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1.
Nano Lett ; 24(5): 1695-1702, 2024 Feb 07.
Artigo em Inglês | MEDLINE | ID: mdl-38261789

RESUMO

To meet the growing demands in both energy and power densities of lithium ion batteries, electrode structures must be capable of facile electron and ion transport while minimizing the content of electrochemically inactive components. Herein, binder-free LiFePO4 (LFP) cathodes are fabricated with a multidimensional conductive architecture that allows for fast-charging capability, reaching a specific capacity of 94 mAh g-1 at 4 C. Such multidimensional networks consist of active material particles wrapped by 1D single-walled carbon nanotubes (CNTs) and bound together using 2D MXene (Ti3C2Tx) nanosheets. The CNTs form a porous coating layer and improve local electron transport across the LFP surface, while the Ti3C2Tx nanosheets provide simultaneously high electrode integrity and conductive pathways through the bulk of the electrode. This work highlights the ability of multidimensional conductive fillers to realize simultaneously superior electrochemical and mechanical properties, providing useful insights into future fast-charging electrode designs for scalable electrochemical systems.

2.
Molecules ; 29(6)2024 Mar 14.
Artigo em Inglês | MEDLINE | ID: mdl-38542935

RESUMO

The phase, mechanical properties, corrosion resistance, hydrophobicity, and interfacial contact resistance of Hastelloy X were investigated to evaluate its performance in proton exchange membrane fuel cells (PEMFCs). For comparison, the corresponding performance of 304 stainless steel (304SS) was also tested. Hastelloy X exhibited a single-phase face-centered cubic structure with a yield strength of 445.5 MPa and a hardness of 262.7 HV. Both Hastelloy X and 304SS exhibited poor hydrophobicity because the water contact angles were all below 80°. In a simulated PEMFC working environment (0.5 M H2SO4 + 2 ppm HF, 80 °C, H2), Hastelloy X exhibited better corrosion resistance than 304SS. At 140 N·cm-2, the interfacial contact resistance of Hastelloy X can reach as low as 7.4 mΩ·cm2. Considering its overall performance, Hastelloy X has better potential application than 304SS as bipolar plate material in PEMFCs.

3.
Molecules ; 29(15)2024 Aug 05.
Artigo em Inglês | MEDLINE | ID: mdl-39125100

RESUMO

Titanium (Ti) is generally considered as an ideal bipolar plate (BPP) material because of its excellent corrosion resistance, good machinability and lightweight nature. However, the easy-passivation property, which leads to increased interfacial contact resistance (ICR) and subsequently decreased cell performance, limits its large-scale commercial application in proton exchange membrane fuel cells (PEMFCs). In this paper, we proposed a NiTi alloy prepared by suction casting as a promising bipolar plate for PEMFCs. This NiTi alloy exhibits significantly decreased ICR values (16.8 mΩ cm2 at 1.4 MPa) compared with pure Ti (88.6 mΩ cm2 at 1.4 MPa), along with enhanced corrosion resistance compared with pure nickel (Ni). The superior corrosion resistance of NiTi alloy is accredited to the nobler open circuit potential and corrosion potential, coupled with low corrosion current densities and passive current densities. The improved ICR can be interpreted by the existence of high-proportioned metallic Ni in the passive film, which contributes to the reduced capacitance characteristic of the passive film (compared with Ti) and enhances charge conduction. This work provides a feasible option to ameliorate BPP material that may have desirable corrosion resistance and ICR.

