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1.
J Am Chem Soc ; 146(21): 14593-14599, 2024 May 29.
Artigo em Inglês | MEDLINE | ID: mdl-38718194

RESUMO

Twisted moiré superlattice is featured with its moiré potential energy, the depth of which renders an effective approach to strengthening the exciton-exciton interaction and exciton localization toward high-performance quantum photonic devices. However, it remains as a long-standing challenge to further push the limit of moiré potential depth. Herein, owing to the pz orbital induced band edge states enabled by the unique sp-C in bilayer γ-graphdiyne (GDY), an ultradeep moiré potential of ∼289 meV is yielded. After being twisted into the hole-to-hole layer stacking configuration, the interlayer coupling is substantially intensified to augment the lattice potential of bilayer GDY up to 475%. The presence of lateral constrained moiré potential shifts the spatial distribution of electrons and holes in excitons from the regular alternating mode to their respective separated and localized mode. According to the well-established wave function distribution of electrons contained in excitons, the AA-stacked site is identified to serve for exciton localization. This work extends the materials systems available for moiré superlattice design further to serial carbon allotropes featured with benzene ring-alkyne chain coupling, unlocking tremendous potential for twistronic-based quantum device applications.

2.
Chem Rev ; 122(23): 17155-17239, 2022 12 14.
Artigo em Inglês | MEDLINE | ID: mdl-36239919

RESUMO

The ever-increasing demand for flexible and portable electronics has stimulated research and development in building advanced electrochemical energy devices which are lightweight, ultrathin, small in size, bendable, foldable, knittable, wearable, and/or stretchable. In such flexible and portable devices, semi-solid/solid electrolytes besides anodes and cathodes are the necessary components determining the energy/power performances. By serving as the ion transport channels, such semi-solid/solid electrolytes may be beneficial to resolving the issues of leakage, electrode corrosion, and metal electrode dendrite growth. In this paper, the fundamentals of semi-solid/solid electrolytes (e.g., chemical composition, ionic conductivity, electrochemical window, mechanical strength, thermal stability, and other attractive features), the electrode-electrolyte interfacial properties, and their relationships with the performance of various energy devices (e.g., supercapacitors, secondary ion batteries, metal-sulfur batteries, and metal-air batteries) are comprehensively reviewed in terms of materials synthesis and/or characterization, functional mechanisms, and device assembling for performance validation. The most recent advancements in improving the performance of electrochemical energy devices are summarized with focuses on analyzing the existing technical challenges (e.g., solid electrolyte interphase formation, metal electrode dendrite growth, polysulfide shuttle issue, electrolyte instability in half-open battery structure) and the strategies for overcoming these challenges through modification of semi-solid/solid electrolyte materials. Several possible directions for future research and development are proposed for going beyond existing technological bottlenecks and achieving desirable flexible and portable electrochemical energy devices to fulfill their practical applications. It is expected that this review may provide the readers with a comprehensive cross-technology understanding of the semi-solid/solid electrolytes for facilitating their current and future researches on the flexible and portable electrochemical energy devices.


Assuntos
Fontes de Energia Elétrica , Eletrólitos , Eletrodos , Eletrônica , Software
3.
Angew Chem Int Ed Engl ; 62(22): e202302640, 2023 May 22.
Artigo em Inglês | MEDLINE | ID: mdl-36964969

RESUMO

The advent of wearable electronics has strongly stimulated advanced research into the exploration of flexible zinc-air batteries (ZABs) with high theoretical energy density, high inherent safety, and low cost. However, the half-open battery structure and the high concentration of alkaline aqueous environment pose great challenges on the electrolyte retention capability and the zinc anode stability. Herein, a starch-based superabsorbent hydrogel polymer electrolyte (SSHPE) with high ionic conductivity, electrolyte absorption and retention capabilities, strong alkaline resistance and high zinc anode stability has been designed and applied in ZABs. Experimental and calculational analyses probe into the root of the superiority of SSHPEs, confirming the significance of the carboxyl functional groups along their polymer chains. These features endow the as-fabricated ZAB a long cycle life of 300 h, much longer than that with commonly used poly(vinyl alcohol)-based electrolyte.

