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1.
ACS Appl Mater Interfaces ; 16(22): 28560-28569, 2024 Jun 05.
Artigo em Inglês | MEDLINE | ID: mdl-38768309

RESUMO

The commercialization process of perovskite solar cells (PSCs) is markedly restricted by the power conversion efficiency (PCE) and long-term stability. During fabrication and operation, the bottom interface of the organic-inorganic hybrid perovskite layer frequently exhibits voids and residual PbI2, while these defects inevitably act as recombination centers and degradation sites, affecting the efficiency and stability of the devices. Therefore, the degradation and nonradiative recombination originating from the buried interface should be thoroughly resolved. Here, we report a multifunctional passivator by introducing malonic dihydrazide as an interfacial chemical bridge between the electron transport layer and the perovskite (PVK) layer. MADH with hydrazine groups improves the surface affinity of SnO2 and provides nucleation sites for the growth of PVK, leading to the reduced residual PbI2 and the voids resulting from the inhomogeneous solvent volatilization at the bottom interface. Meanwhile, the hydrazine group and carbonyl group synergistically coordinate with Pb2+ to improve the crystal growth environment, reducing the number of Pb-related defects. Eventually, the PCE of the PSCs is significantly enhanced benefiting from the reduced interfacial defects and the increased carrier transport. Moreover, the reductive nature of hydrazide further inhibits I2 generation during long-term operation, and the device retains 90% of the initial PCE under a 1 sun continuous illumination exposure of 700 h.

2.
Dalton Trans ; 53(21): 9081-9091, 2024 May 28.
Artigo em Inglês | MEDLINE | ID: mdl-38738658

RESUMO

Lithium-ion batteries (LIBs) are greatly limited in their practical application because of their poor cycle performance, low conductivity and volume expansion. Herein, molten salts (MSs) FeCl3·6H2O-NMP with low temperature via simple preparation are used as the anode material of LIBs for the first time to break through the bottleneck of LIBs. The good fluidity and high self-healing of FeCl3·6H2O-NMP effectively avoid the collapse and breakage of the structure. Based on this feature, the initial discharge specific capacity reached 770.28 mA h g-1, which was more than twice that of the commercial graphite anode. After 200 cycles at a current density of 100 mA g-1, the specific capacity did not decrease rather it was found to be higher than the initial discharge specific capacity, reaching 867.24 mA h g-1. Besides, the good conductivity of MSs provides convenience for the removal and intercalation of Li+. The active H sites that can combine with lithium ions form LiH and provide capacity for LIBs. Density functional theory (DFT) calculation also provided theoretical proof for the mechanism of LIBs.

3.
Dalton Trans ; 53(11): 4900-4921, 2024 Mar 12.
Artigo em Inglês | MEDLINE | ID: mdl-38321942

RESUMO

With the advent of lithium-ion batteries (LIBs), the selection and application of electrode materials have been the subject of much discussion and study. Among them, graphite has been widely investigated for use as electrode materials in LIBs due to its abundant resources, low cost, safety and electrochemical diversity. While it is commonly recognized that conventional graphite materials utilized for commercial purposes have a limited theoretical capacity, there has been a steady emergence of new and improved carbonaceous materials for use as anodes in light of the progressive development of LIBs. In this paper, the latest research progress of various carbon materials in LIBs is systematically and comprehensively reviewed. Firstly, the rocking chair charging and discharging mechanism of LIBs is briefly introduced in this paper, using graphite anodes as an example. After that, the general categories of carbonaceous materials are highlighted, and the recent research on the recent progress of various carbonaceous materials (graphite-based, amorphous carbon-based, and nanocarbon-based) used in LIB anodes is presented separately based on the classification of the structural morphology, emphasizing the influence of the morphology and structure of carbon-based materials on the electrochemical performance of the batteries. Finally, the current challenges of carbonaceous materials in LIB applications and the future development of other novel carbonaceous materials are envisioned.

