising but challenging prelithiation agent candidate. Herein, extracting a trace amount of Co from LiCoO2 (LCO), a lattice engineering is developed through substituting Li sites with Co and inducing Li defects to obtain a composite structure consisting of (Li0.906Co0.043▫0.051)2CO2.934 and ball milled LiCoO2 (Co-Li2CO3@LCO). Notably, both the bandgap and Li─O bond strength have essentially declined in this structure. Benefiting from the synergistic effect of Li defects and bulk phase catalytic regulation of Co, the potential of Li2CO3 deep decomposition significantly decreases from typical >4.7 to ≈4.25 V versus Li/Li+, presenting >600 mAh g-1 compensation capacity. Impressively, coupling 5 wt% Co-Li2CO3@LCO within NCM-811 cathode, 235 Wh kg-1 pouch-type full-cell is achieved, performing 88% capacity retention after 1000 cycles.

5.
Science ; 385(6710): 744-752, 2024 Aug 16.
Artigo em Inglês | MEDLINE | ID: mdl-39146426

RESUMO

Air sensitivity remains a substantial barrier to the commercialization of sodium (Na)-layered oxides (NLOs). This problem has puzzled the community for decades because of the complexity of interactions between air components and their impact on both bulk and surfaces of NLOs. We show here that water vapor plays a pivotal role in initiating destructive acid and oxidative degradations of NLOs only when coupled with carbon dioxide or oxygen, respectively. Quantification analysis revealed that reducing the defined cation competition coefficient (η), which integrates the effects of ionic potential and sodium content, and increasing the particle size can enhance the resistance to acid attack, whereas using high-potential redox couples can eliminate oxidative degradation. These findings elucidate the underlying air deterioration mechanisms and rationalize the design of air-stable NLOs.

6.
ACS Nano ; 2024 Aug 20.
Artigo em Inglês | MEDLINE | ID: mdl-39165001

RESUMO

Topological spin textures are of great significance in magnetic information storage and spintronics due to their high storage density and low drive current. In this work, the transformation of magnetic configuration from chaotic labyrinth domains to uniform stripe domains was observed in MnFe1-xCoxGe magnets. This change occurs due to the noncollinear magnetic structure switching to a uniaxial ferromagnetic structure with increasing Co content, as identified by neutron diffraction results and Lorentz transmission electron microscopy (L-TEM). Of utmost importance, a hexagonal lattice of high-density robust type-II magnetic bubble lattice was established for x = 0.8 through out-of-plane magnetic field stimulation and field-cooling. The dimensions of the type-II magnetic bubbles were found to be tuned by the sample thickness. Therefore, the stabilization of complex magnetic spin textures, associated with enhanced uniaxial ferromagnetic interaction and magnetic dipole-dipole interaction in MnFe1-xCoxGe through magnetic structure manipulation, as further confirmed by the micromagnetic simulations, will provide a convenient and efficient strategy for designing topological spin textures with potential applications in spintronic devices.

7.
Adv Mater ; : e2407720, 2024 Jul 20.
Artigo em Inglês | MEDLINE | ID: mdl-39032096

RESUMO

Compensating for the irreversible loss of limited active sodium (Na) is crucial for enhancing the energy density of practical sodium-ion batteries (SIBs) full-cell, especially when employing hard carbon anode with initially lower coulombic efficiency. Introducing sacrificial cathode presodiation agents, particularly those that own potential anionic oxidation activity with a high theoretical capacity, can provide additional sodium sources for compensating Na loss. Herein, Ni atoms are precisely implanted at the Na sites within Na2O framework, obtaining a (Na0.89Ni0.05□0.06)2O (Ni-Na2O) presodiation agent. The synergistic interaction between Na vacancies and Ni catalyst effectively tunes the band structure, forming moderate Ni-O covalent bonds, activating the oxidation activity of oxygen anion, reducing the decomposition overpotential to 2.8 V (vs Na/Na+), and achieving a high presodiation capacity of 710 mAh/g≈Na2O (Na2O decomposition rate >80%). Incorporating currently-modified presodiation agent with Na3V2(PO4)3 and Na2/3Ni2/3Mn1/3O2 cathodes, the energy density of corresponding Na-ion full-cells presents an essential improvement of 23.9% and 19.3%, respectively. Further, not limited to Ni-Na2O, the structure-function relationship between the anionic oxidation mechanism and electrode-electrolyte interface fabrication is revealed as a paradigm for the development of sacrificial cathode presodiation agent.

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