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1.
Small ; 20(27): e2309600, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38403846

RESUMO

Constructing a stable and robust solid electrolyte interphase (SEI) has a decisive influence on the charge/discharge kinetics of lithium-ion batteries (LIBs), especially for silicon-based anodes which generate repeated destruction and regeneration of unstable SEI films. Herein, a facile way is proposed to fabricate an artificial SEI layer composed of lithiophilic chitosan on the surface of two-dimensional siloxene, which has aroused wide attention as an advanced anode for LIBs due to its special characteristics. The optimized chitosan-modified siloxene anode exhibits an excellent reversible cyclic stability of about 672.6 mAh g-1 at a current density of 1000 mA g-1 after 200 cycles and 139.9 mAh g-1 at 6000 mA g-1 for 1200 cycles. Further investigation shows that a stable and LiF-rich SEI film is formed and can effectively adhere to the surface during cycling, redistribute lithium-ion flux, and enable a relatively homogenous lithium-ion diffusion. This work provides constructive guidance for interface engineering strategy of nano-structured silicon anodes.

2.
Small ; 20(8): e2306997, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-37823688

RESUMO

MXenes have demonstrated significant potential in electrochemical energy storage, particularly in supercapacitors, owing to their exceptional properties. The surface terminal groups of MXene play a pivotal role in pseudocapacitive mechanism. Considering the hindered electrolyte ion transport caused by -F terminal groups and the limited ion binding sites associated with -O terminal groups, this study proposes a novel strategy of replacing -F with -N terminal groups. The modulated MXene-N electrode, featuring a substantial number of -N terminal groups, demonstrates an exceptionally high gravimetric capacitance of 566 F g-1 (at a scan rate of 2 mV s-1 ) or 588 F g-1 (at a discharge rate of 1 A g-1 ) in 1 м H2 SO4 electrolyte, and the potential window is significantly increased. Furthermore, subsequent spectra analysis and density functional theory calculations are employed to investigate the mechanism associated with -N terminal groups. This work exemplifies the significance of terminal modulation in the context of electrochemical energy storage.

3.
Small ; 20(27): e2310972, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38282180

RESUMO

Recently, aqueous zinc-ion batteries with conversion mechanisms have received wide attention in energy storage systems on account of excellent specific capacity, high power density, and energy density. Unfortunately, some characteristics of cathode material, zinc anode, and electrolyte still limit the development of aqueous zinc-ion batteries possessing conversion mechanism. Consequently, this paper provides a detailed summary of the development for numerous aqueous zinc-based batteries: zinc-sulfur (Zn-S) batteries, zinc-selenium (Zn-Se) batteries, zinc-tellurium (Zn-Te) batteries, zinc-iodine (Zn-I2) batteries, and zinc-bromine (Zn-Br2) batteries. Meanwhile, the reaction conversion mechanism of zinc-based batteries with conversion mechanism and the research progress in the investigation of composite cathode, zinc anode materials, and selection of electrolytes are systematically introduced. Finally, this review comprehensively describes the prospects and outlook of aqueous zinc-ion batteries with conversion mechanism, aiming to promote the rapid development of aqueous zinc-based batteries.

4.
Small ; 19(50): e2304504, 2023 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-37635108

RESUMO

Aqueous zinc-ion batteries (AZIBs) are considered to be one of the most promising devices for large-scale energy storage systems owing to their high theoretical capacity, environmental friendliness, and safety. However, the ionic intercalation or surface redox mechanisms in conventional cathode materials generally result in unsatisfactory capacities. Conversion-type aqueous zinc-tellurium (Zn-Te) batteries have recently gained widespread attention owing to their high theoretical specific capacities. However, it remains an enormous challenge to improve the slow kinetics of the aqueous Zn-Te batteries. Here, MoO2 nanoclusters embedded in hierarchical nitrogen-doped carbon nanoflower (MoO2 /NC) hosts are successfully synthesized and loaded with Te in aqueous Zn-Te batteries. Benefitting from the highly dispersed MoO2 nanoclusters and hierarchical nanoflower structure with a large specific surface area, the electrochemical kinetics of the Te redox reaction are significantly improved. As a result, the Te-MoO2 /NC electrode exhibits superior cycling stability and a high specific capacity of 493 mAh g-1 at 0.1 A g-1 . Meanwhile, the conversion mechanism is systematically explored using a variety of ex situ characterization methods. Therefore, this study provides a novel approach for enhancing the kinetics of the Te redox reaction in aqueous Zn-Te batteries.

