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1.
Small ; 20(6): e2306195, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-37789582

RESUMO

The poor reversibility and stability of Zn metal anode (ZMA) caused by uncontrolled Zn deposition behaviors and serious side reactions severely impeded the practical application of aqueous Zn metal battery. Herein, a liquid-dynamic and self-adaptive protective layer (LSPL) was constructed on the ZMA surface for inhibiting dendrites and by-products formation. Interestingly, the outer LSPL consists of liquid perfluoropolyether (PFPE), which can dynamically adapt volume change during repeat cycling and inhibit side reactions. Moreover, it can also decrease the de-solvation energy barrier of Zn2+ by strong interaction between C-F bond and foreign Zn2+ , improving Zn2+ transport kinetics. For the LSPL inner region, in-situ formed ZnF2 through the spontaneous chemical reaction between metallic Zn and part PFPE can establish an unimpeded Zn2+ migration pathway for accelerating ion transfer, thereby restricting Zn dendrites formation. Consequently, the LSPL-modified ZMA enables reversible Zn deposition/dissolution up to 2000 h at 1 mA cm-2 and high coulombic efficiency of 99.8% at 4 mA cm-2 . Meanwhile, LSPL@Zn||NH4 V4 O10 full cells deliver an ultralong cycling lifespan of 100 00 cycles with 0.0056% per cycle decay rate at 10 A g-1 . This self-adaptive layer provides a new strategy to improve the interface stability for next-generation aqueous Zn battery.

2.
Chemistry ; 30(21): e202304152, 2024 Apr 11.
Artigo em Inglês | MEDLINE | ID: mdl-38311589

RESUMO

Due to the ultrahigh theoretical specific capacity (3860 mAh g-1) and low redox potential (-3.04 V vs. standard hydrogen electrode), Lithium (Li) metal anode (LMA) received increasing attentions. However, notorious dendrite and volume expansion during the cycling process seriously hinder the development of high energy density Li metal batteries. Constructing three-dimensional (3D) current collectors for Li can fundamentally solve the intrinsic drawback of hostless for Li. Therefore, this review systematically introduces the design and synthesis engineering and the current development status of different 3D collectors in recent years (the current collectors are divided into two major parts: metal-based current collectors and carbon-based current collectors). In the end, some perspectives of the future promotion for LMA application are also presented.

3.
Small ; 19(12): e2205936, 2023 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-36634970

RESUMO

It remains a great challenge to design and manufacture battery-type supercapacitors with satisfactory flexibility, appropriate mechanical property, and high energy density under high power density. Herein, a concept of porous engineering is proposed to simply prepare two-layered bimetallic heterojunction with porous structures. This concept is successfully applied in fabrication of flexible electrode based on CuO-Co(OH)2 lamella on Cu-plated carbon cloth (named as CPCC@CuO@Co(OH)2 ). The unique structure brings the electrode a high specific capacity of 3620 mF cm-2 at 2 mA cm-2 and appropriate mechanical properties with Young's modulus of 302.0 MPa. Density functional theory calculations show that porous heterojunction provides a higher intensity of electron state density near the Fermi level (E-Ef  = 0 eV), leading to a highly conductive CPCC@CuO@Co(OH)2 electrode with both efficient charge transport and rapid ion diffusion. Notably, the supercapacitor assembled from CPCC@CuO@Co(OH)2 //CC@AC shows high energy density of 127.7 W h kg-1 at 750.0 W kg-1 , remarkable cycling performance (95.53% capacity maintaining after 10 000 cycles), and desired mechanical flexibility. The methodology and results in this work will accelerate the transformative developments of flexible energy storage devices in practical applications.

4.
Small ; 19(31): e2206597, 2023 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-36617512

RESUMO

Electrolyte additive is an effective strategy to inhibit the uncontrolled growth of Li dendrites for lithium metal batteries (LMBs). However, most of the additives are complex synthesis and prone to decompose in cycling. Herein, in order to guide the homogeneous deposition of Li+ , carbonized polymer dots (CPDs) as electrolyte additives are successfully designed and synthesized by microwave (M-CPDs) and hydrothermal (H-CPDs) approaches. The controllable functional groups containing N or O (especially pyridinic-N, pyrrolic-N, and carboxyl group) enable CPDs to keep stable in electrolytes for at least 3 months. Meanwhile, the clusters formed between CPDs and Li+ through electrostatic interaction effectively guide the uniform Li dispersion and limit the "tip effect" and dendrite formation. Moreover, as lithiophilic groups increase, the strong electrostatic interference for the solvation effect of Li+ in the electrolyte is formed, which induces faster Li+ diffusion/transfer. As expected, H-CPDs achieve the ultra-even Li+ transfer. The corresponding Li//LiFePO4 full cell delivers a high capacity retention rate of 93.8% after 200 cycles, which is much higher than that of the cells without additives (61.2%) and with M-CPDs (83.7%) as additives. The strategy in this work provides a theoretical direction for CPDs as electrolyte additives used in energy storage devices.