4.
Nano Lett ; 22(24): 10232-10239, 2022 Dec 28.
Artigo em Inglês | MEDLINE | ID: mdl-36367407

RESUMO

Patterned electrodes were developed for use in solid-state lithium-ion batteries, with the ultimate goal to promote fast-charging attributes through improving electrochemically activated surfaces within electrodes. By a conventional photolithography, patterned arrays of SnO2 nanowires were fabricated directly on the current collector, and empty channel structures formed between the resulting arrays were customized through modifying the size and interval of the SnO2 patterns. The composite electrolyte comprising Li7La3Zr2O12 and poly(ethylene oxide) was exploited to secure intimate interfacial contact at the electrode/electrolyte junction while preserving ionic conductivity in the bulk electrolyte. The potential and limitation of the electrode patterning approach were then explored experimentally. For example, the electrochemical behaviors of patterned electrodes were investigated as a function of variations in microchannel structures, and compared with those of conventional film-type electrodes. The findings show promise to improve electrode dynamics when electrochemical reaction kinetics could be hindered by poor interfacial characteristics on electrodes.

5.
Molecules ; 28(6)2023 Mar 21.
Artigo em Inglês | MEDLINE | ID: mdl-36985793

RESUMO

In order to obtain films with high corrosion resistance and excellent interfacial contact resistance (ICR) on 316L stainless steel used for bipolar plates in proton-exchange membrane fuel cells (PEMFCs), Cr, Ti co-doped amorphous carbon films were prepared on 316L stainless steel. The preparation method for the coating was magnetron sputtering. The doping amount of the Ti element was controlled by a Cr target and a Ti target current. The change in the structure and properties of the coating after the change from Cr single-element doping to Cr and Ti co-doping was studied. The change rule of the structure and properties of the coating from Cr single-element doping to Cr and Ti co-doping was studied. An increase in the Ti content led to a decreased grain boundary, a flatter surface, and a higher sp2-hybridized carbon content. TiC and CrC nanocrystals were formed in the amorphous carbon structure together. The amorphous carbon films doped with Cr and Ti simultaneously achieved a low ICR and high corrosion resistance compared with single-Cr-doped amorphous carbon. The enhanced corrosion resistance was attributed to the decreasing grain boundary, the formation of the TiC crystal structure, and the smaller grain size. The best performance was obtained at a Ti target current of 2A. Compared with bare 316L stainless steel, the corrosion resistance of Cr, Ti co-doped amorphous carbon (Icorr = 5.7 × 10-8 A/cm2, Ti-2 sample) was greatly improved. Because Ti doping increased the content of sp2-hybridized carbon in the coating, the contact resistance of the coating decreased. Moreover, the interfacial contact resistance was 3.1 mΩ·cm2 in the Ti-2 sample, much lower than that of bare 316L stainless steel. After the potentiostatic polarization test, the coating still had excellent conductivity.

6.
Small ; 18(24): e2201694, 2022 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-35578914

RESUMO

Inverted perovskite solar cells (PSCs) have received widespread attention due to their facile fabrication and wide applications. However, their power conversion efficiency (PCE) is reported lower than that of regular PSCs because of the undesirable interfacial contact between perovskite and the hydrophobic hole transport layer (HTL). Here, an interface regulation strategy is proposed to overcome this limitation. A small molecule ([2-(9H-carbazol-9-yl) ethyl] phosphonic acid, abbreviated as 2P), composed of carbazole and phosphonic acid groups, is inserted between perovskite and HTL. Morphological characterization and theoretical calculation reveal that perovskite bonds stronger on 2P-modified HTL than on pristine HTL. The improved interfacial contact facilitates hole extraction and retards degradation. Upon the incorporation of 2P, inverted PSCs deliver a high PCE of over 22% with superior stability, keeping 84.6% of initial efficiency after 7200 h storage under an ambient atmosphere with a relative humidity of ≈30-40%. This strategy provides a simple and efficient way to boost the performance of inverted PSCs.