5.
Small ; 18(4): e2105696, 2022 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-34837326

RESUMO

The oxygen evolution reaction (OER) plays a key role in many electrochemical energy conversion systems, but it is a kinetically sluggish reaction and requires a large overpotential to deliver appreciable current, especially for the non-noble metal electrocatalysts. In this study, the authors report a surface phase engineering strategy to improve the OER performance of transition metal nitrides (TMNs). The iron-nickel nitrides/alloy nanospheres (FeNi3 -N) wrapped in carbon are synthesized, and the optimized FeNi3 -N catalyst displays dual-phase nitrides on the surface induced by atom migration phenomenon, resulting from the different migration rates of metal atoms during the nitridation process. It shows excellent OER performance in alkaline media with an overpotential of 222 mV at 10 mA cm-2 , a small Tafel slope of 41.53 mV dec-1 , and long-term durability under high current density (>0.5 A cm-2 ) for at least 36 h. Density functional theory (DFT) calculations further reveal that the dual-phase nitrides are favorable to decrease the energy barrier, modulate the d-band center to balance the absorption and desorption of the intermediates, and thus promote the OER electrochemical performance. This strategy may shed light on designing OER and other catalysts based on surface phase engineering.

6.
Small ; 17(13): e2007858, 2021 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-33690975

RESUMO

Transition metal phosphides (TMPs), especially the dual-metal TMPs, are highly active non-precious metal oxygen evolution reaction (OER) electrocatalysts. Herein, an interesting atom migration phenomenon induced by Kirkendall effect is reported for the preparation of cobalt-iron (Co-Fe) phosphides by the direct phosphorization of Co-Fe alloys. The compositions and distributions of the Co and Fe phosphides phases on the surfaces of the electrocatalysts can be readily controlled by Cox Fey alloys precursors and the phosphorization process with interesting atom migration phenomenon. The optimized Co7 Fe3 phosphides exhibit a low overpotential of 225 mV at 10 mA cm-2 in 1 m KOH alkaline media, with a small Tafel slope of 37.88 mV dec-1 and excellent durability. It only requires a voltage of 1.56 V to drive the current density of 10 mA cm-2 when used as both anode and cathode for overall water splitting. This work opens a new strategy to controllable preparation of dual-metal TMPs with designed phosphides active sites for enhanced OER and overall water splitting.

7.
Environ Sci Technol ; 55(21): 14828-14835, 2021 11 02.
Artigo em Inglês | MEDLINE | ID: mdl-34647733

RESUMO

Improving the stability of aminated metal-free catalysts is a big challenge in Fenton-like reactions. Herein, trinuclear iron cluster (Fe3 cluster)-protected aminated graphene (Fe3-NH2-GR) is designed by a protective strategy. By protecting with the Fe3 cluster, the lone pair electrons of amino groups are protected and the N content of Fe3-NH2-GR can be fixed steadily. In peroxymonosulfate (PMS)-based Fenton-like reactions with a fixed-bed reactor, the lifetime of Fe3-NH2-GR is two times longer than that of aminated graphene (NH2-GR) under the same conditions. The deactivation kinetics shows that both Fe3-NH2-GR and NH2-GR follow zero-order kinetics and the deactivation rate constants of Fe3-NH2-GR are lower than that of NH2-GR at every period. Moreover, Fe3-NH2-GR still maintains 50% phenol degradation after 40 h rather than being constantly deactivated as NH2-GR. This stable activity is attributed to the formation of -O-NO2, while the N content will be lost in NH2-GR. This protective strategy by the Fe3 cluster provides a reliable method to enhance the efficiency and stability of carbon catalysts in Fenton-like reactions.


Assuntos
Grafite , Carbono , Catálise , Peróxido de Hidrogênio , Ferro , Oxirredução
8.
Langmuir ; 36(48): 14710-14716, 2020 12 08.
Artigo em Inglês | MEDLINE | ID: mdl-33227197

RESUMO

Hydrodeoxygenation (HDO) of bio-oil is a crucial step for improving the bio-fuel quality, but developing highly dispersed Pt-based catalysts with high selectivity for target alkanes remains a great challenge. This study presents a fast surfactant-free method to prepare the MoS2-supported Pt catalyst for HDO. Ultrafine Pt nanoparticles with sizes of <5 nm can be readily grown on chemically exfoliated MoS2 nanosheets (NSs) via the direct microwave-assisted thermal reduction. The obtained Pt NPs/MoS2 composites show excellent catalytic performance in the conversion of palmitic acid, and the best selectivity (also the yield) of hexadecane and pentadecane is 80.56 and 19.43%, respectively.