4.
Small ; 20(26): e2310426, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38229551

RESUMO

Sodium-ion batteries (SIBs), as the next-generation high-performance electrochemical energy storage devices, have attracted widespread attention due to their cost-effectiveness and wide geographical distribution of sodium. As a crucial component of the structure of SIBs, the anode material plays a crucial role in determining its electrochemical performance. Significantly, metal phosphide exhibits remarkable application prospects as an anode material for SIBs because of its low redox potential and high theoretical capacity. However, due to volume expansion limitations and other factors, the rate and cycling performance of metal phosphides have gradually declined. To address these challenges, various viable solutions have been explored. In this paper, the recent research progress of metal phosphide materials for SIBs is systematically reviewed, including the synthesis strategy of metal phosphide, the storage mechanism of sodium ions, and the application of metal phosphide in electrochemical aspects. In addition, future challenges and opportunities based on current developments are presented.

5.
Small Methods ; : e2300804, 2023 Sep 10.
Artigo em Inglês | MEDLINE | ID: mdl-37691014

RESUMO

The practical application of aqueous zinc-ion batteries (AZIBs) is limited by serious side reactions, such as the hydrogen evolution reaction and Zn dendrite growth. Here, the study proposes a novel adoption of a biodegradable electrolyte additive, γ-Valerolactone (GVL), with only 1 vol.% addition (GVL-to-H2 O volume ratio) to enable a stable Zn metal anode. The combination of experimental characterizations and theoretical calculations verifies that the green GVL additive can competitively engage the solvated structure of Zn2+ via replacing a H2 O molecule from [Zn(H2 O)6 ]2+ , which can efficiently reduce the reactivity of water and inhibit the subsequent side reactions. Additionally, GVL molecules are preferentially adsorbed on the surface of Zn to regulate the uniform Zn deposition and suppress the Zn dendrite growth. Consequently, the Zn anode exhibits boosted stability with ultralong cycle lifespan (over 3500 h) and high reversibility with 99.69% Coulombic efficiency. The Zn||MnO2 full batteries with ZnSO4 -GVL electrolyte show a high capacity of 219 mAh g-1 at 0.5 A g-1 and improved capacity retention of 78% after 550 cycles. This work provides inspiration on bio-based electrolyte additives for aqueous battery chemistry and promotes the practical application of AZIBs.

6.
Dalton Trans ; 52(33): 11526-11534, 2023 Aug 22.
Artigo em Inglês | MEDLINE | ID: mdl-37540012

RESUMO

Regulating the structural and interfacial properties of transition metal phosphides (TMPs) by coupling carbon-based materials with large surface areas to enhance hydrogen evolution reaction (HER) performance presents significant progress for water splitting technology. Herein, we constructed a composite substrate of a three-dimensional porous graphene oxide matrix (3D-GO) embedded in nickel foam (NF) to grow a Co2P electrocatalyst. Well-defined gladiolus-like Co2P nanowire arrays tightly anchored on the substrate show enhanced electrochemical characteristics for the hydrogen evolution reaction (HER) based on the promoting roles of 3D porous reduced GO (3D-rGO) derived from 3D-GO, which promotes the dispersion of active components, improves the rate of electron transfer, and facilitates the transport of water molecules. As a result, the obtained Co2P@3D-rGO/NF electrode exhibits superior HER activity in 1.0 M KOH media, achieving overpotentials of 36.5 and 264.7 mV at current densities of 10 and 100 mA cm-2, respectively. The electrode also has a low Tafel slope of 55.5 mV dec-1, a large electrochemical surface area, and small charge-transfer resistance, further revealing its mechanism of high intrinsic activity. Moreover, the electrode exhibits excellent HER stability and durability without surface morphology and chemical state changes.