7.
Environ Res ; 214(Pt 3): 113948, 2022 11.
Artigo em Inglês | MEDLINE | ID: mdl-35940228

RESUMO

Designing intimate interfacial contact between nanostructures and two-dimensional (2D) materials is highly desirable to influence the movement of generated charge carriers. Nanostructured zinc oxide (ZnO) is a fascinating material with unique optical and electrical properties. 2D reduced graphene oxide (rGO) exhibits semiconductor behaviour with tunable catalytic activity and excellent biocompatibility. Hence, we have designed a hybrid material by selecting nanostructures of an oxide semiconductor (ZnO) with reduced graphene oxide (rGO) using a hard integration technique followed by a low-temperature hydrothermal route. The good encapsulation of rGO over the ZnO nanorods was confirmed by powder X-ray diffraction, scanning electron microscopy, transmission electron microscopy, Fourier transform infrared spectroscopy, and Raman spectroscopy. The photocatalytic activities of ZnO, rGO, and ZnO/rGO were studied under visible-light irradiation using three different toxic dyes, methylene blue (MB), methyl orange (MO), and Congo red (CR). The composite materials exhibited excellent efficiencies of 100, 95, and 90% for the degradation of MB, MO, and CR, respectively. Moreover, the degradation of the dye was found to follow first-order kinetics. The enhanced efficiencies are attributed to the adsorption and efficient charge transfer from rGO to the conduction band of ZnO. The role of the multifunctional facets of graphene was presented to elucidate the visible-light activity of the composite materials for enhanced efficiency. The main reactive species (e-) of the reduction reaction were confirmed through a radical trapping experiment, which showed the generation of highly reactive •OH radicals that decompose the toxic dye. The results provide a perspective for developing graphene-based composite materials with desired preselected nanostructures for solar energy utilisation.


Assuntos
Grafite , Nanoestruturas , Óxido de Zinco , Catálise , Corantes , Vermelho Congo , Grafite/química , Azul de Metileno/química , Nanoestruturas/química , Óxido de Zinco/química
8.
Sensors (Basel) ; 22(3)2022 01 19.
Artigo em Inglês | MEDLINE | ID: mdl-35161496

RESUMO

Bipolar Plates (BPPs) are the most crucial component of the Polymer Electrolyte Membrane (PEM) fuel cell system. To improve fuel cell stack performance and lifetime, corrosion resistance and Interfacial Contact Resistance (ICR) enhancement are two essential factors for metallic BPPs. One of the most effective methods to achieve this purpose is adding a thin solid film of conductive coating on the surfaces of these plates. In the present study, 410 Stainless Steel (SS) was selected as a metallic bipolar plate. The coating process was performed using titanium nitride and chromium nitride by the Cathodic Arc Evaporation (CAE) method. The main focus of this study was to select the best coating among CrN and TiN on the proposed alloy as a substrate of PEM fuel cells through the comparison technique with simultaneous consideration of corrosion resistance and ICR value. After verifying the TiN and CrN coating compound, the electrochemical assessment was conducted by the potentiodynamic polarization (PDP) and electrochemical impedance spectroscopy (EIS) tests. The results of PDP show that all coated samples have an increase in the polarization resistance (Rp) values (ranging from 410.2 to 690.6 Ω·cm2) compared to substrate 410 SS (230.1 Ω·cm2). Corrosion rate values for bare 410 SS, CrN, and TiN coatings were measured as 0.096, 0.032, and 0.060 mpy, respectively. Facilities for X-ray Diffraction (XRD), Scanning Electron Microscope (FE-SEM, TeScan-Mira III model and made in the Czech Republic), and Energy Dispersive X-ray Spectroscopy (EDXS) were utilized to perform phase, corrosion behavior, and microstructure analysis. Furthermore, ICR tests were performed on both coated and uncoated specimens. However, the ICR of the coated samples increased slightly compared to uncoated samples. Finally, according to corrosion performance results and ICR values, it can be concluded that the CrN layer is a suitable choice for deposition on 410 SS with the aim of being used in a BPP fuel cell system.

