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1.
J Am Chem Soc ; 2024 Sep 25.
Artigo em Inglês | MEDLINE | ID: mdl-39320037

RESUMO

The practical application of Li-CO2 batteries is significantly hindered by high charge potential and short lifespan, mainly due to sluggish reaction kinetics and inadequate reaction reversibility. Homogeneous catalysts added to the electrolyte provide a promising strategy to address these issues. In this work, the third-generation Grubbs catalyst (G-III), which is efficient for olefin metathesis reactions, has been adopted as a homogeneous catalyst for Li-CO2 batteries. Batteries with G-III exhibited a low overpotential of 0.86 V and a lifespan of 1300 h at a current density of 300 mA g-1. Even at a high current density of 2000 mA g-1, the batteries remained stable for over 300 cycles, with an initial overpotential of 1.11 V. A two-step discharge/charge reaction involving Li2C2O4 as an intermediate was well illustrated, attributed to both low overpotentials and high specific capacity. These findings provide insights into catalyst selection and mechanism analysis for Li-CO2 batteries, offering practical strategies for Li-CO2 battery performance enhancement and practical applications.

2.
Angew Chem Int Ed Engl ; : e202413452, 2024 Aug 18.
Artigo em Inglês | MEDLINE | ID: mdl-39155243

RESUMO

Organic-metal coordination materials with rich structural diversity are considered as promising electrode materials for rechargeable sodium-ion batteries. However, the electrochemical performance can be constrained by the limited number of active sites and structural instability under the discharge/charge process. Herein, organometallic polymer microspheres (Fe-PDA-220) with a unique d-π conjugated structure was designed and successfully constructed through a simple synchronous polymerization and coordination reactions. Polymerization of phenylenediamine was initiated by Fe3+ and Fe2+ ions generated synchronously during the polymerization integrated with poly-aminoquinone chains to form Fe-C12N8 active centers. Used as electrode materials for sodium-ion batteries, the distinctive Fe-C bond significantly boosts the structural stability, and the π-d conjugation system could facilitate electron transfer. A high reversible capacity of 345 mAh g-1 was delivered at 0.1 A g-1 and a capacity of 106 mAh g-1 was maintained even after discharged/charged at 1.0 A g-1 for 5000 cycles, outperforming most reported coordination materials. Spectroscopic and electronic analyses revealed that a two-electron reaction occurred per active unit, accompanied by the reversible redox evolution of the C=N groups and Fe ions during  sodiation/desodiation. This work provides a promising and efficient strategy for boosting the electrochemical performance of organic electrode materials by the design of organometallic polymers.

3.
Small ; 18(8): e2105825, 2022 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-34889023

RESUMO

Organic electrode materials with the advantages of renewability, environment-friendliness, low cost, and high capacity have received widespread attention in recent years for sodium-ion batteries. However, small molecular organic materials suffer from issues such as low conductivity and the high dissolution rate in electrolytes. Herein, a phthalocyanine derivative (TPcDS) with a large non-localized π-electron system, obtained through thermodynamic polymerization of 4-aminophthalonitrile (AP) monomers, is designed to address these issues. According to the density function theory calculation, six sodium ions can be attracted by one polymer molecule, indicating a high theoretical capacity of 375 mA h g-1 . The TPcDS molecule realizes sodium storage through a non-localized π-electron system of phthalocyanine macrocycles. When employed as an anode material for sodium-ion batteries, the functional groups of phthalocyanine macrocycles, such as CN groups in TPcDS, experience obviously reversible structural variation upon discharge/charge. A high reversible capacity of 364 mAh g-1 is achieved at a current density of 0.05 A g-1 , and a charge capacity of as high as 246 mAh g-1 is still maintained after 500 cycles at 0.1 A g-1 . This work provides an effective strategy for the design and synthesis of new oligomeric organic electrode materials.

4.
Appl Opt ; 58(27): 7609-7614, 2019 Sep 20.
Artigo em Inglês | MEDLINE | ID: mdl-31674416

RESUMO

This paper proposes an accommodative intraocular lens (IOL), which consists of a two-element Alvarez lens and an aspheric lens for changing focal power and refractive power, respectively. The four-freeform-surface Alvarez lens is optimized for a multiple field of view; further, the aspheric lens also corrects the aberrations induced by the corneal asphericity of the human eye over the whole range of accommodation. A simulation using optical design software demonstrates its excellent performance in that the values of the modulation transfer function at 100 cycles/mm all reach ∼0.4 with a ±5° field of view for 3 and 5 mm pupils.

