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1.
Nat Commun ; 11(1): 606, 2020 Jan 30.
Artigo em Inglês | MEDLINE | ID: mdl-32001696

RESUMO

Manipulating liquids with tunable shape and optical functionalities in real time is important for electroactive flow devices and optoelectronic devices, but remains a great challenge. Here, we demonstrate electrotunable liquid sulfur microdroplets in an electrochemical cell. We observe electrowetting and merging of sulfur droplets under different potentiostatic conditions, and successfully control these processes via selective design of sulfiphilic/sulfiphobic substrates. Moreover, we employ the electrowetting phenomena to create a microlens based on the liquid sulfur microdroplets and tune its characteristics in real time through changing the shape of the liquid microdroplets in a fast, repeatable, and controlled manner. These studies demonstrate a powerful in situ optical battery platform for unraveling the complex reaction mechanism of sulfur chemistries and for exploring the rich material properties of the liquid sulfur, which shed light on the applications of liquid sulfur droplets in devices such as microlenses, and potentially other electrotunable and optoelectronic devices.

2.
Adv Sci (Weinh) ; 7(2): 1903603, 2020 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-31993298

RESUMO

[This corrects the article DOI: 10.1002/advs.201800981.].

3.
Nat Nanotechnol ; 2020 Jan 27.
Artigo em Inglês | MEDLINE | ID: mdl-31988508

RESUMO

It has recently been shown that sulfur, a solid material in its elementary form S8, can stay in a supercooled state as liquid sulfur in an electrochemical cell. We establish that this newly discovered state could have implications for lithium-sulfur batteries. Here, through in situ studies of electrochemical sulfur generation, we show that liquid (supercooled) and solid elementary sulfur possess very different areal capacities over the same charging period. To control the physical state of sulfur, we studied its growth on two-dimensional layered materials. We found that on the basal plane, only liquid sulfur accumulates; by contrast, at the edge sites, liquid sulfur accumulates if the thickness of the two-dimensional material is small, whereas solid sulfur nucleates if the thickness is large (tens of nanometres). Correlating the sulfur states with their respective areal capacities, as well as controlling the growth of sulfur on two-dimensional materials, could provide insights for the design of future lithium-sulfur batteries.

4.
Nano Lett ; 20(2): 1252-1261, 2020 Feb 12.
Artigo em Inglês | MEDLINE | ID: mdl-31887051

RESUMO

Lithium-sulfur (Li-S) batteries are promising next-generation energy storage technologies due to their high theoretical energy density, environmental friendliness, and low cost. However, low conductivity of sulfur species, dissolution of polysulfides, poor conversion from sulfur reduction, and lithium sulfide (Li2S) oxidation reactions during discharge-charge processes hinder their practical applications. Herein, under the guidance of density functional theory calculations, we have successfully synthesized large-scale single atom vanadium catalysts seeded on graphene to achieve high sulfur content (80 wt % sulfur), fast kinetic (a capacity of 645 mAh g-1 at 3 C rate), and long-life Li-S batteries. Both forward (sulfur reduction) and reverse reactions (Li2S oxidation) are significantly improved by the single atom catalysts. This finding is confirmed by experimental results and consistent with theoretical calculations. The ability of single metal atoms to effectively trap the dissolved lithium polysulfides (LiPSs) and catalytically convert the LiPSs/Li2S during cycling significantly improved sulfur utilization, rate capability, and cycling life. Our work demonstrates an efficient design pathway for single atom catalysts and provides solutions for the development of high energy/power density Li-S batteries.

5.
ACS Appl Mater Interfaces ; 11(51): 47956-47962, 2019 Dec 26.
Artigo em Inglês | MEDLINE | ID: mdl-31782303

RESUMO

A binder plays an important role in stabilizing the electrode structure and improving the cyclic stability of batteries. However, the traditional binders are no longer satisfactory in lithium-sulfur (Li-S) batteries because of their failure in accommodating the large volume changes of sulfur and trapping soluble intermediate polysulfides, thus causing severe capacity decay. In this work, we prepared a multifunctional binder for Li-S batteries by merely modifying the acacia gum (AG), a low-cost biomass polymer, with l-cysteine under mild conditions. Owing to the introduced amino and carboxyl branches by the l-cysteine, the modified AG shows enhanced polysulfide trapping ability and can effectively restrain the shuttling of polysulfides. In addition, the introduction of branches can help form a cross-linked 3D network with better mechanical strength and flexibility for adhering sulfur and accommodating the volume changes of cathode materials. As a result, compared with the normally used polyvinylidene fluoride binder and the unmodified AG binder, the l-cysteine-modified AG binder effectively enhanced the rate capability and cycling stability of the Li-S batteries directly using sulfur as the cathode, showing a promising way to prompt the practical use of Li-S batteries.

