Your browser doesn't support javascript.
loading
Mostrar: 20 | 50 | 100
Resultados 1 - 20 de 67
Filtrar
Mais filtros










Base de dados
Intervalo de ano de publicação
1.
Adv Mater ; : e2105812, 2021 Oct 22.
Artigo em Inglês | MEDLINE | ID: mdl-34677873

RESUMO

Next-generation batteries based on conversion reactions, including aqueous metal-air batteries, nonaqueous alkali metal-O2 and -CO2 batteries, alkali metal-chalcogen batteries, and alkali metal-ion batteries have attracted great interest. However, their use is restricted by inefficient reversible conversion of active agents. Developing bifunctional catalysts to accelerate the conversion reaction kinetics in both discharge and charge processes is urgently needed. Graphene-, or graphene-like carbon-supported atomically dispersed metal catalysts (G-ADMCs) have been demonstrated to show excellent activity in various electrocatalytic reactions, making them promising candidates. Different from G-ADMCs for catalysis, which only require high activity in one direction, G-ADMCs for rechargeable batteries should provide high activity in both discharging and charging. This review provides guidance for the design and fabrication of bifunctional G-ADMCs for next-generation rechargeable batteries based on conversion reactions. The key challenges that prevent their reversible conversion, the origin of the activity of bifunctional G-ADMCs, and the current design principles of bifunctional G-ADMCs for highly reversible conversion, have been analyzed and highlighted for each conversion-type battery. Finally, a summary and outlook on the development of bifunctional G-ADMC materials for next-generation batteries with a high energy density and excellent energy efficiency are given.

2.
Nat Commun ; 12(1): 6122, 2021 10 21.
Artigo em Inglês | MEDLINE | ID: mdl-34675199

RESUMO

Perspiration evaporation plays an indispensable role in human body heat dissipation. However, conventional textiles tend to focus on sweat removal and pay little attention to the basic thermoregulation function of sweat, showing limited evaporation ability and cooling efficiency in moderate/profuse perspiration scenarios. Here, we propose an integrated cooling (i-Cool) textile with unique functional structure design for personal perspiration management. By integrating heat conductive pathways and water transport channels decently, i-Cool exhibits enhanced evaporation ability and high sweat evaporative cooling efficiency, not merely liquid sweat wicking function. In the steady-state evaporation test, compared to cotton, up to over 100% reduction in water mass gain ratio, and 3 times higher skin power density increment for every unit of sweat evaporation are demonstrated. Besides, i-Cool shows about 3 °C cooling effect with greatly reduced sweat consumption than cotton in the artificial sweating skin test. The practical application feasibility of i-Cool design principles is well validated based on commercial fabrics. Owing to its exceptional personal perspiration management performance, we expect the i-Cool concept can provide promising design guidelines for next-generation perspiration management textiles.

3.
ACS Nano ; 15(9): 13901-13923, 2021 Sep 28.
Artigo em Inglês | MEDLINE | ID: mdl-34516074

RESUMO

The increasing demand for wearable electronic devices necessitates flexible batteries with high stability and desirable energy density. Flexible lithium-sulfur batteries (FLSBs) have been increasingly studied due to their high theoretical energy density through the multielectron chemistry of low-cost sulfur. However, the implementation of FLSBs is challenged by several obstacles, including their low practical energy density, short life, and poor flexibility. Various graphene-based materials have been applied to address these issues. Graphene, with good conductivity and flexibility, exhibits synergistic effects with other active/catalytic/flexible materials to form multifunctional graphene-based materials, which play a pivotal role in FLSBs. This review summarizes the recent progress of graphene-based materials that have been used as various FLSB components, including cathodes, interlayers, and anodes. Particular attention is focused on the precise nanostructures, graphene efficacy, interfacial effects, and battery layout for realizing FLSBs with good flexibility, energy density, and cycling stability.

4.
Nano Lett ; 21(19): 8447-8454, 2021 Oct 13.
Artigo em Inglês | MEDLINE | ID: mdl-34591497

RESUMO

Lithium-ion batteries (LIBs) are still facing safety problems, mainly due to dendrite growth on the anode that leads to combustion and explosion. Forming a stable solid electrolyte interface (SEI) layer is an effective way to suppress this. To induce the formation of stable SEI using simple methods at a low cost, we report an ultrathin and large-scale hexagonal boron nitride (h-BN)/polyimide (PI) layer that was coated on a commercial polypropylene (PP) separator. The formation of a stabilized SEI component induced by the h-BN coating layer is proposed, as suggested by theoretical calculations and confirmed by electrochemical analysis and spectroscopy. It effectively suppresses Li dendrite growth and reduces the consumption of active lithium. The separator also has good electrolyte wettability, excellent mechanical strength and thermal conductivity, and high thermal stability. When using the h-BN modified separator in a full cell, the capacity is extremely stable after long cycling and high temperature.

