High-Rate SiO Lithium-Ion Battery Anode Enabled by Rationally Interfacial Hybrid Encapsulation Engineering
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The development of a high-rate SiO lithium-ion battery anode is seriously limited by its low intrinsic conductivity, sluggish interfacial charge transfer (ICT), and unstable dynamic interface. To tackle the above issues, interfacial encapsulation engineering for effectively regulating the interfacial reaction and thus realizing a stable solid electrolyte interphase is significantly important. Hybrid coating, which aims to enhance the coupled e–/Li+ transport via the employment of dual layers, has emerged as a promising strategy. Herein, we construct a hybrid MXene-graphene oxide (GO) coating layer on the SiO microparticles. In the design, Ti3C2Tx MXene acts as a "bridge", which forms a close covalent connection with SiO and GO through Ti–O–Si and Ti–O–C bonds, respectively, thus greatly reducing the ICT resistance. Moreover, the Ti3C2Tx with rich surface groups (e.g., –OH, –F) and GO outer layers with an intertwined porous framework synergistically enable the pseudocapacitance dominated behavior, which is beneficial for fast lithium-ion storage. Accordingly, the as-made Si@MXene@GO anode exhibits considerably reinforced lithium-ion storage performance in terms of superior rate performance (1175.9 mA h g–1 at 5 A g–1) and long cycling stability (1087.6 mA h g–1 capacity retained after 1000 cycles at 2.0 A g–1). In-depth interfacial chemical composition analysis further reveals that an inorganically rich interphase with a gradient distribution of LiF and Li2O formed at the electrolyte/anode interface ensures mechanical stability during repeated cycles. This work paves a feasible way for maximizing the potential of SiO anodes toward fast-charging lithium-ion batteries.Keywords:
Pseudocapacitance
Pseudocapacitive materials that store charges via reversible surface or near‐surface faradaic reactions are capable of overcoming the capacity limitations of electrical double‐layer capacitors. Revealing the structure–activity relationship between the microstructural features of pseudocapacitive materials and their electrochemical performance on the atomic scale is the key to build high‐performance capacitor‐type devices containing ideal pseudocapacitance effect. Currently, the high brightness (flux), and spectral and coherent nature of synchrotron X‐ray analytical techniques make it a powerful tool for probing the structure–property relationship of pseudocapacitive materials. Herein, we report a comprehensive and systematic review of four typical characterization techniques (synchrotron X‐ray diffraction, pair distribution function [PDF] analysis, soft X‐ray absorption spectroscopy, and hard X‐ray absorption spectroscopy) for the study of pseudocapacitance mechanisms. In addition, we offered significant insights for understanding and identifying pseudocapacitance mechanisms (surface redox pseudocapacitance, intercalation pseudocapacitance, and the extrinsic pseudocapacitance phenomenon in battery materials) by combining in situ hard XAS and electrochemical analyses. Finally, a perspective for further depth of understanding into the pseudocapacitance mechanism using synchrotron X‐ray analytical techniques is proposed.
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Pseudocapacitive material development is a promising approach toward realizing high-rate sodium-ion storage, through either surface redox pseudocapacitance or intercalation pseudocapacitance. This review describes the fundamental mechanisms and electrochemical features of various vanadium-based electrode materials which exhibit pseudocapacitive sodium-ion storage. In particular, areas for further research are identified and a perspective on the future of high-power sodium-ion device applications is provided.
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Pseudocapacitive charge storage with Ti3C2Tx in protic electrolytes has received significant attention. However, other MXene compositions have received less attention so far. Additionally, pseudocapacitance of MXenes has only been reported in acidic electrolytes. Herein, we report on the pseudocapacitance of two vanadium carbide MXenes (V2CTx and V4C3Tx) in various basic electrolytes and sulfuric acid, showing distinct redox couples in their cyclic voltammograms. Freestanding V2CTx film electrodes could deliver gravimetric capacitances above 250 F g–1 in different basic electrolytes with the highest capacitance of 386 F g–1 in 1 M LiOH at 2 mV s–1. Moreover, the cycle life performance showed an increasing capacitance over thousands of cycles (121% of initial capacitance after 60,000 cycles at 10 A g–1 in 6 M KOH). Both materials also exhibit higher capacitances than Ti3C2Tx in 3 M sulfuric acid, with 475 and 284 F g–1 for V2CTx and V4C3Tx, respectively.
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The efficient storage of energy in hybrid capacitors is based upon the co-optimization of both double-layer capacitance and pseudocapacitive (Faradic) charge storage. This inevitably involves a delicate balance of nano-structural and nano-porosity engineering, coupled with carefully designed electron transfer properties giving rise to pseudocapacitance. In this talk we explore how one might systematically tune the redox properties of nanoparticles to facilitate a near ideal pseudocapacitive response. Subsequently, we examine fundamental constraints on such nanoparticle derived pseudocapacitance and its implications for hybrid capacitors derived from nanostructured electrodes. The “battery like” Faradaic features of pseudocapacitance will also be discussed. In general this work is intended to provide benchmarks on the optimal performance capabilities of hybrid capacitors and their construction via nanoporous/nanostructured electrodes.
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Abstract Early transition‐metal nitrides, especially vanadium nitride (VN), have shown promise for use in high energy density supercapacitors due to their high electronic conductivity, areal specific capacitance, and ability to be synthesized in high surface area form. Their further development would benefit from an understanding of their pseudocapacitive charge storage mechanism. In this paper, the extent of pseudocapacitance exhibited by vanadium nitride in aqueous electrolytes was investigated using cyclic voltammetry and electrochemical impedance spectroscopy. The pseudocapacitance contribution to the total capacitance in the nitride material was much higher than the double‐layer capacitance and ranged from 85 % in basic electrolyte to 87 % in acidic electrolyte. The mole of electrons transferred per VN material during pseudocapacitive charge storage was also evaluated. This pseudocapacitive charge‐storage is the key component in the full utilization of the properties of early‐transition metal nitrides for high‐energy density supercapacitors.
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