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1.
J Am Chem Soc ; 146(32): 22257-22265, 2024 Aug 14.
Artículo en Inglés | MEDLINE | ID: mdl-39013600

RESUMEN

The electrode-electrolyte interface governs the kinetics and reversibility of all electrochemical processes. While theoretical models can calculate and simulate the structure and associated properties of this intriguing component, their validation by direct experimental measurement has been a long-standing challenge. Electrocapillarity is a classical technique that derives the interfacial structure through potential-dependent surface tensions, but its limited resolution has confined its application to ideal systems such as extremely diluted aqueous electrolytes. In this work, we revive this technique with unprecedented time resolution, which allows fast and precise extraction of intrinsic interfacial structure and properties for a wide spectrum of electrolytes, be it ideal or nonideal, aqueous or nonaqueous, dilute or superconcentrated. For the very first time, this new electrocapillarity enables the measurements of a set of interfacial quantities, such as ion concentration distribution and potential drop across Helmholtz planes. Applying it on Zn-battery electrolytes, we discovered that Cl- specific adsorption at the inner-Helmholtz plane results in unexpected Zn2+ aggregation at the outer-Helmholtz plane, and identified such a unique interfacial structure as the fundamental driving force for fast Zn deposition/stripping kinetics and crystallographic texturing. The renaissance of electrocapillarity brings a new tool to the understanding and design of new electrolytes for future battery systems.

2.
J Am Chem Soc ; 2024 Jun 07.
Artículo en Inglés | MEDLINE | ID: mdl-38847794

RESUMEN

Traditional Li-ion intercalation chemistry into graphite anodes exclusively utilizes the cointercalation-free or cointercalation mechanism. The latter mechanism is based on ternary graphite intercalation compounds (t-GICs), where glyme solvents were explored and proved to deliver unsatisfactory cyclability in LIBs. Herein, we report a novel intercalation mechanism, that is, in situ synthesis of t-GIC in the tetrahydrofuran (THF) electrolyte via a spontaneous, controllable reaction between binary-GIC (b-GIC) and free THF molecules during initial graphite lithiation. The spontaneous transformation from b-GIC to t-GIC, which is different from conventional cointercalation chemistry, is characterized and quantified via operando synchrotron X-ray and electrochemical analyses. The resulting t-GIC chemistry obviates the necessity for complete Li-ion desolvation, facilitating rapid kinetics and synchronous charge/discharge of graphite particles, even under high current densities. Consequently, the graphite anode demonstrates unprecedented fast charging (1 min), dendrite-free low-temperature performance, and ultralong lifetimes exceeding 10 000 cycles. Full cells coupled with a layered cathode display remarkable cycling stability upon a 15 min charging and excellent rate capability even at -40 °C. Furthermore, our chemical strategies are shown to extend beyond Li-ion batteries to encompass Na-ion and K-ion batteries, underscoring their broad applicability. Our work contributes to the advancement of graphite intercalation chemistry and presents a low-cost, adaptable approach for achieving fast-charging and low-temperature batteries.

3.
Nat Commun ; 15(1): 5066, 2024 Jun 13.
Artículo en Inglés | MEDLINE | ID: mdl-38871716

RESUMEN

With the rapid increase in lithium consumption for electric vehicle applications, its price soared during the past decade. To secure a reliable and cost-effective supply chain, it is critical to unlock alternative lithium extraction resources beyond conventional brine. In this study, we develop an electrochemical method to directly leach lithium from α-phase spodumene. We find the H2O2 promoter can significantly reduce the leaching potential by facilitating the electron transfer and changing the reaction path. Upon leaching, ß-phase spodumene shows a typical phase transformation to HAlSi2O6, while leached α-phase remains its original crystal phase with a lattice shrinkage. To demonstrate the scale-up potential of electrochemical leaching, we design a catalyst-modified high-throughput current collector for high loading of suspended spodumene, achieving a leaching current of 18 mA and a leaching efficiency of 92.2%. Electrochemical leaching will revolutionize traditional leaching and recycling processes by minimizing the environmental footprint and energy consumption.