5.
Adv Mater ; 33(44): e2105947, 2021 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-34569660

RESUMO

Single-atom metal catalysts (SACs) are used as sulfur cathode additives to promote battery performance, although the material selection and mechanism that govern the catalytic activity remain unclear. It is shown that d-p orbital hybridization between the single-atom metal and the sulfur species can be used as a descriptor for understanding the catalytic activity of SACs in Li-S batteries. Transition metals with a lower atomic number are found, like Ti, to have fewer filled anti-bonding states, which effectively bind lithium polysulfides (LiPSs) and catalyze their electrochemical reaction. A series of single-atom metal catalysts (Me = Mn, Cu, Cr, Ti) embedded in three-dimensional (3D) electrodes are prepared by a controllable nitrogen coordination approach. Among them, the single-atom Ti-embedded electrode has the lowest electrochemical barrier to LiPSs reduction/Li2 S oxidation and the highest catalytic activity, matching well with the theoretical calculations. By virtue of the highly active catalytic center of single-atom Ti on the conductive transport network, high sulfur utilization is achieved with a low catalyst loading (1 wt.%) and a high area-sulfur loading (8 mg cm-2 ). With good mechanical stability for bending, these 3D electrodes are suitable for fabricating bendable/foldable Li-S batteries for wearable electronics.

6.
ACS Nano ; 15(6): 9841-9850, 2021 Jun 22.
Artigo em Inglês | MEDLINE | ID: mdl-34033458

RESUMO

As one of the CO2 capture and utilization technologies, Li-CO2 batteries have attracted special interest in the application of carbon neutral. However, the design and fabrication of a low-cost high-efficiency cathode catalyst for reversible Li2CO3 formation and decomposition remains challenging. Here, guided by theoretical calculations, CO2 was utilized to activate the catalytic activity of conventional nitrogen-doped graphene, in which pyridinic-N and pyrrolic-N have a high total content (72.65%) and have a high catalytic activity in both CO2 reduction and evolution reactions, thus activating the reversible conversion of Li2CO3 formation and decomposition. As a result, the designed cathode has a low voltage gap of 2.13 V at 1200 mA g-1 and long-life cycling stability with a small increase in the voltage gap of 0.12 V after 170 cycles at 500 mA g-1. Our work suggests a way to design metal-free catalysts with high activity that can be used to activate the performance of Li-CO2 batteries.

7.
Small ; : e2007676, 2021 Apr 18.
Artigo em Inglês | MEDLINE | ID: mdl-33870632

RESUMO

Fast-charging batteries have attracted great attention, and are anticipated to charge electrical vehicles and consumer electronics to full-capacity in several minutes. However, commercial electrode materials in batteries generally have a limited rate performance and are difficult to be used in fast-charging batteries. Designing electrodes with an aligned structure is an effective way to shorten the ion transport path and improve the rate performance of a battery. The excellent electronic conductivity of carbon-based electrodes is another key factor for increasing the rate capability of rechargeable batteries. Therefore, aligned carbon-based electrodes (ACBEs) can significantly improve the power density by combining the advantages of an aligned structure and carbon-based materials. In this review, the mechanism, advantages, and challenges of ACBEs for fast-charging batteries are evaluated, and then the design and preparation methods of ACBEs based on their different dimensions are summarized, and their applications in different batteries are illustrated. Finally, the future development of ACBEs for fast-charging batteries is considered.

8.
Adv Mater ; 33(12): e2007090, 2021 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-33599013

RESUMO

Sodium-ion batteries (SIBs) based on conversion-type metal sulfide (MS) anodes have attracted extraordinary attention due to relatively high capacity and intrinsic safety. The highly reversible conversion of M/Na2 S to pristine MS in charge plays a vital role with regard to the electrochemical performance. Here, taking conventional MoS2 as an example, guided by theoretical simulations, a catalyst of iron single atoms on nitrogen-doped graphene (SAFe@NG) is selected and first used as a substrate to facilitate the reaction kinetics of MoS2 in the discharging process. In the following charging process, using a combination of spectroscopy and microscopy, it is demonstrated that the SAFe@NG catalyst enables an efficient reversible conversion reaction of Mo/Na2 S→NaMoS2 →MoS2 . Moreover, theoretical simulations reveal that the reversible conversion mechanism shows favorable formation energy barrier and reaction kinetics, in which SAFe@NG with the Fe-N4 coordination center facilitates the uniform dispersion of Na2 S/Mo and the decomposition of Na2 S and NaMoS2 . Therefore, efficient reversible conversion reaction MoS2 ↔NaMoS2 ↔Mo/Na2 S is enabled by the SAFe@NG catalyst. This work contributes new avenues for designing conversion-type materials with an efficient reversible mechanism.

