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1.
Small ; : e2404984, 2024 Jul 19.
Artigo em Inglês | MEDLINE | ID: mdl-39031101

RESUMO

The instability to moisture, heat, and ultraviolet (UV) light is the main problem in the application of quantum dot solar cells (QDSCs). Thin film encapsulation can effectively improve their operational stability. However, it is difficult to achieve multiple barrier effects with single layer of encapsulated film. Here, a hybrid thin-film encapsulation strategy is reported to encapsulate lead sulfide QDSCs, which can isolate moisture and partial thermal, and prevent the penetration of UV light, thus retarding the surface oxidation process of the quantum dots. After 60 h, the encapsulated device retains a normalized power conversion efficiency of 83.8% and 80.6% at 85% humidity and 75 °C, respectively, which is three and six times of the value obtained in unencapsulated devices. At continuous UV illumination, encapsulated device exhibits five times higher stability than the reference. This strategy provides the way for the overall improvement of the operating stability of lead sulfide QDSCs in harsh environments of high humidity, high temperature, and UV light.

2.
Angew Chem Int Ed Engl ; : e202412964, 2024 Jul 24.
Artigo em Inglês | MEDLINE | ID: mdl-39048539

RESUMO

High efficiently photocatalytic CO2 reduction (CO2RR) into liquid fuels in pure water system remains challenged. Iron polyphthalocyanine (FePPc) with strong light harvesting, unique Fe-N4 structure, abundant pores, and good stability could serve as a promising catalyst for CO2 photoreduction. To further improve the catalytic efficiency, herein, symmetry-breaking Fe sites are constructed by coupling with atomically precise M1Ag24 (M=Ag, Au, Pt) series clusters. Especially, the introduction of Pt1Ag24 causes the most asymmetric charge distribution of Fe in FePPc (followed by Au1Ag24 and Ag25), leading to the favorable CO2 adsorption and activation. In addition, Pt1Ag24-FePPc exhibits the most effective photogenerated carriers transfer and separation. As a result, Pt1Ag24-FePPc shows the methanol/ethanol yield of 48.55/32.97 µmol·gcat-1·h-1 in H2O-CO2 system under visible light irradiation, ~ 1.65/1.25-fold, 1.83/1.37-fold, and 3.6/1.61-fold higher than that of Au1Ag24-FePPc, Ag25-FePPc, and FePPc, respectively. This work provides a concept for precisely construction and regulation symmetry-breaking sites of cluster-based catalysts for effective CO2 conversion.

3.
Materials (Basel) ; 17(3)2024 Jan 24.
Artigo em Inglês | MEDLINE | ID: mdl-38591400

RESUMO

This paper introduces a method for high-resolution lattice image reconstruction and dislocation analysis based on diffraction extinction. The approach primarily involves locating extinction spots in the Fourier transform spectrum (reciprocal space) and constructing corresponding diffraction wave functions. By the coherent combination of diffraction and transmission waves, the lattice image of the extinction planes is reconstructed. This lattice image is then used for dislocation localization, enabling the observation and analysis of crystal planes that exhibit electron diffraction extinction effects and atomic jump arrangements during high-resolution transmission electron microscopy (HRTEM) characterization. Furthermore, due to the method's effectiveness in localizing dislocations, it offers a unique advantage when analyzing high-resolution images with relatively poor quality. The feasibility of this method is theoretically demonstrated in this paper. Additionally, the method was successfully applied to observed edge dislocations, such as 1/6[211-], 1/6[2-11-], and 1/2[01-1], which are not easily observable in conventional HRTEM characterization processes, in electro-deposited Cu thin films. The Burgers vectors were determined. Moreover, this paper also attempted to observe screw dislocations that are challenging to observe in high-resolution transmission electron microscopy. By shifting a pair of diffraction extinction spots and superimposing the reconstructed images before and after the shift, screw dislocations with a Burgers vector of 1/2[011-] were successfully observed in electro-deposited Cu thin films.