7.
Dalton Trans ; 51(16): 6390-6398, 2022 Apr 20.
Artigo em Inglês | MEDLINE | ID: mdl-35388395

RESUMO

With a high specific capacity, MoP2 has been identified as an ideal electrode material for LIBs. However, the specific capacity is negatively affected due to its poor conductivity and severe volume expansion during insertion and extraction of Li+. In this paper, MoP2-C synthesized by using a Mo-MOF as a precursor, with the generation of C, can effectively solve the agglomeration problem in the synthesis process and alleviate serious volume changes during cycling. Due to the lack of carbon sources provided by a Mo-MOF, the conductivity of MoP2-C cannot be greatly improved. Therefore, rGO and PPy are added to improve the conductivity of MoP2 and further increase the stability of the structure. Compared with MoP2/C and MoP2/C@PPy, MoP2/C@rGO exhibits the highest initial discharge specific capacity of 1208 mA h g-1 at a current density of 100 mA g-1 and rate performances of 830, 750, 630, 550, and 430 mA h g-1 with the current density increasing from 100 mA g-1 to 2000 mA g-1. Notably, the specific capacity remains at 640 mA h g-1 at a current density of 100 mA g-1 after 100 cycles. Followed by 200 cycles at a current density of 2000 mA h g-1, the specific capacity remains at 395 mA h g-1 with a capacity retention rate of 80%.

8.
Artigo em Inglês | MEDLINE | ID: mdl-34961306

RESUMO

Organic-inorganic perovskites face the issues of being vulnerable to oxygen and moisture and the trap sites located at the surface and grain boundaries. Integration of two-dimensional (2D) perovskites as a capping layer is an effective route to enhance both photovoltaic efficiency and environmental stability of the three-dimensional (3D) underlayer. Here, we employ 1,4-butanediammonium diiodide (BDADI), which has a short chain length and diammonium cations, to construct a 3D/2D stacking perovskite solar cells (PSCs). The introduction of BDA2+ could passivate surface defects in 3D perovskites by forming 2D Dion-Jacobson (DJ) phase perovskites and effectively suppressing nonradiative recombination, thus resulting in a longer carrier lifetime. The DJ 2D capping layer also regulate the energy level arrangement, enabling a better charge extraction and transport process. In addition, the water-resistance ability of 3D perovskite gets improved because of the hydrophobic characteristic of 1,4-butanediammonium cations. Consequently, the 3D/2D stacking PSCs yield an energy conversion efficiency of 20.32% in company with the enhanced long-term stability.

9.
ACS Appl Mater Interfaces ; 13(43): 51057-51065, 2021 Nov 03.
Artigo em Inglês | MEDLINE | ID: mdl-34672534

RESUMO

Benefiting from the advantages of cost-effectiveness and sustainability, lithium-ion batteries (LIBs) are recognized as a next-generation energy technology with great development potential. Herein, niobium oxide hydrate (H3ONb3O8) synthesized by a facile and inexpensive solvothermal method is proposed as the anode of LIBs. It is a layered two-dimensional material composed of negatively charged two-dimensional lamellae and positively charged interlayer hydronium ions. The former consist of NbO6 octahedral units connected by bridging oxygen. Because of the mutual effect of hydronium ions and niobium oxide quantum dots, niobium oxide hydrate exhibits excellent electrochemical activity when used as an anode material. This compound is first applied to lithium-ion batteries, obtaining a high specific capacity (1232 mAh g-1) at 100 mA g-1 and maintaining an outstanding performance after 200 cycles. Therefore, this work not only proposes a simple preparation method of niobium oxide hydrate but also expands the variety of high-performance anode materials.