5.
Small ; 19(47): e2304751, 2023 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-37485645

RESUMO

The dendrite growth and parasitic reactions that occur on Zn metal anode (ZMA)/electrolyte interface hinder the development of aqueous zinc ion batteries (AZIBs) in next-generation renewable energy storage systems. Fortunately, reconstructing the inner Helmholtz layer (IHL) by introducing an electrolyte additive, is viewed as one of the most promising strategies to harvest the stable ZMA. Herein, (4-chloro-3-nitrophenyl) (pyridin-4-yl) methanone (CNPM) with quadruple functional groups is introduced into the ZnSO4 electrolyte to reshape the interface between ZMA and electrolyte and change the solvation structure of Zn2+ . Density functional theory (DFT) calculations manifest that the ─C═O, ─Cl, ─C═N─, and ─NO2 functional groups of CNPM interact with metallic Zn simultaneously and adsorb on the ZMA surface in a parallel arrangement manner, thus forming a water-poor IHL and creating well-arranged ion transportation channels. Furthermore, theoretical calculations and experimental results demonstrate that CNPM absorbed on the Zn anode surface can serve as zincophilic sites for inducing uniform Zn deposition along the (002) plane. Benefiting from the synergistic effect of these functions, the dendrite growth and parasitic reactions are suppressed significantly. As a result, ZMA exhibits a long cycle life (2900 h) and high coulombic efficiency (CE) (500 cycles) in the ZnSO4 +CNPM electrolyte.

6.
Small ; 19(52): e2304459, 2023 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-37649202

RESUMO

Despite being one of the most promising materials in anode materials, molybdenum sulfide (MoS2 ) encounters certain obstacles, such as inadequate cycle stability, low conductivity, and unsatisfactory charge-discharge (CD) rate performance. In this study, a novel approach is employed to address the drawbacks of MoS2 . Carbon polymer dots (CPDs) are incorporated to prepare three-dimensional (3D) nanoflower-like spheres of MoS2 @CPDs through the self-assembly of MoS2 2D nanosheets, followed by annealing at 700 °C. The CPDs play a main role in the creation of the nanoflower-like spheres and also mitigate the MoS2 nanosheet limitations. The nanoflower-like spheres minimize volume changes during cycling and improve the rate performance, leading to exceptional rate performance and cycling stability in both Lithium-ion and Sodium-ion batteries (LIBs and SIBs). The optimized MoS2 @CPDs-2 electrode achieves a superb capacity of 583.4 mA h g-1 at high current density (5 A g-1 ) after 1000 cycles in LIBs, and the capacity remaining of 302.8 mA h g-1 after 500 cycles at 5 A g-1 in SIBs. Additionally, the full cell of LIBs/SIBs exhibits high capacity and good cycling stability, demonstrating its potential for practical application in fast-charging and high-energy storage.

7.
Opt Express ; 31(15): 25013-25024, 2023 Jul 17.
Artigo em Inglês | MEDLINE | ID: mdl-37475315

RESUMO

Improving imaging quality and reducing time consumption are the key problems that need to be solved in the practical application of ghost imaging. Hence, we demonstrate a double filter iterative ghost imaging method, which adopts the joint iteration of projected Landweber iterative regularization and double filtering based on block matching three dimensional filtering and guided filtering to achieve high-quality image reconstruction under low measurement and low iteration times. This method combines the advantages of ill-posed problem solution of projected Landweber iterative regularization with double filtering joint iterative de-noising and edge preservation. The numerical simulation results show that our method outperforms the comparison method by 4 to 6 dB in terms of peak signal-to-noise ratio for complex binary target 'rice' and grayscale target 'aircraft' after 1500 measurements. The comparison results of experiments and numerical simulations using similar aircraft targets show that this method is superior to the comparison method, especially in terms of richer and more accurate edge detection results. This method can simultaneously obtain high quality reconstructed image and edge feature information under low measurement and iteration times, which is of great value for the practical application fields of imaging and edge detection at the same time, such as intelligent driving, remote sensing and other fields.