9.
Molecules ; 27(24)2022 Dec 11.
Artigo em Inglês | MEDLINE | ID: mdl-36557922

RESUMO

Highly efficient interfacial contact between components in nanohybrids is a key to achieving great photocatalytic activity in photocatalysts and degradation of organic model pollutants under visible light irradiation. Herein, we report the synthesis of nano-assembly of graphene oxide, zinc oxide and cerium oxide (GO-ZnO@CeO2) nanohybrids constructed by the hydrothermal method and subsequently annealed at 300 °C for 4 h. The unique graphene oxide sheets, which are anchored with semiconducting materials (ZnO and CeO2 nanoparticles), act with a significant role in realizing sufficient interfacial contact in the new GO-ZnO@CeO2 nanohybrids. Consequently, the nano-assembled structure of GO-ZnO@CeO2 exhibits a greater level (96.66%) of MB dye degradation activity than GO-ZnO nanostructures and CeO2 nanoparticles on their own. This is due to the thin layers of GO-ZnO@CeO2 nanohybrids with interfacial contact, suitable band-gap matching and high surface area, preferred for the improvement of photocatalytic performance. Furthermore, this work offers a facile building and cost-effective construction strategy to synthesize the GO-ZnO@CeO2 nanocatalyst for photocatalytic degradation of organic pollutants with long-term stability and higher efficiency.

10.
Molecules ; 27(19)2022 Oct 06.
Artigo em Inglês | MEDLINE | ID: mdl-36235180

RESUMO

The liquid and gas diffusion layer is a key component of proton exchange membrane water electrolyzer (PEMWE), and its interfacial contact resistance (ICR) and corrosion resistance have a great impact on the performance and durability of PEMWE. In this work, a novel hybrid coating with Au contacts discontinuously embedded in a titanium oxidized layer was constructed on a Ti felt via facile electrochemical metallizing and followed by a pre-oxidization process. The physicochemical characterizations, such as scanning electron microscopy, energy dispersive spectrometer, and X-ray diffraction results confirmed that the distribution and morphology of the Au contacts could be regulated with the electrical pulse time, and a hybrid coating (Au-TiO2/Ti) was eventually achieved after the long-term stability test under anode environment. At the compaction force of 140 N cm-2, the ICR was reduced from 19.7 mΩ cm2 of the P-Ti to 4.2 mΩ cm2 of the Au-TiO2/Ti. The corrosion current density at 1.8 V (RHE) is 0.689 µA cm-2. Both the ICR and corrosion resistance results showed that the prepared protective coating could provide comparable ICR and corrosion resistance to a dense Au coating.

11.
Nano Lett ; 16(9): 5902-8, 2016 09 14.
Artigo em Inglês | MEDLINE | ID: mdl-27504675

RESUMO

To lower the overpotential of a lithium-oxygen battery, electron transport at the solid-to-solid interface between the discharge product Li2O2 and the cathode catalyst is of great significance. Here we propose a strategy to enhance electron transport property of the cathode catalyst by the replace of oxygen atoms in the generally used metal oxide-based catalysts with nitrogen atoms to improve electron density at Fermi energy after nitridation. Hierarchically porous CoN nanorods were obtained by thermal treatment of Co3O4 nanorods under ammonia atmosphere at 350 °C. Compared with that of the pristine Co3O4 precursor before nitridation, the overpotential of the obtained CoN cathode was significantly decreased. Moreover, specific capacity and cycling stability of the CoN nanorods were enhanced. It is assumed that the discharged products with different morphologies for Co3O4 and CoN cathodes might be closely associated with the variation in the electronic density induced by occupancy of nitrogen atoms into interstitial sites of metal lattice after nitridation. The nitridation strategy for improved electron density proposed in this work is proved to be a simple but efficient way to improve the electrochemical performance of metal oxide based cathodes for lithium-oxygen batteries.