10.
Dalton Trans ; 50(28): 9775-9786, 2021 Jul 21.
Artigo em Inglês | MEDLINE | ID: mdl-34180480

RESUMO

In this work, a honeycomb-shaped meso@mesoporous carbon nanofiber material incorporating homogeneously dispersed ultra-fine Fe2O3 nanoparticles (denoted as Fe2O3@g-C3N4@H-MMCN) is synthesised through a pyrolysis process. The honeycomb-shaped configuration of the meso@mesoporous carbon nanofiber material derived from a natural bio-carbon source (crab shell) acts as a support for an anode material for Li-ion batteries. Graphitic carbon nitride (g-C3N4) is produced via the one-step pyrolysis of urea at high temperature under an N2 atmosphere without the assistance of additives. The resulting favorable electrochemical performance, with superior rate capabilities (1067 mA h g-1 at 1000 mA g-1), a remarkable specific capacity (1510 mA h g-1 at 100 mA g-1), and steady cycling performance (782.9 mA h g-1 after 500 cycles at 2000 mA g-1), benefitted from the advantages of both the host material and the Fe2O3 nanoparticles, which play an important role due to their ultra-fine particle size of 5 nm. The excellent cycle life and high capacity demonstrate that this strategy of strong synergistic effects represents a new pathway for pursuing high-electrochemical-performance materials for lithium-ion batteries.

11.
Dalton Trans ; 50(10): 3660-3670, 2021 Mar 16.
Artigo em Inglês | MEDLINE | ID: mdl-33629984

RESUMO

Gallium oxide as a novel electrode material has attracted attention because of its high stability and conductivity. In addition, Ga2O3 will be converted to Ga during the charge and discharge process, and the self-healing behavior of Ga can improve the cycling stability. In this paper, we synthesized Ga2O3 nanoparticles with a size of about 4 nm via a facile sol-gel method. Meanwhile, we employed three types of carbon materials (reduced graphene oxide, mesoporous carbon nanofiber arrays, and carbon nanotubes) to avoid the aggregation of Ga2O3 nanoparticles and improve the conductivity of Ga2O3 during the discharge/charge process as well. Among the three samples, the deactivating defective sites and special carbon matrix of reduced graphene oxide can provide more attachment points for Ga ions, so the Ga2O3 nanoparticles can be more closely and uniformly distributed on rGO. Benefitting from the perfect combination of reduced graphene oxide sheets and Ga2O3 nanoparticles, a stable capacity of the Ga2O3/rGO electrode can be maintained at 411 mA h g-1 at a current density of 1000 mA g-1 after 600 cycles. We believe that this work provides a novel and efficient way to improve the electrochemical stability of Li-ion batteries.

12.
ACS Appl Mater Interfaces ; 12(47): 52864-52872, 2020 Nov 25.
Artigo em Inglês | MEDLINE | ID: mdl-33174724

RESUMO

Mg-MOF-74/Cu was synthesized by a one-step method and then using the product as a lithium-ion anode material. The flocculent Cu caused by the Jahn-Teller effect conspicuously improves the electrochemical performance of Mg-MOF-74 by enhancing the conductivity of electrode materials. The as-prepared materials exhibited superior rate performance (298.3 mAh g-1 at a current density of 2000 mA g-1) and remarkable cyclability (a specific capacity of 534.5 mAh g-1 is obtained after 300 cycles at 500 mA g-1, which remains at 89.1%). In addition, an electrochemical test of coating an anode material on a stainless steel sheet has also been carried out, and the performance is comparable to that of traditional coating on copper foil (a reversible capacity of 531.7 mAh g-1 is collected, which retains 88.7% of initial capacity). The superior performance, facile one-step synthesis, and low cost of Mg-MOF-74/Cu show promise for practical applications.