4.
Adv Mater ; 36(31): e2401965, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38631703

RESUMO

Tailorable lithium (Li) nucleation and uniform early-stage plating is essential for long-lifespan Li metal batteries. Among factors influencing the early plating of Li anode, the substrate is critical, but a fine control of the substrate structure on a scale of ≈10 nm has been rarely achieved. Herein, a carbon consisting of ordered grids is prepared, as a model to investigate the effect of substrate structure on the Li nucleation. In contrast to the individual spherical Li nuclei formed on the flat graphene, an ultrauniform and nuclei-free Li plating is obtained on the ordered carbon with a grid size smaller than the thermodynamical critical radius of Li nucleation (≈26 nm). Simultaneously, an inorganic-rich solid-electrolyte-interphase is promoted by the cross-sectional carbon layers of such ordered grids which are exposed to the electrolyte. Consequently, the carbon grids with a grid size of ≈10 nm show a favorable cycling stability for more than 1100 cycles measured at 2 mA cm-2 in a half cell. With LiNi0.8Co0.1Mn0.1O2 as cathode, the assembled full cell with a cathode capacity of 3 mAh cm-2 and a negative/positive ratio of 1.67 demonstrates a stable cycling for over 130 cycles with a capacity retention of 88%.

5.
Adv Mater ; 36(24): e2313931, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38552603

RESUMO

Current reconstruction chemistry studies are mainly operated at the laboratory scale, where the operating parameters are different from those used in industrial water electrolyzers. This gap leads to unclear reconstruction behaviors under industrial conditions and constrains the application of catalysts. Here, this work presents a new reconstruction mechanism and anomalous detachment phenomena observed in leaching-type oxygen-evolving precatalysts under industrial conditions, different from the reported results obtained under laboratory conditions. The identified detachment issues are closely linked to the production of a potassium salt separate phase, which proves sensitive to the local environment, and its instability easily leads to catalyst stripping from the substrate. By establishing detachment critical point and operating parameter-detachment correlation, a targeted reconstruction strategy is proposed to achieve smooth ligand leaching and effectively solve the detachment issue. Theoretical analyses validate the dual-site regulation in directionally reconstructed catalysts with optimized intermediate adsorption. Under industrial conditions, the coupled electrolyzer delivers an industrial-level current density at low cell voltage with prolonged durability, 1 A cm-2 at 2 V for over 340 h. This work bridges the gap of leaching-type precatalysts between laboratory test conditions and industrial operating conditions.

6.
Int Immunopharmacol ; 128: 111530, 2024 Feb 15.
Artigo em Inglês | MEDLINE | ID: mdl-38278068

RESUMO

Preoperative stress has been recognized as an independent risk factor for chronic postsurgical pain (CPSP). However, the underlying mechanisms of CPSP influenced by preoperative stress remain elusive. Previous studies indicated that excessive stress could induce disruption of the blood-spinal cord barrier (BSCB). We wondered whether and how BSCB involves in CPSP by using a single prolonged stress (SPS) combining plantar incision model in male rats to mimic preoperative stress-related postsurgical pain. Here, we observed that preoperative SPS-exposed rats exhibited relentless incisional pain, which was accompanied by impairment of BSCB and persistent elevation of serum IL-6. Intraperitoneal injections of Tocilizumab (an IL-6 receptor monoclonal antibody) not only mitigated BSCB breakdown but also alleviated pain behaviors. In addition, intervening ß3-adrenoceptor (ADRB3) signaling in brown adipocytes by SR59230a (a specific ADRB3 antagonist) treatment or removal of brown adipose tissues could effectively decrease serum IL-6 levels, ameliorate BSCB disruption, and alleviate incisional pain. Further results displayed that SI-exposed rats also showed markedly spinal microglia activation. And exogenous His-tagged IL-6 could pass through the disrupted BSCB, which might contribute to microglia activation. Injection of SR59230a or ablation of brown adipose tissues could effectively reduce the activation of spinal microglia. Thus, our findings suggest that serum IL-6 induced by brown adipocyte ADRB3 signaling contributed to BSCB disruption and spinal microglia activation, which might be involved in preoperative stress mediated CPSP. This work indicates a promising treatment strategy for preoperative stress induced CPSP by blocking ADRB3.


Assuntos
Adipócitos Marrons , Propanolaminas , Traumatismos da Medula Espinal , Animais , Masculino , Ratos , Adipócitos Marrons/metabolismo , Interleucina-6/metabolismo , Dor Pós-Operatória , Ratos Sprague-Dawley , Receptores Adrenérgicos/metabolismo , Medula Espinal , Traumatismos da Medula Espinal/metabolismo , Receptores Adrenérgicos beta 3/metabolismo
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