9.
ACS Nano ; 14(10): 14026-14035, 2020 Oct 27.
Artigo em Inglês | MEDLINE | ID: mdl-33016705

RESUMO

Potassium ion batteries (PIBs) have shown great potential as a next-generation electrochemical energy storage system, due to the natural abundance of potassium and the relatively low redox potential of K ions. To accommodate the large ionic radius of K ions, conversion-type electrode materials are regarded as suitable candidates for K ion storage. However, the triggering mechanism of a conversion reaction in most anode materials of PIBs is unclear, which limits their further development. To reveal the mechanism, in this work, MoSe2, MoS2, and MoO2 were selected as model materials, guided by theoretical calculations, to investigate the K ion storage process. Through ex situ characterization, it was found that intercalation reactions preferentially occur in MoSe2 and MoS2, while an adsorption reaction preferentially occurs in MoO2. This is because of the larger interlayer spacing and lower K ion intercalation barrier in MoSe2 and MoS2 than in MoO2. The preferential intercalation reactions are able to induce a further conversion reaction by reducing the reaction barrier, thereby realizing high K ion storage capacities. As a result, the MoSe2-rGO and MoS2-rGO hybrids showed higher reversible capacities than the MoO2-rGO hybrid. By demonstrating a relationship between intercalation and the conversion reaction and understanding the mechanism, guidance is provided for selecting the electrode materials to obtain PIBs with high performance.

10.
Research (Wash D C) ; 2020: 7163948, 2020.
Artigo em Inglês | MEDLINE | ID: mdl-32734276

RESUMO

Lithium (Li) metal has been regarded as one of the most promising anode materials to meet the urgent requirements for the next-generation high-energy density batteries. However, the practical use of lithium metal anode is hindered by the uncontrolled growth of Li dendrites, resulting in poor cycling stability and severe safety issues. Herein, vertical graphene (VG) film grown on graphite paper (GP) as an all-carbon current collector was utilized to regulate the uniform Li nucleation and suppress the growth of dendrites. The high surface area VG grown on GP not only reduces the local current density to the uniform electric field but also allows fast ion transport to homogenize the ion gradients, thus regulating the Li deposition to suppress the dendrite growth. The Li deposition can be further guided with the lithiation reaction between graphite paper and Li metal, which helps to increase lithiophilicity and reduce the Li nucleation barrier as well as the overpotential. As a result, the VG film-based anode demonstrates a stable cycling performance at a current density higher than 5 mA cm-2 in half cells and a small hysteresis of 50 mV at 1 mA cm-2 in symmetric cells. This work provides an efficient strategy for the rational design of highly stable Li metal anodes.

11.
Adv Mater ; 32(32): e2000315, 2020 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-32627911

RESUMO

Accelerated conversion by catalysis is a promising way to inhibit shuttling of soluble polysulfides in lithium-sulfur (Li-S) batteries, but most of the reported catalysts work only for one direction sulfur reaction (reduction or oxidation), which is still not a root solution since fast cycled use of sulfur species is not finally realized. A bidirectional catalyst design, oxide-sulfide heterostructure, is proposed to accelerate both reduction of soluble polysulfides and oxidation of insoluble discharge products (e.g., Li2 S), indicating a fundamental way for improving both the cycling stability and sulfur utilization. Typically, a TiO2 -Ni3 S2 heterostructure is prepared by in situ growing TiO2 nanoparticles on Ni3 S2 surface and the intimately bonded interfaces are the key for bidirectional catalysis. For reduction, TiO2 traps while Ni3 S2 catalytically converts polysulfides. For oxidation, TiO2 and Ni3 S2 both show catalytic activity for Li2 S dissolution, refreshing the catalyst surface. The produced sulfur cathode with TiO2 -Ni3 S2 delivers a low capacity decay of 0.038% per cycle for 900 cycles at 0.5C and specially, with a sulfur loading of 3.9 mg cm-2 , achieves a high capacity retention of 65% over 500 cycles at 0.3C. This work unlocks how a bidirectional catalyst works for boosting Li-S batteries approaching practical uses.

12.
Sci Adv ; 6(21): eaay5098, 2020 May.
Artigo em Inglês | MEDLINE | ID: mdl-32494732

RESUMO

In lithium-sulfur (Li-S) chemistry, the electrically/ionically insulating nature of sulfur and Li2S leads to sluggish electron/ion transfer kinetics for sulfur species conversion. Sulfur and Li2S are recognized as solid at room temperature, and solid-liquid phase transitions are the limiting steps in Li-S batteries. Here, we visualize the distinct sulfur growth behaviors on Al, carbon, Ni current collectors and demonstrate that (i) liquid sulfur generated on Ni provides higher reversible capacity, faster kinetics, and better cycling life compared to solid sulfur; and (ii) Ni facilitates the phase transition (e.g., Li2S decomposition). Accordingly, light-weight, 3D Ni-based current collector is designed to control the deposition and catalytic conversion of sulfur species toward high-performance Li-S batteries. This work provides insights on the critical role of the current collector in determining the physical state of sulfur and elucidates the correlation between sulfur state and battery performance, which will advance electrode designs in high-energy Li-S batteries.

13.
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.

14.
Adv Sci (Weinh) ; 7(2): 1903603, 2020 01.
Artigo em Inglês | MEDLINE | ID: mdl-31993298

RESUMO

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

15.
Nat Nanotechnol ; 15(3): 231-237, 2020 Mar.
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.

16.
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.

17.
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.

18.
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.

19.
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.

20.
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.

SELEÇÃO DE REFERÊNCIAS
DETALHE DA PESQUISA
...