Abstract:Poor cyclic stability and low rate performance due to dramatic volume change and low intrinsic electronic conductivity are the two key issues needing to be urgently solved in silicon (Si)-based anodes for lithium-ion batteries. Herein, a novel tin (Sn)-bonded Si anode is proposed for the first time. Sn, which has a high electronic conductivity, is used to bond the Sianode material and copper (Cu) current collector together using a hot-pressed method with a temperature slightly above the melting point of Sn. Th… Show more
“…Lithium-ion diffusivity at the ACEI is an important parameter for lithium-ion electrodes. From GITT, we can calculate the lithium-ion diffusivity of the electrodes under quasi-static equilibrium conditions without any influence from the ACEI layers on the cathode material. ,− Figure S8a–c shows time vs GITT plots for uncoated NMC811 and Zr x PO y - and Li x Zr y PO z -coated NMC811 electrodes. Figure S8d,e shows lithium-ion diffusion coefficient curves during charging and discharging for the uncoated and Zr x PO y - and Li x Zr y PO z -coated NMC811 electrodes.…”
Owing to its high energy density, LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NMC811) is a cathode material of prime interest for electric vehicle battery manufacturers. However, NMC811 suffers from several irreversible parasitic reactions that lead to severe capacity fading and impedance buildup during prolonged cycling. Thin surface protection films coated on the cathode material mitigate degradative chemomechanical reactions at the electrode−electrolyte interphase, which helps to increase cycling stability. However, these coatings may impede the diffusion of lithium ions, and therefore, limit the performance of the cathode material at a high C-rate. Herein, we report on the synthesis of zirconium phosphate (Zr x PO y ) and lithium-containing zirconium phosphate (Li x Zr y PO z ) coatings as artificial cathode−electrolyte interphases (ACEIs) on NMC811 using the atomic layer deposition technique. Upon prolonged cycling, the Zr x PO y -and Li x Zr y PO zcoated NMC811 samples show 36.4 and 49.4% enhanced capacity retention, respectively, compared with the uncoated NMC811. Moreover, the addition of Li ions to the Li x Zr y PO z coating enhances the rate performance and initial discharge capacity in comparison to the Zr x PO y -coated and uncoated samples. Using online electrochemical mass spectroscopy, we show that the coated ACEIs largely suppress the degradative parasitic side reactions observed with the uncoated NMC811 sample. Our study demonstrates that providing extra lithium to the ACEI layer improves the cycling stability of the NMC811 cathode material without sacrificing its rate capability performance. KEYWORDS: LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811), metal phosphate, atomic layer deposition (ALD), surface passivation, suppressed parasitic reactions, high rate performance
“…Lithium-ion diffusivity at the ACEI is an important parameter for lithium-ion electrodes. From GITT, we can calculate the lithium-ion diffusivity of the electrodes under quasi-static equilibrium conditions without any influence from the ACEI layers on the cathode material. ,− Figure S8a–c shows time vs GITT plots for uncoated NMC811 and Zr x PO y - and Li x Zr y PO z -coated NMC811 electrodes. Figure S8d,e shows lithium-ion diffusion coefficient curves during charging and discharging for the uncoated and Zr x PO y - and Li x Zr y PO z -coated NMC811 electrodes.…”
Owing to its high energy density, LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NMC811) is a cathode material of prime interest for electric vehicle battery manufacturers. However, NMC811 suffers from several irreversible parasitic reactions that lead to severe capacity fading and impedance buildup during prolonged cycling. Thin surface protection films coated on the cathode material mitigate degradative chemomechanical reactions at the electrode−electrolyte interphase, which helps to increase cycling stability. However, these coatings may impede the diffusion of lithium ions, and therefore, limit the performance of the cathode material at a high C-rate. Herein, we report on the synthesis of zirconium phosphate (Zr x PO y ) and lithium-containing zirconium phosphate (Li x Zr y PO z ) coatings as artificial cathode−electrolyte interphases (ACEIs) on NMC811 using the atomic layer deposition technique. Upon prolonged cycling, the Zr x PO y -and Li x Zr y PO zcoated NMC811 samples show 36.4 and 49.4% enhanced capacity retention, respectively, compared with the uncoated NMC811. Moreover, the addition of Li ions to the Li x Zr y PO z coating enhances the rate performance and initial discharge capacity in comparison to the Zr x PO y -coated and uncoated samples. Using online electrochemical mass spectroscopy, we show that the coated ACEIs largely suppress the degradative parasitic side reactions observed with the uncoated NMC811 sample. Our study demonstrates that providing extra lithium to the ACEI layer improves the cycling stability of the NMC811 cathode material without sacrificing its rate capability performance. KEYWORDS: LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811), metal phosphate, atomic layer deposition (ALD), surface passivation, suppressed parasitic reactions, high rate performance