9.
Small ; 14(2)2018 01.
Artigo em Inglês | MEDLINE | ID: mdl-29149471

RESUMO

The development of highly efficient and durable non-noble metal electrocatalysts for the hydrogen evolution reaction (HER) is significant for clean and renewable energy research. This work reports the synthesis of N-doped graphene nanosheets supported N-doped carbon coated cobalt phosphide (CoP) nanoparticles via a pyrolysis and a subsequent phosphating process by using polyaniline. The obtained electrocatalyst exhibits excellent electrochemical activity for HER with a small overpotential of -135 mV at 10 mA cm-2 and a low Tafel slope of 59.3 mV dec-1 in 0.5 m H2 SO4 . Additionally, the encapsulation of N-doped carbon shell prevents CoP nanoparticles from corrosion, exhibiting good stability after 14 h operation. Moreover, the as-prepared electrocatalyst also shows outstanding activity and stability in basic and neutral electrolytes.

10.
Nanotechnology ; 29(50): 505603, 2018 Dec 14.
Artigo em Inglês | MEDLINE | ID: mdl-30272574

RESUMO

A Cu2O based multi-layered photocathode was fabricated with a layer-by-layer assembly method for enhanced photoelectrochemical (PEC) hydrogen evolution. Au was first electrodeposited on the fluorine-doped tin oxide glass to decrease the electrochemical impedance of the Cu2O photocathode. A layer of TiO2 was then coated to increase the light-to-electricity energy conversion efficiency and the chemical stability by forming a p-n junction with Cu2O. Exfoliated WS2 nanosheets obtained from lithium insertion were then coated as the electron acceptor to facilitate the hydrogen evolution. This photocathode is effective for PEC hydrogen evolution, and a photocurrent of -10 mA cm-2 can be obtained at -0.33 V versus RHE in a phosphorus buffer (pH = 6.0) under visible light (λ ≥ 420 nm, 100 mW cm-2) on the optimized photocathode.

11.
Nanotechnology ; 28(20): 205603, 2017 May 19.
Artigo em Inglês | MEDLINE | ID: mdl-28358723

RESUMO

The detection and removal of nitroaromatic compounds is an important issue for environmental protection. In this study, a hybrid of molybdenum disulfide (MoS2) and graphene (GR) was first synthesized using a facile hydrothermal method. Au and Ag nanoparticles were then deposited onto the surface of the MoS2/GR hybrid with sodium citrate as the stabilizer and reductant. Compared to using pure MoS2 as the support, the obtained Au (Ag)-MoS2/GR composites showed improved activity for electrochemical detection and chemical reduction of 4-nitrophenol. The activity enhancement appears to be due to the addition of GR, which could improve the conductivity as well as provide more active sites. The successful synthesis of Au (Ag)-MoS2/GR composites could provide new multi-function catalysts for environmental protection.

12.
Zhongguo Yi Liao Qi Xie Za Zhi ; 41(2): 79-83, 2017 Mar 30.
Artigo em Chinês | MEDLINE | ID: mdl-29862673

RESUMO

A cardiovascular function testing system was designed in platform which was built with ARM microprocessor s3c2440 and Linux system, to achieve pulse wave acquisition, feature extraction, index calculation and so on. This article mainly describes the hardware circuit, and describes the touchscreen driver, external ADC driver, and visualization QT-based applications in detail. The system is easy to use, with real-time, low power consumption. Compared with common cardiovascular function test instrument, the results shows that the system can better assess the cardiovascular function, expecially in several key indicators like subendocardial myocardial viability rate and augmentation index, the indicators show good correlations.