12.
Chemphyschem ; 16(15): 3214-32, 2015 Oct 26.
Artigo em Inglês | MEDLINE | ID: mdl-26336943

RESUMO

A facile three-step co-precipitation method is developed to synthesize graphitic carbon nanofibers (CNFs) decorated with ZnO nanoparticles (NPs). By interchanging intermediate steps of the reaction processes, two kinds of nanohybrids are fabricated with stark morphological and physicochemical differences. The morphologies differ because of the different chemical environments of the NP/nanocluster formation. The hybrid with larger and non-uniform ZnO nanocluster size is formed in liquid phase and resulted in considerable interfacial defects that deteriorate the charge-transfer properties. The hybrid with smaller and uniform ZnO NPs was formed in a dry solid phase and produced near-defect-free interfaces, leading to efficient charge transfer for superior photocatalytic performance. The results broaden the understanding of the anchoring/bonding mechanism in ZnO/CNF hybrid formation and may facilitate further development of more effective exfoliation strategies for the preparation of high-performance composites/hybrids.

13.
Materials (Basel) ; 17(13)2024 Jun 21.
Artigo em Inglês | MEDLINE | ID: mdl-38998129

RESUMO

Strengthening the interfacial contact between the reactive components effectively boosts the energy release of energetic materials. In this study, we aimed to create a close-knit interfacial contact condition between aluminum nanoparticles (Al NPs) and Polyvinylidene fluoride-hexafluoropropylene (P(VDF-HFP)) through hydrolytic adsorption and assembling 1H, 1H, 2H, 2H-Perfluorododecyltrichlorosilane (FTCS) on the surface of Al NPs. Leveraging hydrogen bonding between -CF and -CH and the interaction between C-F⋯F-C groups, the adsorbed FTCS directly leads to the growth of the P(VDF-HFP) coating layer around the treated Al NPs, yielding Al@FTCS/P(VDF-HFP) energetic composites. In comparison with the ultrasonically processed Al/P(VDF-HFP) mixture, thermal analysis reveals that Al@FTCS/P(VDF-HFP) exhibits a 57 °C lower reaction onset temperature and a 1646 J/g increase in heat release. Associated combustion tests demonstrate a 52% shorter ignition delay, 62% shorter combustion time, and a 288% faster pressurization rate. These improvements in energetic characteristics stem from the reactivity activation of FTCS towards Al NPs by the etching effect to the surface Al2O3. Moreover, enhanced interfacial contact facilitated by the FTCS-directed growth of P(VDF-HFP) around Al NPs further accelerates the whole reaction process.

14.
Artigo em Inglês | MEDLINE | ID: mdl-39213643

RESUMO

A reasonable porous transport layer (PTL) is crucial to decreasing the mass-transfer loss in proton-exchange membrane water electrolyzers (PEMWEs). In this study, it was experimentally demonstrated that the gradient porosity PTL is beneficial in improving the performance of electrolyzers. The research comprehensively investigates the impact of gradient porosity PTL structures on the performance of the PEMWE, considering mass transfer and interfacial contact. It offers insights into the two-phase (oxygen-water) flow transport mechanisms within the PTLs using a 2D numerical model based on the actual PTL geometry. At the microscopic level, it analyzes how the interfacial contact impacts proton and electron transport mechanisms, affecting not only the contact resistance but also the number of effective catalytic sites for the oxygen evolution reaction. Experimental results demonstrate that the cis-gradient porosity PTL leads to a performance enhancement of 9.3% at 2.2 A/cm2. Numerical simulations reveal that the drivers of oxygen transport include the surface tension of the fibers and the pressure drop influenced by the local PTL porosity. Further analysis indicates that the lower oxygen saturation in the bottom region of the PTL with cis-gradient porosity favors a lower oxygen coverage area in the catalyst layers (CL) since the narrower pore space and higher capillary pressure increase the number of water flow paths into the CL. Overall, this study provides valuable insights for designing high-performance PTLs for use in electrolyzers.