6.
Chem Rev ; 119(20): 11042-11109, 2019 Oct 23.
Artigo em Inglês | MEDLINE | ID: mdl-31566351

RESUMO

Nanomaterials provide many desirable properties for electrochemical energy storage devices due to their nanoscale size effect, which could be significantly different from bulk or micron-sized materials. Particularly, confined dimensions play important roles in determining the properties of nanomaterials, such as the kinetics of ion diffusion, the magnitude of strain/stress, and the utilization of active materials. Nanowires, as one of the representative one-dimensional nanomaterials, have great capability for realizing a variety of applications in the fields of energy storage since they could maintain electron transport along the long axis and have a confinement effect across the diameter. In this review, we give a systematic overview of the state-of-the-art research progress on nanowires for electrochemical energy storage, from rational design and synthesis, in situ structural characterizations, to several important applications in energy storage including lithium-ion batteries, lithium-sulfur batteries, sodium-ion batteries, and supercapacitors. The problems and limitations in electrochemical energy storage and the advantages in utilizing nanowires to address the issues and improve the device performance are pointed out. At the end, we also discuss the challenges and demonstrate the prospective for the future development of advanced nanowire-based energy storage devices.

7.
Adv Mater ; 31(48): e1904991, 2019 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-31549760

RESUMO

Lithium metal anodes with high energy density are important for further development of next-generation batteries. However, inhomogeneous Li deposition and dendrite growth hinder their practical utilization. 3D current collectors are widely investigated to suppress dendrite growth, but they usually occupy a large volume and increase the weight of the system, hence decreasing the energy density. Additionally, the nonuniform distribution of Li ions results in low utilization of the porous structure. A lightweight, 3D Cu nanowire current collector with a phosphidation gradient is reported to balance the lithiophilicity with conductivity of the electrode. The phosphide gradient with good lithiophilicity and high ionic conductivity enables dense nucleation of Li and its steady deposition in the porous structure, realizing a high pore utilization. Specifically, the homogenous deposition of Li leads to the formation of an oriented texture on the electrode surface at high capacities. A high mass loading (≈44 wt%) of Li with a capacity of 3 mAh cm-2 and a high average Coulombic efficiency of 97.3% are achieved. A lifespan of 300 h in a symmetrical cell is obtained at 2 mA cm-2 , implying great potential to stabilize lithium metal.

8.
Nano Lett ; 19(10): 7487-7493, 2019 10 09.
Artigo em Inglês | MEDLINE | ID: mdl-31509421

RESUMO

With the increasing strategies aimed at repressing shuttle problems in the lithium-sulfur battery, dissolved contents of polysulfides are significantly reduced. Except for solid-state Li2S2 and Li2S, aggregated phases of polysulfides remain unexplored, especially in well confined cathode material systems. Here, we report a series of nanosize polysulfide clusters and solid phases from an atomic perspective. The calculated phase diagram and formation energy evolution process demonstrate their stabilities and cohesive tendency. It is interesting to find that Li2S6 can stay in the solid state and contains short S3 chains, further leading to the unique stability and dense structure. Simulated electronic properties indicate reduced band gaps when polysulfides are aggregated, especially for solid phase Li2S6 with a band gap as low as 0.47 eV. Their dissolution behavior and conversion process are also investigated, which provides a more realistic model and gives further suggestions on the future design of the lithium-sulfur battery.

9.
Nano Lett ; 19(10): 7293-7300, 2019 10 09.
Artigo em Inglês | MEDLINE | ID: mdl-31499003

RESUMO

A variety of methods including tuning chemical compositions, structures, crystallinity, defects and strain, and electrochemical intercalation have been demonstrated to enhance the catalytic activity. However, none of these tuning methods provide direct dynamical control during catalytic reactions. Here we propose a new method to tune the activity of catalysts through solid-state ion gating manipulation and adjustment (SIGMA) using a catalysis transistor. SIGMA can electrostatically dope the surface of catalysts with a high electron concentration over 5 × 1013 cm-2 and thus modulate both the chemical potential of the reaction intermediates and their electrical conductivity. The hydrogen evolution reaction (HER) on both pristine and defective MoS2 were investigated as model reactions. Our theoretical and experimental results show that the overpotential at 10 mA/cm2 and Tafel slope can be in situ, continuously, dynamically, and reversibly tuned over 100 mV and around 100 mV/dec, respectively.