Assuntos
Fenômenos Fisiológicos Cardiovasculares , Computadores , Frequência Cardíaca , Sistema Cardiovascular
13.
Nanotechnology ; 27(38): 385604, 2016 Sep 23.
Artigo em Inglês | MEDLINE | ID: mdl-27528593

RESUMO

Exfoliated molybdenum disulfide (MoS2) has unique 2H phase and semiconductor properties and potential applications across a wide range of fields. However, the chemically exfoliated MoS2 nanosheets from Li x MoS2 have a 1T phase, and searching for a fast route to get processable 2H-MoS2 nanosheets and its nanocomposites is still an urgent task. This study reports on a simple, fast and efficient microwave strategy to achieve the 1T to 2H phase conversion of MoS2 and the successful preparation of processable 2H-MoS2 nanosheets and their nanocomposites. The method here may be easily changed to achieve the phase change of other exfoliated TMDs.

14.
ACS Appl Mater Interfaces ; 16(20): 26079-26087, 2024 May 22.
Artigo em Inglês | MEDLINE | ID: mdl-38742759

RESUMO

Vanadium-based oxides, known for their high capacity and low cost, have garnered significant attention as promising cathode candidates in aqueous zinc-ion batteries. Nonetheless, their poor rate performance and limited durability in aqueous electrolytes present a challenge to the realistic implementation of vanadium-based aqueous zinc-ion batteries. Here, we synthesized nitrogen-doped V2O3@C (N-V2O3@N-C) via ammonia treatment of V2O3@C derived from vanadium-based metal-organic framework (V-MOF), aiming to achieve outstanding rate and cycling performance. The N-V2O3@N-C electrode exhibits notable in situ self-transformation into an amorphous state. Density functional theory calculations reveal that the distorted N-V2O3 structure and uneven charge distribution result in the creation of an amorphous state. As expected, Zn/N-V2O3@N-C aqueous zinc-ion batteries can achieve remarkable specific capacity (349.0 mAh g-1 at 0.1 A g-1), along with impressive rate performance, showcasing a capacity of 253.5 mAh g-1 at 5 A g-1 and exceptional durability at 5 A g-1 (96.4% after 1350 cycles). The employed induced amorphization approach offers novel perspectives for designing high-performance cathodes that exhibit both sturdy structures and extended cycling lifespans.

15.
Chemosphere ; 355: 141799, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38554876

RESUMO

Designing iron-based catalysts for Fenton-like reactions with peroxymonosulfate (PMS) as oxidants have attracted growing attentions. Herein, pyrite FeS2 supported on carbon spheres (FeS2@C) is synthesized by a facile low-temperature method. The FeS2@C/PMS system can degrade carbamazepine (CBZ) effectively in a wide pH range. Sulfate radicals (SO4·-), hydroxyl radicals (·OH), superoxide radical (O2·-), and singlet oxygen (1O2) are the responsible reactive oxygen species (ROSs) for CBZ degradation. Moreover, in the simulated fixed-bed reactor, the FeS2@C/PMS system can maintain a high CBZ removal ratio of >95% for than 8 h, exhibiting its excellent stability. The outstanding performance of FeS2@C/PMS system is attributed to the presence of carbon spheres and lattice S2-, which together promote the Fe(III)/Fe(II) redox cycle. The FeS2@C is a promising catalyst due to its facile synthesis, low cost, high efficiency, and excellent stability to activate PMS for organics degradation.


Assuntos
Carbono , Compostos Férricos , Sulfetos , Ferro , Peróxidos
16.
J Colloid Interface Sci ; 665: 838-845, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38564947

RESUMO

Currently, aqueous zinc ion batteries (AZIBs) have grown to be a good choice for large-scale energy storage systems due to their high theoretical specific capacity, low redox potential, low cost, and non-toxicity of the aqueous electrolyte. However, it is still challenging to obtain high specific capacity and stability suitable cathodes. Herein, hierarchical self-supporting potassium ammonium vanadate@MXene (KNVO@MXene) hybrid films were prepared by vacuum filtration method. Due to the three-dimensional nanoflower structure of KNVO with dual ions intercalation, high conductivity of two-dimensional Ti3C2Tx MXene, and the hierarchical self-supporting structure, the AZIB based on the KNVO@MXene hybrid film cathode possessed superior specific capacity (481 mAh/g at 0.3 A/g) and cycling stability (retaining 125 mAh/g after 1000 cycles at a high current density of 10 A/g). In addition, the storage mechanism was revealed by various ex-situ characterizations. Hence, a new viewpoint for the preparation of AZIB self-supporting cathode materials is presented.