8.
Nanotechnology ; 34(40)2023 Jul 19.
Artigo em Inglês | MEDLINE | ID: mdl-37369182

RESUMO

Although significant achievements in improving the stability of MoS2anodes have been made, the cycling life in most studies is still less than 1000 cycles. This is because MoS2anodes directly contact the electrolyte and generate byproducts, leading to the loss of active mass and capacity decay. Herein, the inner-outer dual space protection of MoS2fibers is realized by regulating the surface and interface structure of electrospinning precursors (noted as X-MoS2/CNFs). Inside the fibers, Mo-N covalent bond is constructed to anchor the active material, preventing MoS2from falling off the matrix after multiple cycles. Simultaneously, surface of the fibers, a stable solid electrolyte interface layer is induced to prevent contact between active materials and electrolytes. In addition, the initial Coulombic efficiency is enhanced as high as 84.4%. The profound investigations of morphological evolution and internal real-time resistance confirm the double structural protection of 800-MoS2/CNFs. As a result, a decent cycling performance (408.9 mAh g-1at 1000 mA g-1for 2000 cycles) and the satisfied rate capacities (100-1000 mA g-1) are achieved. This work provides a new idea for the preparation of stable anodes for alkali metal ion secondary batteries.

9.
Angew Chem Int Ed Engl ; 62(45): e202308182, 2023 Nov 06.
Artigo em Inglês | MEDLINE | ID: mdl-37750328

RESUMO

Zn-I2 batteries have attracted attention due to their low cost, safety, and environmental friendliness. However, their performance is still limited by the irreversible growth of Zn dendrites, hydrogen evolution reactions, corrosion, and shuttle effect of polyiodide. In this work, we have prepared a new porous polymer (CD-Si) by nucleophilic reaction of ß-cyclodextrin with SiCl4 , and CD-Si is applied to the solid polymer electrolyte (denoted PEO/PVDF/CD-Si) to solve above-mentioned problems. Through the anchoring of the CD-Si, a conductive network with dual transmission channels was successfully constructed. Due to the non-covalent anchoring effect, the ionic conductivity of the solid polymer electrolytes (SPE) can reach 1.64×10-3  S cm-1 at 25 °C. The assembled symmetrical batteries can achieve highly reversible dendrite-free galvanizing/stripping (stable cycling for 7500 h at 5 mA cm-2 and 1200 h at 20 mA cm-2 ). The solid-state Zn-I2 battery shows an ultra-long life of over 35,000 cycles at 2 A g-1 . Molecular dynamics simulations are performed to elucidate the working mechanism of CD-Si in the polymer matrix. This work provides a novel strategy towards solid electrolytes for Zn-I2 batteries.

10.
Angew Chem Int Ed Engl ; 62(7): e202216934, 2023 Feb 06.
Artigo em Inglês | MEDLINE | ID: mdl-36478517

RESUMO

Uncontrolled dendrites growth and serious parasitic reactions in aqueous electrolytes, greatly hinder the practical application of aqueous zinc-ion battery. On the basis of in situ-chemical construction and performance-improving mechanism, multifunctional fluoroethylene carbonate (FEC) is introduced into aqueous electrolyte to construct a high-quality and ZnF2 -riched inorganic/organic hybrid SEI (ZHS) layer on Zn metal anode (ZMA) surface. Notably, FEC additive can regulate the solvated structure of Zn2+ to reduce H2 O molecules reactivity. Additionally, the ZHS layer with strong Zn2+ affinity can avoid dendrites formation and hinder the direct contact between the electrolyte and anode. Therefore, the dendrites growth, Zn corrosion, and H2 evolution reaction on ZMA in FEC-included ZnSO4 electrolyte are highly suppressed. Thus, ZMA in such electrolyte realize a long cycle life over 1000 h and deliver a stable coulombic efficiency of 99.1 % after 500 cycles.