10.
Adv Sci (Weinh) ; 6(4): 1800981, 2019 Feb 20.
Artigo em Inglês | MEDLINE | ID: mdl-30828520

RESUMO

Rechargeable magnesium/sulfur (Mg/S) batteries are widely regarded as one of the alternatives to lithium-ion batteries. However, a key factor restricting their application is the lack of suitable electrolyte. Herein, an electrolyte additive that can reduce the polarization voltage is developed and 98.7% coulombic efficiency is realized. The as-prepared Mg-ion electrolyte exhibits excellent Mg plating/stripping performance with a low overpotential of 0.11 V for plating process, and high anodic stability up to 3.0 V (vs Mg/Mg2+). When it is coupled with magnesium polysulfide, which has high reactivity and is homogeneously distributed on carbon matrix, the Mg/S cells deliver a good cycling stability with a high discharge capacity over 1000 mAh g-1 for more than 50 cycles.

11.
Sci Adv ; 5(3): eaau5655, 2019 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-30899782

RESUMO

Lithium metal-based batteries are attractive energy storage devices because of high energy density. However, uncontrolled dendrite growth and virtually infinite volume change, which cause performance fading and safety concerns, have limited their applications. Here, we demonstrate that a composite lithium metal electrode with an ion-conducting mesoscale skeleton can improve electrochemical performance by locally reducing the current density. In addition, the potential for short-circuiting is largely alleviated due to side deposition of mossy lithium on the three-dimensional electroactive surface of the composite electrode. Moreover, the electrode volume only slightly changes with the support of a rigid and stable scaffold. Therefore, this mesoscale composite electrode can cycle stably for 200 cycles with low polarization under a high areal current density up to 5 mA/cm2. Most attractively, the proposed fabrication process, which only involves simple mechanical deformation, is scalable and cost effective, providing a new strategy for developing high performance and long lifespan lithium anodes.

12.
Proc Natl Acad Sci U S A ; 116(3): 765-770, 2019 01 15.
Artigo em Inglês | MEDLINE | ID: mdl-30602455

RESUMO

Supercooled liquid sulfur microdroplets were directly generated from polysulfide electrochemical oxidation on various metal-containing electrodes. The sulfur droplets remain liquid at 155 °C below sulfur's melting point (T m = 115 °C), with fractional supercooling change (T m - T sc)/T m larger than 0.40. In operando light microscopy captured the rapid merging and shape relaxation of sulfur droplets, indicating their liquid nature. Micropatterned electrode and electrochemical current allow precise control of the location and size of supercooled microdroplets, respectively. Using this platform, we initiated and observed the rapid solidification of supercooled sulfur microdroplets upon crystalline sulfur touching, which confirms supercooled sulfur's metastability at room temperature. In addition, the formation of liquid sulfur in electrochemical cell enriches lithium-sulfur-electrolyte phase diagram and potentially may create new opportunities for high-energy Li-S batteries.

13.
Nat Prod Res ; 33(8): 1122-1126, 2019 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-29607747

RESUMO

A novel, green, rapid, and precise polar RP-HPLC method has been successfully developed and screened for ectoine high-yield strain in marine bacteria. Ectoine is a polar and extremely useful solute which allows microorganisms to survive in extreme environmental salinity. This paper describes a polar-HPLC method employed polar RP-C18 (5 µm, 250 × 4.6 mm) using pure water as the mobile phase and a column temperature of 30 °C, coupled with a flow rate at 1.0 mL/min and detected under a UV detector at wavelength of 210 nm. Our method validation demonstrates excellent linearity (R 2 = 0.9993), accuracy (100.55%), and a limit of detection LOQ and LOD of 0.372 and 0.123 µgmL-1, respectively. These results clearly indicate that the developed polar RP-HPLC method for the separation and determination of ectoine is superior to earlier protocols.