5.
Appl Opt ; 58(18): 5040-5044, 2019 Jun 20.
Artigo em Inglês | MEDLINE | ID: mdl-31503824

RESUMO

This paper describes a new type of multifacet echelle grating (MFEG) for use in an echelle spectrometer. This new type of echelle grating broadens the spectral distribution on the spectral plane. We built a geometric model of MFEG to analyze the influence of the blaze angle and number of facet shapes on the spectral evolution. A dual-facet echelle grating and a four-facet echelle grating with different parameters were fabricated by rotating ion-beam etching with a self-shadowing rotating mask, based on the existing single-facet echelle grating (SFEG) with a line density of 52.7 g/mm and a blaze angle of 63.5°. The distributions of diffraction efficiency for different orders were measured with a He-Ne laser (632.8 nm); furthermore, these echelle gratings were applied in an echelle spectrometer (ICP-OES, Plasma2000), and testing spectra were obtained. The experimental results demonstrate that the MFEG can broaden the intensity distribution on the spectral plane, overcoming the weak spectral margin signal of SFEG spectrometers.

6.
ACS Appl Mater Interfaces ; 15(37): 44364-44372, 2023 Sep 20.
Artigo em Inglês | MEDLINE | ID: mdl-37668259

RESUMO

Metal-organic frameworks (MOFs) with well-defined porous structures and highly active frameworks are considered as promising electrode materials for sodium-ion batteries (SIBs). However, the structure pulverization upon sodiation/desodiation impacts on their practical application in SIBs. To address this issue, poly(p-phenylenediamine) (PPA) was uniformly coated onto the surface of MIL-88A, a typical Fe-based MOF through in situ polymerization initiated by the metal ions (Fe3+) of MIL-88A. Used as an anode material for SIBs, the PPA-coated MIL-88A, denoted as PPA@MIL-88A, showed significantly improved electrochemical performance. A reversible capacity as high as 230 mAh g-1 was achieved at 0.2 A g-1 even after 500 cycles. MIL-88A constructed with electrochemically active Fe3+ and fumaric acid ligands guarantees the high specific capacity, while the PPA polymer coating effectively inhibits the pulverization of MIL-88A. This work provides an efficient strategy for improving the structure and cycling stability of MOFs-based electrode materials.

7.
ACS Nano ; 16(4): 6906-6915, 2022 Apr 26.
Artigo em Inglês | MEDLINE | ID: mdl-35417134

RESUMO

Rechargeable aqueous zinc-ion batteries (ZIBs) have attracted extensive attention due to their low cost and high safety. However, the critical issues of dendrite growth and side reactions on the Zn metal anode hinder the commercialization of ZIBs. Herein, we demonstrated that the formation of Zn4SO4(OH)6·5H2O byproducts is closely relevant to the direct contact between the Zn electrode and SO42-/H2O. On the basis of this finding, we developed a cation-exchange membrane of perfluorosulfonic acid (PFSA) coated on the Zn surface to regulate the Zn plating/stripping behavior. Importantly, the PFSA film with abundant sulfonic acid groups could simultaneously block the access of SO42- and H2O, accelerate the Zn2+ ion transport kinetics, and uniformize the electrical and Zn2+ ion concentration field on the Zn surface, thus achieving a highly reversible Zn plating/stripping process with corrosion-free and dendrite-free behavior. Consequently, the PFSA-modified Zn anode exhibits high reversibility with 99.5% Coulombic efficiency and excellent plating/stripping stability (over 1500 h), subsequently enabling a highly rechargeable Zn-MnO2 full cell. The strategy of the cation-exchange membrane proposed in this work provides a simple but efficient method for suppression of side reactions.