17.
J Colloid Interface Sci ; 672: 688-699, 2024 Jun 06.
Artigo em Inglês | MEDLINE | ID: mdl-38865882

RESUMO

In this study, a series of Fe-based materials are facilely synthesized using MIL-88A and melamine as precursors. Changing the mass ratio of melamine and MIL-88A could tune the coating layers of generated zero-valent iron (Fe0) particles from Fe3C to Fe3N facilely. Compared to Fe/Fe3N@NC sample, Fe/Fe3C@NC exhibits better catalytic activity and stability to degrade carbamazepine (CBZ) with peroxymonosulfate (PMS) as oxidant. Free radical quenching tests, open-circuit potential (OCP) test and electron paramagnetic resonance spectra (EPR) prove that hydroxyl radicals (OH) and superoxide radical (O2-) are dominant reactive oxygen species (ROSs) with Fe/Fe3C@NC sample. For Fe/Fe3N@NC sample, the main ROSs are changed into sulfate radicals (SO4-) and high valent iron-oxo (Fe (IV)=O) species. In addition, the better conductivity of Fe3C is beneficial for the electron transfer from Fe0 to the Fe3C, thus could keep the activity of the surface sites and obtain better stability. DFT calculation reveals the better adsorption and activation ability of Fe3C than Fe3N. Moreover, PMS can also be adsorbed on the Fe sites of Fe3N with shorter FeO bonds and longer SO bonds than on Fe3C, the Fe (IV)=O is thus present in the Fe/Fe3N@NC/PMS system. This study provides a novel strategy for the development of highly active Fe-based materials for Fenton-like reactions and thus could promote their real application.

18.
J Colloid Interface Sci ; 665: 219-231, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38522161

RESUMO

Herein, a new heterogeneous CoSe2-x@NC material with abundant selenium vacancies is synthesized via an in-situ carbonization-selenization process from cobaltic metal organic framework (Co-MOF). The obtained CoSe2-x@NC has a unique electronic structure and rich active sites, which can activate peroxymonosulfate (PMS) to degrade carbamazepine (CBZ) with superior catalytic performance and stability. The quenchingexperiments and EPR test show that SO4•- is the dominant reactive oxidation species (ROSs) for CBZ degradation. Significantly, systemic electrochemical tests and theoretical calculations illustrated that the dominant role of SO4•- is attributed to the existence of abundant selenium vacancies in CoSe2-x@NC, which can adjust the density of electron cloud of the Co atoms in CoSe2-x@NC to improve the PMS adsorption and promoting the conversion of transition metallic redox pairs (Co3+/Co2+). This work provides a facile way to improve the activity and stability of CoSe2 by defect engineering in the PMS based advanced oxidation process (AOPs).

19.
Chem Commun (Camb) ; 59(23): 3427-3430, 2023 Mar 16.
Artigo em Inglês | MEDLINE | ID: mdl-36857619

RESUMO

The oxygen evolution reaction (OER) is a vital half-reaction in several electrochemical energy conversion devices. Herein, we report a hierarchical NiMoO4/NiFe LDH pre-catalyst that enables complete reconstruction and fine structural inheritance, while exhibiting a low overpotential of 188 mV at 10 mA cm-2 in 1.0 M KOH.

20.
J Colloid Interface Sci ; 629(Pt B): 473-481, 2023 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-36174290

RESUMO

HYPOTHESIS: Na5V12O32 (NVO) is a potential cathode for aqueous zinc ion batteries (AZIBs). However, it suffers severe capacity decay due to the dissolution of the active material. The structural design may be an effective solution to the problem. EXPERIMENTS: Herein, we construct a typical two-dimensional hierarchical structure of Na5V12O32@graphene (NVO@G) via a facile molten salt method. FINDINGS: The capacity fading problem is solved by the in-situ conversion of NVO@G to a more stable hierarchical system during cycling. The in-situ formed zinc pyrovanadate (Zn3V2O7(OH)2·2H2O, ZVO) nanosheets on the surface of graphene exhibits excellent zinc-ion storage stability. The presence of graphene induces the growth of NVO nanobelts to construct the typical two-dimensional hierarchical structure. Additionally, the in-situ conversion makes the formed ZVO nanosheets contact with graphene better. Benefitting from the hierarchical nanostructure and in-situ phase conversion, the NVO@G electrode shows excellent long-term stability (96.4% retention after 340 cycles at 0.3 A g-1, 85.7% retention after 4400 cycles at 5 A g-1) and high zinc ion storage capacity (220 mAh g-1 at 0.3 A g-1), which is superior to those of most electrode materials previously reported.

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