4.
Artículo en Inglés | MEDLINE | ID: mdl-37549074

RESUMEN

Fabric-based pneumatic actuators (FPAs) are extensively employed in the design of lightweight and compliant soft wearable assistive gloves. However, conventional FPAs typically exhibit limited output force, thereby restricting the applications of such gloves. This paper presents the development of a novel honeycomb pneumatic actuator (HPA) constructed using flexible thermoplastic polyurethane (TPU) coating through hot pressing or ultrasonic welding techniques. Compared to the previously utilized double-layer fabric-based pneumatic actuators (DLFPAs), the HPAs yields a remarkable 862% increase in end output force. It can produce a tip force of 13.57 N at a pressure of 150 kPa. The integration of HPAs onto a soft pneumatic glove enables the facilitation of various activities of daily living. A series of trials involving nine patients were conducted to assess the effectiveness of the soft glove. The experimental results indicate that when assisted by the glove, the patients' finger metacarpophalangeal (MCP) and proximal interphalangeal (PIP) joints achieved angles of 87.67 ± 19.27° and 64.2 ± 30.66°, respectively. Additionally, the average fingertip force reached 10.16 ± 4.24 N, the average grip force reached 26.04 ± 15.08 N, and the completion rate of daily functions for the patients increased from 39% to 76%. These outcomes demonstrate that the soft glove effectively aids in finger movements and significantly enhances the patients' daily functioning.


Asunto(s)
Dispositivo Exoesqueleto , Robótica , Humanos , Actividades Cotidianas , Diseño de Equipo , Dedos
5.
J Glob Antimicrob Resist ; 30: 199-204, 2022 09.
Artículo en Inglés | MEDLINE | ID: mdl-35618209

RESUMEN

OBJECTIVES: This study aimed to investigate the annual incidence, molecular epidemiological characteristics, and antimicrobial resistance of group A Streptococcus (GAS) clinical isolates from paediatric patients at Shenzhen Children's Hospital during 2016-2020. METHODS: Clinical samples were collected from paediatric patients with a suspected diagnosis of GAS infections. We studied the annual incidence and characteristics of GAS infections using the GAS antigen detection method. Additionally, 250 GAS isolates were randomly selected for genotyping of the emm gene, and antimicrobial susceptibility assay was performed using the Kirby-Bauer paper dispersion strategy. RESULTS: Among 43 593 collected samples, 9313 were positive for the GAS antigen. The main emm type was emm12, followed by emm1, emm6, and emm 4, which were used for distinguishing 90% of the scarlet fever isolated strains. The percentage of emm1 increased from 36% in 2016 to 44% in 2019, whereas the percentage of emm12 decreased from 62% to 50%. Several unusual emm types isolated from scarlet fever patients showed an increase in proportions from 2016 to 2020. These GAS isolates were sensitive to penicillin, ceftriaxone, and vancomycin and were highly resistant to erythromycin and clindamycin. CONCLUSION: There was a high incidence of GAS infections during 2016-2020 in Shenzhen, China. The GAS isolates had a high resistance rate to erythromycin and clindamycin; penicillin was the antibiotic of choice for GAS infections. The common emm types were emm12 and emm1. Future studies should investigate the clonal structure and superantigen profiles of the population of GAS isolates associated with scarlet fever.


Asunto(s)
Escarlatina , Infecciones Estreptocócicas , Antibacterianos/farmacología , Antibacterianos/uso terapéutico , Antígenos Bacterianos/genética , Proteínas de la Membrana Bacteriana Externa/genética , Proteínas Portadoras/genética , Niño , China/epidemiología , Clindamicina , Eritromicina , Humanos , Pruebas de Sensibilidad Microbiana , Penicilinas , Prevalencia , Escarlatina/epidemiología , Infecciones Estreptocócicas/tratamiento farmacológico , Infecciones Estreptocócicas/epidemiología , Streptococcus pyogenes/genética
6.
Nanoscale Adv ; 3(23): 6580-6586, 2021 Nov 24.
Artículo en Inglés | MEDLINE | ID: mdl-36132663