11.
Chemistry ; 27(31): 8168-8177, 2021 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-33783042

RESUMO

Lithium metal anodes (LMAs) with high energy density have recently captured increasing attention for development of next-generation batteries. However, practical viability of LMAs is hindered by the uncontrolled Li dendrite growth and infinite dimension change. Even though constructing 3D conductive skeleton has been regarded as a reliable strategy to prepare stable and low volume stress LMAs, engineering the renewable and lithiophilic conductive scaffold is still a challenge. Herein, a robust conductive scaffold derived from renewable cellulose paper, which is coated with reduced graphene oxide and decorated with lithiophilic Au nanoparticles, is engineered for LMAs. The graphene cellulose fibres with high surface area can reduce the local current density, while the well-dispersed Au nanoparticles can serve as lithiophilic nanoseeds to lower the nucleation overpotential of Li plating. The coupled relationship can guarantee uniform Li nucleation and unique spherical Li growth into 3D carbon matrix. Moreover, the natural cellulose paper possesses outstanding mechanical strength to tolerate the volume stress. In virtue of the modulated deposition behaviour and near-zero volume change, the hybrid LMAs can achieve reversible Li plating/stripping even at an ultrahigh current density of 10 mA cm-2 as evidenced by high Coulombic efficiency (97.2 % after 60 cycles) and ultralong lifespan (1000 cycles) together with ultralow overpotential (25 mV). Therefore, this strategy sheds light on a scalable approach to multiscale design versatile Li host, promising highly stable Li metal batteries to be feasible and practical.

12.
Chemistry ; 26(4): 853-862, 2020 Jan 16.
Artigo em Inglês | MEDLINE | ID: mdl-31691394

RESUMO

The Fe-based transition metal oxides are promising anode candidates for lithium storage considering their high specific capacity, low cost, and environmental compatibility. However, the poor electron/ion conductivity and significant volume stress limit their cycle and rate performances. Furthermore, the phenomena of capacity rise and sudden decay for α-Fe2 O3 have appeared in most reports. Here, a uniform micro/nano α-Fe2 O3 nanoaggregate conformably enclosed in an ultrathin N-doped carbon network (denoted as M/N-α-Fe2 O3 @NC) is designed. The M/N porous balls combine the merits of secondary nanoparticles to shorten the Li+ transportation pathways as well as alleviating volume expansion, and primary microballs to stabilize the electrode/electrolyte interface. Furthermore, the ultrathin carbon shell favors fast electron transfer and protects the electrode from electrolyte corrosion. Therefore, the M/N-α-Fe2 O3 @NC electrode delivers an excellent reversible capacity of 901 mA h g-1 with capacity retention up to 94.0 % after 200 cycles at 0.2 A g-1 . Notably, the capacity rise does not happen during cycling. Moreover, the lithium storage mechanism is elucidated by ex situ XRD and HRTEM experiments. It is verified that the reversible phase transformation of α↔γ occurs during the first cycle, whereas only the α-Fe2 O3 phase is reversibly transformed during subsequent cycles. This study offers a simple and scalable strategy for the practical application of high-performance Fe2 O3 electrodes.

13.
Small ; 14(47): e1803072, 2018 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-30307697

RESUMO

Water soluble nanocrystals (NCs) are promising materials in aqueous-processed solar cells because of their high extinction coefficient, low-cost, and favorable photoelectric characteristics. However, the power conversion efficiency (PCE) of the present aqueous-processed NC solar cells is restricted by the short depletion region of the active layer and limited Fermi level offset between NCs and the electron transport layer. Herein, these issues are effectively addressed by preparing Cdx Zn1- x Te NCs capped with 2-aminoethanethiol hydrochloride. The introduction of Zn2+ into CdTe NCs widens the Fermi level offset from 0.68 to 0.74 eV, lengthens the depletion region from 130 to 137 nm, and hence brings obvious improvement in the open circuit voltage (Voc ) and fill factor. Especially, the depletion region is successfully tuned from 137 to 171 nm, and even lengthened to a record thickness of 200 nm based on aqueous-processed solar cells. As a result, a champion thickness ratio (74%) of depletion region to active layer (200/270 nm) is achieved. A champion PCE of 5.96% and short-circuit current (Jsc ) of 21.2 mA cm-2 are achieved among aqueous-processed NC solar cells. This work provides a simple way to prepare polynary NCs and highlights a prospective method to develop more efficient and cost-effective solution-processed environment friendly solar cells.