4.
Adv Mater ; 35(7): e2209290, 2023 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-36455877

RESUMO

Increasing pursuit of next-generation wearable electronics has put forward the demand of reliable energy devices with high flexibility, durability, and enhanced electrochemical performances. Flexible aqueous zinc-air batteries (FAZABs) have attracted great interests owing to the high energy density, safety, and environmental benignity, for which quasi-solid-state gel polymer electrolytes (QSGPEs) are state-of-the-art electrolytes with high ionic conductivity, flexibility, and resistance to leakage problems of traditional liquid electrolytes. Compared to commonly used PVA-KOH electrolyte with poor electrolyte retention capability and cycling stability, a new type of sulfonate functionalized nanocomposite QSGPE is applied in FAZABs with high ionic conductivity, strong alkaline tolerance, and high zinc anode stability. Notably, the existence of (1) strong anionic sulfonate groups of QSGPEs, contributing to the exposure of preferred Zn (002) plane that is more resistant to zinc dendrite formation, and (2) nano-attapulgite electrolyte additives, beneficial for the enhancement of ionic conductivity, electrolyte uptake, and retention capability, endows a ultralong cycling life of 450 h for the fabricated FAZAB. Furthermore, flexible energy belts and knittable energy wires fabricated with a series/parallel unit of several FAZABs can be used to power various wearable electronics.

5.
ACS Appl Mater Interfaces ; 14(51): 56856-56866, 2022 Dec 28.
Artigo em Inglês | MEDLINE | ID: mdl-36528818

RESUMO

Zinc-nickel batteries are promising competitors for next-generation power supply due to their benefits of high safety, high working voltage, and attractive rate performance. However, their practical applications are plagued by their poor cycling performance, stemming from uneven redistribution of zinc during cycling that results in dendrite formation and shape changes of the electrode. In this work, mesoporous Ti4O7 microspheres are prepared and are employed as additives of a zinc anode. Notably, the presence of mesopores provides abundant chemisorption sites for Zn(OH)42- ions, inhibiting severe zinc redistribution in the electrode. Moreover, due to the good electrical conductivity and mesopores that serve as ion diffusion channels, the reaction reactivity and reversibility of the zinc electrode are greatly facilitated. As a result, the fabricated zinc-nickel battery with mesoporous Ti4O7 additives (ms-Ti4O7) exhibits an enhanced discharge capacity and a significantly prolonged cycling life. Even at a current of 10 A (∼138 mA cm-2), the ms-Ti4O7-modified anode demonstrates stable operation for longer than 718 h (700 cycles) with a discharge voltage of 1.2 V, which is much longer than those of a ZnO anode (192 h, 117 cycles) and a Ti4O7-particle (p-Ti4O7)-modified battery (590 h, 443 cycles). Furthermore, due to the anchoring effect for Zn(OH)42- and the uniform electric field, the effect of mesoporous Ti4O7 on inhibiting dendrite formation and shape change of the zinc electrode is highlighted.

6.
Artigo em Inglês | MEDLINE | ID: mdl-35103471

RESUMO

Because of their high theoretical value of volumetric energy density, excellent rate performance, and high level of safety, zinc-nickel batteries (ZNBs) show potential applications for uninterrupted power supply (UPS) systems. However, despite all the advantages of ZNBs, the commercial application of ZNBs has been prevented by their short lifetime caused by the shape change, the corrosion, and the dendrite formation of the Zn anode. In this work, we proposed a flexible and durable potassium polyacrylate (PAAK)-KOH gel polymer electrolyte (GPE) prepared in a very simple way to solve the above problems of the Zn anode. The obtained highly porous gel electrolyte showed higher water retention, satisfying ionic conductivity (0.918 S cm-1), and a broad electrochemical stable voltage window. By providing a stable and homogeneous electrode/electrolyte interface for the Zn anode, the gel electrolyte can inhibit the uneven deposition and dendrite formation. As a result, the gel electrolyte greatly prolonged the cycling life to 776 h. In addition, because of the considerably batter corrosion resistance of the Zn anode in the PAAK-KOH GPE, the ZNB with gel electrolyte also exhibited a superior shelf life of more than 431 h and a superior cycling performance under float charge for more than 400 h at 60 °C. This work demonstrates that the gel electrolyte with a simple preparation method is suitable for large-scale practical production and can be successfully used in Zn-Ni batteries as an electrolyte exhibiting excellent performance.