Assuntos
Diamino Aminoácidos/análise , Diamino Aminoácidos/metabolismo , Bactérias/metabolismo , Cromatografia Líquida de Alta Pressão/métodos , Organismos Aquáticos , Cromatografia Líquida de Alta Pressão/instrumentação , Sedimentos Geológicos/microbiologia , Química Verde , Limite de Detecção , Temperatura Ambiente , Raios Ultravioleta
14.
ACS Appl Mater Interfaces ; 11(3): 3080-3086, 2019 Jan 23.
Artigo em Inglês | MEDLINE | ID: mdl-30588794

RESUMO

Lithium-sulfur batteries are promising for low-cost and high-energy storage, but their applications are still limited by poor cycling stability owing to soluble lithium polysulfide shuttling during battery operation. Avoiding shuttle effect is challenging but it is essential to avoid active material loss and prevent performance decay. Here, we use an ultrathin layer of MoS2 with thickness of 10-40 nm, which is 1-2 orders of magnitude thinner than conventional interlayers, for Li-S batteries to mitigate polysulfide shuttling. The MoS2 layer formed by exfoliated nanoflakes is deposited by the scalable liquid-based self-assembly method. With less than 1% of additional weight in the cathode, the MoS2 interlayer with complete coverage inhibits polysulfide diffusion across the separator and therefore remarkably improves the battery performances. Reversible specific capacity reaches 1010 and 600 mA h g-1 at 0.5 and 2C rates, respectively, which decay slowly over 400 cycles (0.11% per cycle). Moreover, the MoS2 films with high density of catalytic active flake edges enable high areal sulfur loading up to 10 mg cm-2 and areal capacity up to 9.7 mA h cm-2 at a current density of 3.2 mA cm-2.

15.
Nat Commun ; 9(1): 5289, 2018 12 11.
Artigo em Inglês | MEDLINE | ID: mdl-30538249

RESUMO

Electrochemical intercalation of ions into the van der Waals gap of two-dimensional (2D) layered materials is a promising low-temperature synthesis strategy to tune their physical and chemical properties. It is widely believed that ions prefer intercalation into the van der Waals gap through the edges of the 2D flake, which generally causes wrinkling and distortion. Here we demonstrate that the ions can also intercalate through the top surface of few-layer MoS2 and this type of intercalation is more reversible and stable compared to the intercalation through the edges. Density functional theory calculations show that this intercalation is enabled by the existence of natural defects in exfoliated MoS2 flakes. Furthermore, we reveal that sealed-edge MoS2 allows intercalation of small alkali metal ions (e.g., Li+ and Na+) and rejects large ions (e.g., K+). These findings imply potential applications in developing functional 2D-material-based devices with high tunability and ion selectivity.

16.
ACS Cent Sci ; 4(7): 894-898, 2018 Jul 25.
Artigo em Inglês | MEDLINE | ID: mdl-30062118

RESUMO

Dust filtration is a crucial process for industrial waste gas treatment. Great efforts have been devoted to improve the performance of dust filtration filters both in industrial and fundamental research. Conventional air-filtering materials are limited by three key issues: (1) Low filtration efficiency, especially for particulate matter (PM) below 1 µm; (2) large air pressure drops across the filter, which require a high energy input to overcome; and (3) safety hazards such as dust explosions and fires. Here, we have developed a "smart" multifunctional material which can capture PM with high efficiency and an extremely low pressure drop, while possessing a flame retardant design. This multifunctionality is achieved through a core-shell nanofiber design with the polar polymer Nylon-6 as the shell and the flame retardant triphenyl phosphate (TPP) as the core. At 80% optical transmittance, the multifunctional materials showed capture efficiency of 99.00% for PM2.5 and >99.50% for PM10-2.5, with a pressure drop of only 0.25 kPa (0.2% of atmospheric pressure) at a flow rate of 0.5 m s-1. Moreover, during direct ignition tests, the multifunctional materials showed extraordinary flame retardation; the self-extinguishing time of the filtrate-contaminated filter is nearly instantaneous (0 s/g) compared to 150 s/g for unmodified Nylon-6.

17.
Adv Sci (Weinh) ; 5(6): 1800384, 2018 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-29938193

RESUMO

Lithium-sulfur (Li-S) batteries are considered as one of the most promising energy storage systems for next-generation electric vehicles because of their high-energy density. However, the poor cyclic stability, especially at a high sulfur loading, is the major obstacles retarding their practical use. Inspired by the nacre structure of an abalone, a similar configuration consisting of layered carbon nanotube (CNT) matrix and compactly embedded sulfur is designed as the cathode for Li-S batteries, which are realized by a well-designed unidirectional freeze-drying approach. The compact and lamellar configuration with closely contacted neighboring CNT layers and the strong interaction between the highly conductive network and polysulfides have realized a high sulfur loading with significantly restrained polysulfide shuttling, resulting in a superior cyclic stability and an excellent rate performance for the produced Li-S batteries. Typically, with a sulfur loading of 5 mg cm-2, the assembled batteries demonstrate discharge capacities of 1236 mAh g-1 at 0.1 C, 498 mAh g-1 at 2 C and moreover, when the sulfur loading is further increased to 10 mg cm-2 coupling with a carbon-coated separator, a superhigh areal capacity of 11.0 mAh cm-2 is achieved.