14.
Inorg Chem ; 57(10): 6029-6037, 2018 May 21.
Artigo em Inglês | MEDLINE | ID: mdl-29741881

RESUMO

To develop B-O complementary-color white organic light-emitting diodes (WOLEDs) exhibiting high efficiency and low roll-off as well as color stability simultaneously, we have designed two orange iridium(III) complexes by simply controlling the position of the methoxyl group on the cyclometalated ligand. The obtained emitters mOMe-Ir-BQ and pOMe-Ir-BQ show good photophysical and electrochemical stabilities with a broadened full width at half-maximum close to 100 nm. The corresponding devices realize highly efficient electrophosphorescence with a maximum current efficiency (CE) and power efficiency (PE) of 24.4 cd A-1 and 15.3 lm W-1 at a high doping concentration of 15 wt %. Furthermore, the complementary-color all-phosphor WOLEDs based on these phosphors exhibit good performance with a maximum CE of 31.8 cd A-1, PE of 25.0 lm W-1, and external quantum efficiency of 15.5%. Particularly, the efficiency of this device is still as high as 29.3 cd A-1 and 14.2% at the practical brightness level of 1000 cd m-2, giving a small roll-off. Meanwhile, extremely high color stability is achieved by these devices with insignificant chromaticity variation.

15.
Chemistry ; 23(40): 9666-9673, 2017 Jul 18.
Artigo em Inglês | MEDLINE | ID: mdl-28508401

RESUMO

In this work, oxygen-deficient anatase TiO2 nanosheets (A-TiO2-x NSs) are proposed as a substrate to improve the electrochemical properties of sulfur electrodes for lithium-sulfur (Li-S) batteries. The A-TiO2-x NSs are prepared by partly reducing pristine TiO2 nanosheets (A-TiO2 NSs) in NaBH4 solution. With some oxygen vacancies on the surface of the TiO2 nanosheets, A-TiO2-x NSs not only promote electronic transfer, but also act as more effective polysulfide reservoirs to minimize the dissolution of lithium polysulfides (LiPSs) than the A-TiO2 NSs control. Hence, upon utilization as modifiers for cathodes of Li-S batteries, the A-TiO2-x NSs-modified sulfur (A-TiO2-x NSs-S) cathode exhibits a higher reversible specific capacity and greater cycling performance and rate capability than the A-TiO2 NSs-modified one (A-TiO2 NSs-S). For example, A-TiO2-x NSs-S delivers an initial specific capacity of 1277.1 mAh g-1 at 0.1 C and maintains a stable Coulombic efficiency of approximately 99.2 % after the first five cycles; these values are higher than those of 997.3 mAh g-1 and around 96.7 %, respectively, for A-TiO2 NSs-S. The enhanced electrochemical properties of the A-TiO2-x NSs-S cathode can be ascribed mainly to the more effective adsorption of dissolvable and diffused LiPSs by the oxygen vacancies. Therefore, utilization of the structure of oxygen vacancies in Li-S batteries demonstrates great prospects for practical application.

16.
J Org Chem ; 82(23): 12813-12820, 2017 12 01.
Artigo em Inglês | MEDLINE | ID: mdl-29076738

RESUMO

A facile and efficient copper-catalyzed azidative multifunctionalization of alkynes has been developed by using N-fluorobenzenesulfonimide (NFSI) as both nitrogen source and aryl source and trimethylsilyl azide (TMSN3) as azido source. This transformation proceeds under mild conditions, providing a series of α-azido-α-aryl imine in good yields by a single operation starting from a wide range of alkynes. The prepared α-azido-α-aryl imines could be easily converted into 1,5-piperizine-fused 1,2,3-triazoles and azido enamines.

17.
Inorg Chem ; 56(16): 9979-9987, 2017 Aug 21.
Artigo em Inglês | MEDLINE | ID: mdl-28795817

RESUMO

Nondoped electroluminescent devices offer advantages over their doped counterparts such as good reproducibility, reduced phase separation between host and guest materials, and potential of lower-cost devices. However, low luminance efficiencies and significant roll-off values are longstanding issues for nondoped devices, and a rational design strategy for the preparation of efficient phosphors is highly desired. In this work, cyclometalated Ir(III) complexes 3CzIr(mtpy), 4CzIr(mtpy), 3POIr(mtpy), and 4POIr(mtpy) bearing carbazole (Cz) or diphenylphosphoryl (Ph2PO) groups substituted at different positions of 1,2-diphenyl-H-benzimidazole (HPBI) were designed and synthesized. Owing to the steric effects induced by these groups, a significant intermolecular interaction was avoided, thereby reducing self-quenching and triplet-triplet annihilation (TTA) at high brightness. Simultaneously, attached functional moieties manipulate the charge-carrier character and enhance the EL performance of the complexes. Device N3-10, based on 3POIr(mtpy), successfully realized excellent performance and improved efficiency stability, rendering a turn-on voltage of 2.5 V, a maximum current efficiency of 29.7 cd A-1, and a maximum power efficiency of 31.1 lm W-1, which are all almost 3-fold higher than that of the control device N-10 based on parent complex. Inspiringly, all of the devices showed reduced efficiency roll-off as luminance increased. To the best of our knowledge, these are good results for green-emitting PHOLEDs using vacuum evaporation techniques, and they provide fundamental insights into the future realization of efficient phosphorescent Ir(III) complexes and corresponding nondoped devices.