“…Although lithium-ion batteries (LIBs) have occupied the main market in the fields of consumer electronics batteries, power batteries, and energy storage batteries, the safety concerns originating from flammable organic liquid electrolytes still need to be solved urgently. , All-solid-state lithium-ion batteries (ASSLIBs) that employ nonflammable inorganic solid electrolytes (SEs) have been considered as the most promising candidate for next-generation energy storage devices due to their excellent safety and high energy density. − SE is the key to the success of ASSLIBs, and it needs to meet multiple requirements, such as high ionic conductivity, low electronic conductivity, mechanical deformability, and wide electrochemical stability window. , …”
Halide solid electrolytes have been considered as the most promising candidates for practical high-voltage all-solidstate lithium-ion batteries (ASSLIBs) due to their moderate ionic conductivity and good interfacial compatibility with oxide cathode materials. Aliovalent ion doping is an effective strategy to increase the ionic conductivity of halide electrolytes. However, the effects of ion doping on the electrochemical stability window of halide electrolytes and carbon additive on electrochemical performance are still unclear by far. Herein, a series of Zr-doped Li 3−x Er 1−x Zr x Cl 6 halide solid electrolytes (SEs) are synthesized through a mechanochemical method and the effects of Zr substitution on the ionic conductivity and electrochemical stability window are systematically investigated. Zr doping can increase the ionic conductivity, whereas it narrows the electrochemical stability window of the Li 3 ErCl 6 electrolyte simultaneously. The optimized Li 2.6 Er 0.6 Zr 0.4 Cl 6 electrolyte exhibits both a high ionic conductivity of 1.13 mS cm −1 and a high oxidation voltage of 4.21 V. Furthermore, carbon additives are demonstrated to be beneficial for achieving high discharge capacity and better cycling stability and rate performance for halide-based ASSLIBs, which are completely different from the case of sulfide electrolytes. ASSLIBs with uncoated LiCoO 2 cathode and carbon additives exhibit a high discharge capacity of 147.5 mAh g −1 and superior cycling stability with a capacity retention of 77% after 500 cycles. This work provides an in-depth understanding of the influence of ion doping and carbon additives on halide solid electrolytes and feasible strategies to realize highenergy-density ASSLIBs.
“…The CV curves of three samples in the initial two cycles are presented in Figures 5(a-c), showing similar electrochemical processes. Specifically, due to the formation of SEI film 53,54 , there was only a small and broad cathodic peak at ~0.75 V in the 1 st cycle, which is much obvious for Si@c-PDA and Si-Cu3Si@c-PDA. A sharp cathodic peak at ~0.05 V in the 1 st cycle is due to the generation of crystalline Li3.75Si (c-Li3.75Si) 55,56 .…”
Section: ) Electrochemical Performance and Analysismentioning
Silicon (Si) is a promising anode material for Li-ion batteries but its application is limited due to its severe volume change during the lithiation/delithiation process leading to a fast degradation of cycle performance. Applying transition metals to dope into the bulk of Si forming active/inactive silicide phase is proved an effective and practical method to solve this issue. However, the classic high-energy ball milling method is faced with the challenges of strict requirements to the machine, long-time working and difficulty to control the morphology of the product. Aiming to this point, the present study proposes a facile and “softer” method via coating the polydopamine (PDA) with the assistance of CuCl2·2H2O followed by a high-temperature annealing process to successfully fabricate the Si-based anode material with a unique structure of Si-Cu3Si@C. We firstly achieved the doping of Cu3Si and at the same time coating the carbon layer on the surface of Si. Owing to the synergistic effect of carbonized PDA layer and doped Cu3Si phase, both structural stability and electronic conductivity of electrode have been significantly enhanced. The Si-Cu3Si@C composite anode not only exhibited a high initial reversible capacity of 2356.7 mAh·g-1 with an initial coulombic efficiency of 83.6%, but also demonstrated a good capacity retention of 89.7% after 100 cycles at the current density of 400 mA·g-1. We believe this work can pave a new way to improve the Si-based anode material.
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