18.
ACS Cent Sci ; 4(2): 260-267, 2018 Feb 28.
Artigo em Inglês | MEDLINE | ID: mdl-29532026

RESUMO

Lithium-sulfur (Li-S) batteries are regarded as promising next-generation high energy density storage devices for both portable electronics and electric vehicles due to their high energy density, low cost, and environmental friendliness. However, there remain some issues yet to be fully addressed with the main challenges stemming from the ionically insulating nature of sulfur and the dissolution of polysulfides in electrolyte with subsequent parasitic reactions leading to low sulfur utilization and poor cycle life. The high flammability of sulfur is another serious safety concern which has hindered its further application. Herein, an aqueous inorganic polymer, ammonium polyphosphate (APP), has been developed as a novel multifunctional binder to address the above issues. The strong binding affinity of the main chain of APP with lithium polysulfides blocks diffusion of polysulfide anions and inhibits their shuttling effect. The coupling of APP with Li ion facilitates ion transfer and promotes the kinetics of the cathode reaction. Moreover, APP can serve as a flame retardant, thus significantly reducing the flammability of the sulfur cathode. In addition, the aqueous characteristic of the binder avoids the use of toxic organic solvents, thus significantly improving safety. As a result, a high rate capacity of 520 mAh g-1 at 4 C and excellent cycling stability of ∼0.038% capacity decay per cycle at 0.5 C for 400 cycles are achieved based on this binder. This work offers a feasible and effective strategy for employing APP as an efficient multifunctional binder toward building next-generation high energy density Li-S batteries.

19.
Nano Lett ; 18(2): 1130-1138, 2018 02 14.
Artigo em Inglês | MEDLINE | ID: mdl-29297691

RESUMO

Aerosol-induced haze problem has become a serious environmental concern. Filtration is widely applied to remove aerosols from gas streams. Despite classical filtration theories, the nanoscale capture and evolution of aerosols is not yet clearly understood. Here we report an in situ investigation on the nanoscale capture and evolution of aerosols on polyimide nanofibers. We discovered different capture and evolution behaviors among three types of aerosols: wetting liquid droplets, nonwetting liquid droplets, and solid particles. The wetting droplets had small contact angles and could move, coalesce, and form axisymmetric conformations on polyimide nanofibers. In contrast, the nonwetting droplets had a large contact angle on polyimide nanofibers and formed nonaxisymmetric conformations. Different from the liquid droplets, the solid particles could not move along the nanofibers and formed dendritic structures. This study provides an important insight for obtaining a deep understanding of the nanoscale capture and evolution of aerosols and benefits future design and development of advanced filters.

20.
Adv Sci (Weinh) ; 5(1): 1700270, 2018 01.
Artigo em Inglês | MEDLINE | ID: mdl-29375960

RESUMO

Lithium-sulfur (Li-S) battery has emerged as one of the most promising next-generation energy-storage systems. However, the shuttle effect greatly reduces the battery cycle life and sulfur utilization, which is great deterrent to its practical use. This paper reviews the tremendous efforts that are made to find a remedy for this problem, mostly through physical or chemical confinement of the lithium polysulfides (LiPSs). Intrinsically, this "confinement" has a relatively limited effect on improving the battery performance because in most cases, the LiPSs are "passively" blocked and cannot be reused. Thus, this strategy becomes less effective with a high sulfur loading and ultralong cycling. A more "positive" method that not only traps but also increases the subsequent conversion of LiPSs back to lithium sulfides is urgently needed to fundamentally solve the shuttle effect. Here, recent advances on catalytic effects in increasing the rate of conversion of soluble long-chain LiPSs to insoluble short-chain Li2S2/Li2S, and vice versa, are reviewed, and the roles of noble metals, metal oxides, metal sulfides, metal nitrides, and some metal-free materials in this process are highlighted. Challenges and potential solutions for the design of catalytic cathodes and interlayers in Li-S battery are discussed in detail.

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