18.
Phys Chem Chem Phys ; 19(25): 16576-16585, 2017 Jun 28.
Artigo em Inglês | MEDLINE | ID: mdl-28613295

RESUMO

A novel two-step solution approach is put forward to design a unique three dimensional (3D) porous ZnO-SnS p-n heterojunction under mild conditions. This special 3D structure is induced via flower-like ZnO in which SnS serves as an efficient photosensitizer to improve the light harvesting across the whole visible range. A profound investigation of the mechanism shows that this 3D porous ZnO-SnS material effectively integrates the large surface area and high redox potential of ZnO, and wide visible-light harvesting of SnS, which largely promotes the transfer and separation rate of carriers. The systematic study on the active species generated during the photocatalysis illustrates that it is the photoelectrons, ˙OH and O2˙- that play the crucial role in the degradation of dyes. As a result, the noble-metal free photocatalyst degrades nearly 100% of rhodamine B (RhB) within 80 min and methylene blue (MB) in 40 min under visible light. The photocatalytic activity is 10 times higher than that of the pure flower-like ZnO and two times higher than that of the SnS material. Moreover, the photocatalyst is easily separated and reused at least four times without obvious change in efficiency and properties. This work provides an effective strategy for the synthesis of 3D porous p-n heterojunction semiconductor-based photocatalysts with low cost and low toxicity, which present promising applications in the field of solar energy storage and conversion.

19.
Chemistry ; 22(10): 3513-3518, 2016 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-26836764

RESUMO

By using N-fluorobenzenesulfonimide as both the oxidant and the amination reagent, we have realized the first example of the intermolecular chalcogenative amination of alkynes, which grants facile, highly regio- and stereoselective access to chalcogenated enamides. The reaction features mild conditions, high yields and selectivities, remarkably broad substrate scope, and excellent functional group tolerance. Mechanistic studies indicate the in situ generated chalcogen imidates to be the actual reactive species, which in turn, has clarified the mechanism of related transformations. These reactions represent significant additions to the development of the highly selective amino bisfunctionalization of alkynes.

20.
Chemistry ; 22(24): 8152-7, 2016 06 06.
Artigo em Inglês | MEDLINE | ID: mdl-27136376

RESUMO

Although graphene oxide (GO) has large interlayer spacing, it is still inappropriate to use it as an anode for sodium-ion batteries (SIBs) because of the existence of H-bonding between the layers and ultralow electrical conductivity which impedes the Na(+) and e(-) transformation. To solve these issues, chemical, thermal, and electrochemical procedures are traditionally employed to reduce GO nanosheets. However, these strategies are still unscalable, consume high amounts of energy, and are expensive for practical application. Here, for the first time, we describe the superior Na storage of unreduced GO by a simple and scalable alkali-metal-ion (Li(+) , Na(+) , K(+) )-functionalized process. The various alkali metals ions, connecting with the oxygen on GO, have played different effects on morphology, porosity, degree of disorder, and electrical conductivity, which are crucial for Na-storage capabilities. Electrochemical tests demonstrated that sodium-ion-functionalized GO (GNa) has shown outstanding Na-storage performance in terms of excellent rate capability and long-term cycle life (110 mAh g(-1) after 600 cycles at 1 A g(-1) ) owing to its high BET area, appropriate mesopore, high degree of disorder, and improved electrical conductivity. Theoretical calculations were performed using the generalized gradient approximation (GGA) to further study the Na-storage capabilities of functionalized GO. These calculations have indicated that the Na-O bond has the lowest binding energy, which is beneficial to insertion/extraction of the sodium ion, hence the GNa has shown the best Na-storage properties among all comparatives functionalized by other alkali metal ions.

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