13.
J Colloid Interface Sci ; 573: 78-86, 2020 Aug 01.
Artigo em Inglês | MEDLINE | ID: mdl-32259694

RESUMO

Inorganic p-type materials show great potential as the hole transport layer in perovskite solar cells with the merits of low costs and enhanced chemical stability. As a p-type material, cobalt oxide (CoO) has received so far not that level of attention despite its high hole mobility. Herein, solution-processed p-type CoO nanocrystalline films are developed for inverted mixed perovskite solar cells. The ultrafine CoO nanocrystals are synthesized via an oil phase method, which are subsequently treated by a ligand exchange process using pyridine solvent to remove the long alkyl chains covering the nanocrystals. From this homogeneous colloidal solution CoO films are obtained, which exhibit a smooth and pin-hole free surface morphology with high transparency and good conductivity. The ultraviolet photoelectron spectrum also indicates that the energy levels of the CoO film match well with the mixed perovskite Cs0.05(FA0.83MA0.17)0.95(I0.83Br0.17)3. Inverted solar cells based on crystalline CoO films with ligand exchange show a reasonable energy conversion efficiency, whereas devices based on CoO films without ligand exchange suffer from a strong S-shape JV-characteristic. Thus, the crystalline CoO films are foreseen to pave a new way of inorganic hole transport materials in the fields of perovskite solar cells.

14.
Dalton Trans ; 48(33): 12386-12390, 2019 Sep 07.
Artigo em Inglês | MEDLINE | ID: mdl-31397458

RESUMO

A Ga/Ga2O3@C dodecahedron composite with a high specific capacity of about 542 mA h g-1 after 200 cycles at the current density of 1000 mA g-1 was synthesized by one-step hydrogen reduction. This hierarchical homogeneous structure combined the Ga, Ga2O3 and carbon frameworks (from Ga-MOF) to exhibit excellent electrochemical performance.

15.
Dalton Trans ; 48(27): 10191-10198, 2019 Jul 21.
Artigo em Inglês | MEDLINE | ID: mdl-31190031

RESUMO

In this work, we synthesized a novel UIO-67@Se@PANI composite cathode material for Li-Se battery applications. Zr-MOFs (metal organic frameworks) were used as a support and a PANI (polyaniline) layer was employed as the coating. UIO-67@Se@PANI was expected to be one of the candidates for Li-Se batteries, with a high specific capacity of 248.3 mA h g-1 at 1C (1C = 675 mA g-1) after 100 cycles. In particular, stable capacities of 203.1 and 167.6 mA h g-1 were received after 100 cycles at high rates of 2C and 5C, respectively. To explain such a good electrochemistry performance of the composite cathode material, multiple characterization methods were carried out. And that can be attributed to the sandwich-like structure of the UIO-67@Se@PANI composite and the fact that UIO-67 can provide unsaturated sites to tether the selenium effectively and the PANI layer can improve the electronic conductivity of the whole electrode significantly.

16.
Dalton Trans ; 48(5): 1906-1914, 2019 Feb 07.
Artigo em Inglês | MEDLINE | ID: mdl-30656345

RESUMO

Bi2S3 is a promising negative electrode material for lithium storage owing to its high theoretical capacity. Nevertheless, the capacity of Bi2S3 decays very rapidly upon Li cycling. Here, Bi2S3 and Bi2S3/C were successfully synthesized by a novel route. Sulfur powder as a kind of sulfur source reacted with a metal organic framework based on bismuth and trimesinic acid-Bi(BTC)(DMF)·DMF·(CH3OH)2 (denoted as Bi-BTC). Trimesic acid further acted as a new type of carbon source to synthesize the Bi2S3/C composite. The particle sizes of the composite were smaller than those of pure Bi2S3, showing the suppression of Bi2S3 aggregation. Charge-discharge performance and cyclability for both the Bi2S3 and Bi2S3/C composites in lithium-ion batteries were measured. Specifically, the specific capacities of Bi2S3/C and Bi2S3 reached 765 and 603 mA h g-1, respectively, at 100 mA g-1 after 100 cycles. Because of its high capacity and excellent cycle life, Bi2S3/C is a promising energy storage material.