8.
Adv Sci (Weinh) ; 9(6): e2104866, 2022 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-34990090

RESUMO

Rechargeable aqueous Zn-ion batteries (ZIBs) are regarded as one of the most promising devices for the next-generation energy storage system. However, the uncontrolled dendrite growth on Zn metal anodes and the side hydrogen evolution reaction, which has not yet been well considered, hinder the practical application of these batteries. Herein, a uniform and robust metallic Sb protective layer is designed based on the theoretic calculation and decorated on Zn plate via in situ replacement reaction. Compared with the bare Zn plate, the as-prepared Zn@Sb electrode provides abundant zincophilic sites for Zn nucleation, and homogenizes the electric field around the Zn anode surface, both of which promote the uniform Zn deposition to achieve a dendrite-free morphology. Moreover, the Gibbs free energy (∆GH ) calculation and in situ characterization demonstrate that hydrogen evolution reaction can be effectively suppressed by the Sb layer. Consequently, Sb-modified Zn anodes exhibit an ultralow voltage hysteresis of 34 mV and achieve excellent cycling stability over 1000 h with hydrogen- and dendrite-free behaviors. This work provides a facile and effective strategy to suppress both hydrogen evolution reaction and dendrite growth.

9.
Front Med (Lausanne) ; 7: 409, 2020.
Artigo em Inglês | MEDLINE | ID: mdl-32754610

RESUMO

Objective: The aim of the study was to analyze the characteristics of renal function in patients diagnosed with COVID-19. Methods: In this retrospective, single-center study, we included all confirmed cases of COVID-19 in a tertiary hospital in Guangdong, China from January 20, 2020 to March 20, 2020. Blood and urine laboratory findings related to renal function were summarized, and the estimated glomerular filtration rate (eGFR) and endogenous creatinine clearance (Ccr) were also calculated to assess the renal function. Results: A total of 12 admitted hospital patients were diagnosed with COVID-19, included 3 severe cases, and 9 common cases. Serum creatinine (Scr) was not abnormally elevated in all of the patients, and blood urea nitrogen (BUN) was abnormally elevated in only 25.0% of the patients. However, compared with the recovery period, the patient's Scr and BUN increased significantly in peak of disease (p-scr = 0.002 & p-bun < 0.001). By observing the fluctuations in Scr and BUN from admission to recovery, it was found that the peak of Scr and BUN appeared within the first 14 day of the course of the disease. Urinary microprotein detection indicated that the abnormally elevated rates of urine microalbumin (UMA), α1-microglobulin (A1M), urine immunoglobulin-G (IGU), and urine transferring (TRU) standardized by urinary creatinine in peak of disease were 41.7, 41.7, 50.0, and 16.7%, respectively. The abnormal rates of the calculated eGFR and Ccr were 66.7 and 41.7%. Conclusion: Scr and BUN were generally increased during the course of COVID-19. Detection of urinary microproteins and application of multiple indicators assessment could be helpful for discovering abnormal renal function in patients with COVID-19. However, the evidence is limited due to the small sample size and observational nature. Additional studies, especially large prospective cohort studies, are required to confirm these findings.

10.
Guang Pu Xue Yu Guang Pu Fen Xi ; 29(12): 3315-8, 2009 Dec.
Artigo em Chinês | MEDLINE | ID: mdl-20210159

RESUMO

Confocal Raman technique was used to investigate the structure changes of the ZnSO4 droplets deposited on Teflon substrate in the efflorescence process at the molecular level. Upon decreasing the relative humidity (RH), the symmetric stretching band (upsilon1-SO4(2-)) of ZnSO4 droplet blue shifted from 981 cm(-1) gradually to 987, 998 and 1,008 cm(-1), respectively, indicating that the free SO4(2-) ion associates with Zn2+ ion as the solution concentration increases and forms various contact ion pairs (CIPs), i. e., monodentate, bidentate and complicated multidentate chain-structured or web-structured CIPs. Accordingly, two obvious transition points were also observed in the hygroscopic curve of ZnSO4 droplet, implying the structure transformations in the droplet. In order to obtain the information about the contents and evolutions of various components in the droplets, curve fitting technique was used to extract the components at positions of 981, 987, 998 and 1,008 cm(-1) in the spectral range of 945-1 065 cm(-1) representing the free SO4(2-) ion, monodentate, bidentate and complicated CIPs, respectively. The results indicated that the main component in droplets was free hydrated SO4(2-) ion at high RHs. With decreasing the RH, monodentate and bidentate CIPs were formed by Zn2+ and SO4(2-) and achieved their highest contents at RHs of 66% to 34%, respectively. Further decreasing the RH, the monodentate and bidentate CIPs gradually changed into multidentate chain-structured CIPs or complicated CIPs webs, which became the main components in supersaturated ZnSO4 droplets as the RH decreased below 34%.

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