7.
Atherosclerosis ; 362: 47-55, 2022 12.
Artigo em Inglês | MEDLINE | ID: mdl-36347649

RESUMO

BACKGROUND AND AIMS: Choline has been shown to exert atherogenic effects in Apoe-/- and Ldlr-/- mice, related to its conversion by gut bacteria into trimethylamine (TMA) that is converted by the liver into the proinflammatory metabolite trimethylamine-N-oxide (TMAO). Since butyrate beneficially modulates the gut microbiota and has anti-inflammatory and antiatherogenic properties, the aim of the present study was to investigate whether butyrate can alleviate choline-induced atherosclerosis. To this end, we used APOE*3-Leiden.CETP mice, a well-established atherosclerosis-prone model with human-like lipoprotein metabolism. METHODS: Female APOE*3-Leiden.CETP mice were fed an atherogenic diet alone or supplemented with choline, butyrate or their combination for 16 weeks. RESULTS: Interestingly, choline protected against fat mass gain, increased the abundance of anti-inflammatory gut microbes, and increased the expression of gut microbial genes involved in TMA and TMAO degradation. Butyrate similarly attenuated fat mass gain and beneficially modulated the gut microbiome, as shown by increased abundance of anti-inflammatory and short chain fatty acid-producing microbes, and inhibited expression of gut microbial genes involved in lipopolysaccharide synthesis. Both choline and butyrate upregulated hepatic expression of flavin-containing monooxygenases, and their combination resulted in highest circulating TMAO levels. Nonetheless, choline, butyrate and their combination did not influence atherosclerosis development, and TMAO levels were not associated with atherosclerotic lesion size. CONCLUSIONS: While choline and butyrate have been reported to oppositely modulate atherosclerosis development in Apoe-/- and Ldlr-/- mice as related to changes in the gut microbiota, both dietary constituents did not affect atherosclerosis development while beneficially modulating the gut microbiome in APOE*3-Leiden.CETP mice.


Assuntos
Aterosclerose , Butiratos , Colina , Microbioma Gastrointestinal , Animais , Feminino , Camundongos , Apolipoproteínas E/genética , Aterosclerose/genética , Aterosclerose/prevenção & controle , Aterosclerose/metabolismo , Butiratos/farmacologia , Proteínas de Transferência de Ésteres de Colesterol/genética , Colina/farmacologia , Metilaminas/metabolismo , Camundongos Endogâmicos C57BL , Camundongos Knockout para ApoE
8.
Adv Mater ; 33(31): e2006461, 2021 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-34050684

RESUMO

Electrically rechargeable zinc-air batteries (ERZABs) have attracted substantial research interest as one of the best candidate power sources for electric vehicles, grid-scale energy storage, and portable electronics owing to their high theoretical capacity, low cost, and environmental benignity. However, the realization of ERZABs with long cycle life and high energy and power densities is still a considerable challenge. The electrolyte, which serves as the ionic conductor, is one of the core components of ERZABs, as it plays a significant role during the discharge-charge process and greatly influences the rechargeability, operating voltage, lifespan, power density, and safety of ERZABs. Herein, the fundamental electrochemistry of electrolyte materials for ERZABs and the associated challenges are presented. Furthermore, recent advances in electrolyte materials for ERZABs, including alkaline aqueous electrolytes, nonalkaline electrolytes, ionic liquids, and semisolid-state electrolytes are discussed. This work aims to provide insights into the future exploration of high-performance electrolytes and thus promote the development of ERZABs.

9.
MethodsX ; 7: 100973, 2020.
Artigo em Inglês | MEDLINE | ID: mdl-32637342

RESUMO

Zinc-air batteries are considered as the promising alternative to conventional power sources and have received revived research efforts recently due to their high energy density, good safety, environmental friendliness, and potential for low material costs. The design and production of zinc-air batteries is critical to accelerate the commercialization for extending the application range. Herein, we proposed a method for producing plate-type primary zinc-air batteries which apply zinc foil as an example. The proposed method includes the design of an easily assembled zinc-air battery configuration, the preparation of air cathodes and assembly of zinc-air battery. In addition, the galvanostatic discharge performance of the assembled non-flow primary zinc-air battery was tested at a current density of 10 mA cm-2. The method can be applied for the production of commercial zinc-air batteries for laboratory research and industrial manufacture for electric vehicles, consumer electronics, and energy storage devices.•The preparation method for components of zinc-air battery configuration and air cathodes was developed.•The assembly of the zinc-air battery was proposed.•Direct evaluation of discharge performance of the zinc-air batteries produced by the method.