17.
J Nanosci Nanotechnol ; 19(1): 263-267, 2019 Jan 01.
Artigo em Inglês | MEDLINE | ID: mdl-30327034

RESUMO

The new demands for energy storage systems have been placed with demands for flexible wearable electronics. Herein, rugby-like GeO2 nanoparticles (NPs) have been directly grown on carbon cloth (GeO2 NPs/CC) through a one-step hydrolysis process at room temperature, which can be used as a self-supporting flexible anode for lithium ion battery (LIBs). The rugby-like GeO2 NPs/CC showed an improved lithium-storage performance with features of high reversible capacity ~2000 mA·h·g-1 even after 100 cycles and good cycling stability. Besides, its initial coulomb efficiency (79.1%) was also enhanced compared to that of some reported GeO2-based materials.

18.
ACS Appl Mater Interfaces ; 10(41): 35385-35394, 2018 Oct 17.
Artigo em Inglês | MEDLINE | ID: mdl-30152674

RESUMO

One major drawback that prevents the large-scale practical implementation of perovskites is their susceptibility to performance degradation in humid environments. Here, we achieved uniform, stable perovskite films within a polyvinylpyrrolidone (PVP) polymer frame via mild solution processing in ambient air with over 60% relative humidity. In addition to facilitating film formation, the hydrophobic PVP served to protect the perovskite grains from atmospheric moisture. Use of PVP, coupled with optimization of the deposition parameters, provided for compact, smooth, pinhole-free perovskite films that when incorporated into a photovoltaic device exhibited highly reproducible efficiencies in the range of up to 17%. In the absence of encapsulation, the devices exhibited stable performance characteristics during exposure to humid ambient air for 600 h. Furthermore, on flexible substrates, the 8 wt % PVP-perovskite samples provided for device efficiencies of ca. 15%. The devices retained ca. 73% of their efficiency after bending 1000 times with a bending radius of 0.5 cm.

19.
ACS Appl Mater Interfaces ; 9(50): 43724-43732, 2017 Dec 20.
Artigo em Inglês | MEDLINE | ID: mdl-29182302

RESUMO

Mesoporous titania is a cheap and widely used material for photovoltaic applications. To enable a large-scale fabrication and a controllable pore size, we combined a block copolymer-assisted sol-gel route with spray coating to fabricate titania films, in which the block copolymer polystyrene-block-poly(ethylene oxide) (PS-b-PEO) is used as a structure-directing template. Both the macroscale and nanoscale are studied. The kinetics and thermodynamics of the spray deposition processes are simulated on a macroscale, which shows a good agreement with the large-scale morphology of the spray-coated films obtained in practice. On the nanoscale, the structure evolution of the titania films is probed with in situ grazing incidence small-angle X-ray scattering (GISAXS) during the spray process. The changes of the PS domain size depend not only on micellization but also on solvent evaporation during the spray coating. Perovskite (CH3NH3PbI3) solar cells (PSCs) based on sprayed titania film are fabricated, which showcases the suitability of spray-deposited titania films for PSCs.

20.
Nanoscale ; 5(24): 12574-81, 2013 Dec 21.
Artigo em Inglês | MEDLINE | ID: mdl-24173030

RESUMO

TiO2 microspheres assembled by single crystalline rutile TiO2 nanorods were synthesized by one-pot solvothermal treatment at 180 °C based on an aqueous-organic mixture solution containing n-hexane, distilled water, titanium n-butoxide and hydrochloric acid. The spheres had a radiative structure from the center, and their diameters were controlled in the range from 1 to 5 µm by adjusting the volume of the reactant water. Nitrogen adsorption-desorption isotherms showed that all the as-prepared microspheres had relatively high specific surface areas of about 50 m(2) g(-1). The 1 µm sized TiO2 nanorod microspheres were fabricated as a scattering overlayer in DSSCs, leading to a remarkable improvement in the power conversion efficiency: 8.22% of the bi-layer DSSCs versus 7.00% for the reference cell made of a single-layer film prepared from nanocrystalline TiO2. Such improvement was mainly attributed to the enhanced light harvesting and dye loading brought by the effective scattering centers.

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