15.
Materials (Basel) ; 17(12)2024 Jun 12.
Artigo em Inglês | MEDLINE | ID: mdl-38930233

RESUMO

In this work, the potential of magnetron sputtering, as well as cathodic arc evaporation, is investigated with regard to its suitability as a bipolar plate coating of a PEM fuel cell. For this purpose, Cr and Ti thin films were deposited onto a 0.1 mm SS316L by varying the power and bias voltage. The surface structure and thickness of the coatings are examined via SEM and tactile profilometry. Moreover, the coating variants are compared with each other based on the electrical and electrochemical properties relevant to bipolar plates. The sputtered Cr thin films achieve the lowest contact resistance values and exhibit a columnar structure with a smooth surface. Regarding the electrochemical properties, titanium deposited via cathodic arc evaporation has a low current density in the passive region and high breakthrough potential. All in all, both deposition techniques have their individual advantages for the preparation of bipolar plates' coatings. However, Ti thin films prepared via cathodic arc seem to be the most suitable option due to the combination of a high deposition rate, a low cost and good coating properties.

16.
Materials (Basel) ; 17(4)2024 Feb 06.
Artigo em Inglês | MEDLINE | ID: mdl-38399030

RESUMO

316 L stainless steel is an ideal bipolar plate material for a proton exchange membrane fuel cell (PEMFC). However, the thickening of the passivation film on the stainless steel surface and the dissolution of corrosive ions during operation will affect the durability of the PEMFC. Herein, a heterogeneous layer is prepared on the surface of 316 L stainless steel through dual ion implantation of molybdenum ion and carbon ion combined with heat treatment to promote the corrosion resistance and conductivity of the bipolar plate. The ion implantation technique resulted in a uniform distribution of Mo and C elements on the surface of 316 L stainless steel, with a modified layer depth of about 70-80 nm. The electrical conductivity of the ion implanted samples was significantly improved, and the interfacial contact resistance was reduced from 464.25 mΩ × cm2 to 42.49 mΩ × cm2. Heat treatment enhances the surface homogenization, repairs the defects of irradiation damage, and improves the corrosion resistance of stainless steel. The corrosion current density of (Mo+C)-600 samples decreased from 1.21 × 10-8 A/cm2 to 2.95 × 10-9 A/cm2 under the long-term corrosion condition of 4 h. These results can provide guidance for the modification of stainless steel bipolar plates.

17.
Nanomicro Lett ; 16(1): 71, 2024 Jan 04.
Artigo em Inglês | MEDLINE | ID: mdl-38175423

RESUMO

The utilization of solid-state electrolytes (SSEs) presents a promising solution to the issues of safety concern and shuttle effect in Li-S batteries, which has garnered significant interest recently. However, the high interfacial impedances existing between the SSEs and the electrodes (both lithium anodes and sulfur cathodes) hinder the charge transfer and intensify the uneven deposition of lithium, which ultimately result in insufficient capacity utilization and poor cycling stability. Hence, the reduction of interfacial resistance between SSEs and electrodes is of paramount importance in the pursuit of efficacious solid-state batteries. In this review, we focus on the experimental strategies employed to enhance the interfacial contact between SSEs and electrodes, and summarize recent progresses of their applications in solid-state Li-S batteries. Moreover, the challenges and perspectives of rational interfacial design in practical solid-state Li-S batteries are outlined as well. We expect that this review will provide new insights into the further technique development and practical applications of solid-state lithium batteries.