RESUMEN

Photocatalysts with a direct Z-scheme heterojunction are promising by virtue of the effectively enhanced separation of charge carriers, high retention of redox ability and the absence of backward photocatalytic reactions. Their activity depends on band alignment and interfacial configurations between two semiconductors for charge carrier kinetics and the effective active sites for photochemical reactions. Herein, a two-dimensional (2D) graphitic carbon nitride/N-doped carbon (C3N4/NC) photocatalyst is synthesized by a gas template (NH4Cl)-assisted thermal condensation method. C3N4/NC has the synthetic merits of a direct Z-scheme heterojunction, 2D-2D interfacial contact, and enhanced specific surface area to improve charge separation kinetics and provide abundant active sites for photochemical reaction. It exhibits an over 46-fold increase of the photocatalytic hydrogen production rate compared to bulk C3N4 under visible light illumination. This work demonstrates the great potential of 2D Z-scheme heterojunctions for photocatalysis and will inspire more related work in the future.

7.
Sci Rep ; 6: 26890, 2016 06 01.
Artículo en Inglés | MEDLINE | ID: mdl-27248510

RESUMEN

Fiber shaped supercapacitors are promising candidates for wearable electronics because they are flexible and light-weight. However, a critical challenge of the widespread application of these energy storage devices is their low cell voltages and low energy densities, resulting in limited run-time of the electronics. Here, we demonstrate a 1.5 V high cell voltage and high volumetric energy density asymmetric fiber supercapacitor in aqueous electrolyte. The lightweight (0.24 g cm(-3)), highly conductive (39 S cm(-1)), and mechanically robust (221 MPa) graphene fibers were firstly fabricated and then coated by NiCo2S4 nanoparticles (GF/NiCo2S4) via the solvothermal deposition method. The GF/NiCo2S4 display high volumetric capacitance up to 388 F cm(-3) at 2 mV s(-1) in a three-electrode cell and 300 F cm(-3) at 175.7 mA cm(-3) (568 mF cm(-2) at 0.5 mA cm(-2)) in a two-electrode cell. The electrochemical characterizations show 1000% higher capacitance of the GF/NiCo2S4 as compared to that of neat graphene fibers. The fabricated device achieves high energy density up to 12.3 mWh cm(-3) with a maximum power density of 1600 mW cm(-3), outperforming the thin-film lithium battery. Therefore, these supercapacitors are promising for the next generation flexible and wearable electronic devices.

8.
Bing Du Xue Bao ; 24(1): 28-33, 2008 Jan.
Artículo en Zh | MEDLINE | ID: mdl-18320819

RESUMEN

The tracheal aspirates and serum samples of a suspected human case of high-pathogenic avian influenza (firstly found in Shenzhen, China) were collected and tested by a series of assays. The results showed that the RNA extracted from the tracheal aspirate specimens of the patient was confirmed positive for H5N1 avian influenza virus by Real-time PCR. The H5N1 avian influenza virus was isolated from patient's tracheal aspirates on MDCK cell and was named A/Guangdong/2/06(H5N1). The viral load of tracheal aspirates collected at different time points were detected by Real-time PCR. The virus microneutralization and the antigenic ratio of human H5N1 isolated were also assayed. It was found that when the virus load decreased gradually after the disease onset, the serum neutralizing antibody titer in the patient increased to 1 : 160 and subsequently decreased gradually. By molecular analysis, the eight gene segments of A/Guangdong/2/06 revealed to be similar to that of H5N1 avian influenza viruses isolated from south China in 2005-2006. However, there were obvious differences in the gene sequence of the detected H5N1 viral RNA as compared with that of the strains isolated from Vietnam, Thailand and Indonesia.


Asunto(s)
Subtipo H5N1 del Virus de la Influenza A/genética , Gripe Humana/virología , Adulto , Secuencia de Aminoácidos , Anticuerpos Antivirales/sangre , Humanos , Subtipo H5N1 del Virus de la Influenza A/inmunología , Subtipo H5N1 del Virus de la Influenza A/aislamiento & purificación , Gripe Humana/diagnóstico , Masculino , Datos de Secuencia Molecular , Mutación , Pruebas de Neutralización , ARN Viral/sangre
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