10.
Front Chem ; 7: 678, 2019.
Artigo em Inglês | MEDLINE | ID: mdl-31696103

RESUMO

Next-generation wearable and portable electronic devices require the development of flexible energy-storage devices with high energy density and low cost. Over the past few decades, flexible zinc-air batteries (FZABs), characterized by their extremely high theoretical energy density from consuming oxygen in air and low cost, have been regarded as one of the most promising power supplies. However, their unique half-open structure poses great challenges for the environmental stability of their components, including the electrolyte and electrodes. As an important ionic conductor, the poly(vinyl alcohol) (PVA)-KOH gel polymer electrolyte (GPE) has been widely utilized in FZABs. To date, most studies have focused on investigations of the electrode, electrocatalyst materials and battery configuration, while very few have paid attention to the influence of the environment on the electrolyte and the corresponding FZAB performance. Herein, for the first time, the environmental stability of PVA-KOH GPE, such as dimensional stability and water and ionic conductivity retention capability, for FZABs in ambient air has been thoroughly studied. Moreover, the properties of the assembled FZABs in terms of cycling stability, discharge performance and power output are investigated. This report aims to play a leading role in examining the environmental stability of electrolytes in FZABs, which is critical for their practical applications.

11.
ACS Appl Mater Interfaces ; 11(32): 28909-28917, 2019 Aug 14.
Artigo em Inglês | MEDLINE | ID: mdl-31318523

RESUMO

Flexible zinc-air batteries (ZABs) have been considered as one of the most outstanding energy storage devices for flexible and portable electronics because of their superior energy density and environmental friendliness. As the "blood" of flexible ZABs, electrolytes play a significant role in determining their performance, such as discharge working time, cycling property, and shelf life. Herein, a novel polymer electrolyte based on quaternary ammonium hydroxides is first applied in flexible zinc-air batteries. Tetraethylammonium hydroxide (TEAOH) is innovatively used as the ionic conductor with poly(vinyl alcohol) (PVA) as the polymer host in the polymer electrolyte and exhibits a good water retention capability, resulting in not only a good shelf life but also a good working life of the flexible zinc-air batteries. The fabricated polymer electrolyte maintains its high ionic conductivity of 30 mS cm-1 even after 2 weeks. In addition, the as-assembled zinc-air batteries based on the TEAOH-PVA electrolyte exhibit excellent discharge performance and cycling life compared to those based on the commonly used KOH-PVA electrolyte, and no notable degradation is observed after 2 weeks. Furthermore, flexible TEAOH-PVA-based zinc-air batteries can power a light-emitting diode (LED) electronic watch, a mobile phone, and an LED screen, indicating the very large potential of the high-performance zinc-air batteries that are safe, cost-effective, and remarkably flexible.

12.
ACS Appl Mater Interfaces ; 9(22): 18856-18864, 2017 Jun 07.
Artigo em Inglês | MEDLINE | ID: mdl-28516779

RESUMO

A new approach has been developed for in situ preparing cubic-shaped Pt particles with (100) preferential orientation on the surface of the conductive support by using a quick, one-step, and clean electrochemical method with periodic square-wave potential. The whole electrochemical deposition process is very quick (only 6 min is required to produce cubic Pt particles), without the use of particular capping agents. The shape and the surface structure of deposited Pt particles can be controlled by the lower and upper potential limits of the square-wave potential. For a frequency of 5 Hz and an upper potential limit of 1.0 V (vs saturated calomel electrode), as the lower potential limit decreases to the H adsorption potential region, the Pt deposits are changed from nearly spherical particles to cubic-shaped (100)-oriented Pt particles. High-resolution transmission electron microscopy and selected-area electron diffraction reveal that the formed cubic Pt particles are single-crystalline and enclosed by (100) facets. Cubic Pt particles exhibit characteristic H adsorption/desorption peaks corresponding to the (100) preferential orientation. Ge irreversible adsorption indicates that the fraction of wide Pt(100) surface domains is 47.8%. The electrocatalytic activities of different Pt particles are investigated by ammonia electro-oxidation, which is particularly sensitive to the amount of Pt(100) sites, especially larger (100) domains. The specific activity of cubic Pt particles is 3.6 times as high as that of polycrystalline spherical Pt particles, again confirming the (100) preferential orientation of Pt cubes. The formation of cubic-shaped Pt particles is related with the preferential electrochemical deposition and dissolution processes of Pt, which are coupled with the periodic desorption and adsorption processes of O-containing species and H adatoms.

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