18.
Heliyon ; 9(5): e16276, 2023 May.
Artigo em Inglês | MEDLINE | ID: mdl-37234641

RESUMO

The phase, mechanical properties, corrosion resistance, hydrophobicity, and interface contact resistance of three typical Ni-based alloys (Hastelloy B, Hastelloy C-276, and Monel 400) and 304 stainless steels were experimentally studied to evaluate their service performances as bipolar plate materials of proton exchange membrane fuel cells. All four alloys exhibit single-phase face-centered cubic structure, high strength, good ductility, and high hardness. Hastelloy C-276 has the best ductility with an uniform elongation of 72.5% and highest hardness of 363.7 HV. Hastelloy B has the highest ultimate tensile strength of 913.6 MPa. The hydrophobicity of all four alloys is not good, although Monel 400 has the highest water contact angle of 84.2°. Hastelloy B, Hastelloy C-276, and 304 stainless steel exhibit unsatisfying corrosion resistance in a simulated acidic work environment of proton exchange membrane fuel cell (0.5 M H2SO4+2 ppm HF, 80 °C, H2) and high interface contact resistance. By contrast, Monel 400 demonstrates excellent corrosion resistance with a corrosion current density of 5.9 × 10-7 A cm-2 and a low interface contact resistance of 7.2 mΩ cm2 at 140 N/cm2. In terms of comprehensive performance, Monel 400 is the best uncoated material for the bipolar plates of proton exchange membrane fuel cells among typical Ni-based alloys.

19.
ACS Appl Mater Interfaces ; 15(18): 22705-22713, 2023 May 10.
Artigo em Inglês | MEDLINE | ID: mdl-37126364

RESUMO

Ni metal has been widely used as a barrier layer in Bi2Te3-based thermoelectric devices, which establishes stable joints to link Bi2Te3-based legs and electrodes. However, the Ni/Bi2Te3 joints become very fragile when the devices were exposed to high temperature, causing severe performance deterioration and even device failure. Herein, stable Ni/Bi2Te3 joints have been established by arc spraying of the Ni barrier layer on the Bi2Te3-based alloys. The interface microstructure and contact performance including the bonding strength and contact resistivity of the arc-sprayed Ni/Bi2Te3 joints are investigated. The results indicate that, as compared with traditional Ni/Bi2Te3 joints, the arc-sprayed Ni/Bi2Te3 joints have comparably low contact resistivity while possessing a 50% higher bonding strength. Aging the joints as an exposure to high-temperature circumstances, the arc-sprayed Ni/Bi2Te3 joints exhibit much better tolerance to the thermal shock with stable bonding strength and contact resistivity. The enhanced interfacial contact performance and thermal tolerance should be attributed to the thick Ni barrier layer and interface reaction layer with good Ohmic contact. This work provides an effective strategy to establish stable joints for the Bi2Te3-based thermoelectric devices with improved thermal stability.

20.
J Colloid Interface Sci ; 630(Pt B): 634-644, 2023 Jan 15.
Artigo em Inglês | MEDLINE | ID: mdl-36343555

RESUMO

The incorporation of inorganic fillers into composite polymer electrolytes (CPEs) is a common strategy to improve ionic conductivity. However, the high surface energy of inorganic fillers typically aggravates poor interfacial contact with polymer chains. Herein, we develop a surface positive-charge modification strategy for enhancing the intermolecular interaction of poly(ethylene oxide) (PEO) electrolytes with inorganic fillers and optimizing lithium ion (Li+) conductive pathways in CPEs. The SiO2 nanoparticles are coated with a polydopamine adhesive layer and then functionalized with a branched polyethyleneimine positively charged functional layer. Such surface modification not only effectively induces more amorphous structure into the PEO matrix but also promotes the dissociation of lithium salts and activates more free Li+ in the PEO to accelerate Li+ transport. The CPEs achieved a superior ionic conductivity of 6.12 × 10-5 S cm-1 at 30 °C. In addition, the modified fillers could induce the formation of a lithium fluoride (LiF)-rich solid-state interphase and correspondingly achieve excellent compatibility with Li metal. The Li symmetric battery using the as-prepared CPEs delivered stable Li plating/stripping performances over 3960 h under 0.2 mA cm-2. The resulting LiFePO4|Li battery has an excellent capacity retention of 92.8 % after 260 cycles at 0.5C and 60 °C.

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