Developing multifunctional amide additive by rational molecular design for high-performance Li metal batteries

Peng, Qingkui; Liu, Ziyi; Chen, Shiyao; Duan, Peiyu; Cheng, Siyuan; Jiang, Lihua; Sun, Jinhua; Wang, Qingsong

doi:10.1016/j.nanoen.2023.108547

Cited by 13 publications

(7 citation statements)

References 55 publications

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“…Figure a–c shows the XPS fitting peaks of C 1s, O 1s, and F 1s, respectively. There are four peaks in the C 1s spectrum, as the C–C bond at 284.8, C–O at 285.9, COOR at 288.2, and C–F/CO 3 2– bond at 290.4 eV. − O 1s spectra can be found to hold four main peaks in Figure b, with the one at 530 eV attributed to Li 2 O bonding from the oxygenated surface species; at 532.6 eV CO, and at 531.3 eV Li 2 CO 3 and C–O bonding are found . As a matter of fact, the unstable interphase of Li 2 CO 3 in the LMO cathode is less in MS-E, while Li 2 CO 3 is regarded as an unstable component in cycling.…”

Section: Resultsmentioning

confidence: 92%

“…The calculation results indicate that MSTFA will undergo a series of chemical bond breaks around the N atom. 43 MSTFA may react with water to form trimethylsilanol and acetamide. Then, trimethylsilanol and acetamide will further break down into small molecules containing F, N, and Si.…”

Section: Resultsmentioning

confidence: 99%

“…Combined with the analysis of XPS and the decomposition pathway, a possible decomposition path of MSTFA is proposed (Figure e). The calculation results indicate that MSTFA will undergo a series of chemical bond breaks around the N atom . MSTFA may react with water to form trimethylsilanol and acetamide.…”

Section: Resultsmentioning

confidence: 99%

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Stabilizing the Lithium-Rich Manganese-Based Oxide Cathode via Regulating a CEI Film

Feng,

Guo,

Liu

et al. 2024

ACS Appl. Energy Mater.

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Targeting high-energy-density batteries, lithium-rich manganese oxide (LMO), with its merits of high working voltage (∼4.8 V vs Li/Li + ) and high capacity (∼250 mAh g −1 ), was considered a promising cathode for a 500 Wh kg −1 project. However, the practical application of LMO was hindered by the parasitic reaction between the electrolyte and the electrode, such as dissolution of surface lattice oxygen. Herein, N-methyl-Ntrimethylsilyl trifluoroacetamide (MSTFA) is introduced as an additive in a common carbonate ester electrolyte to modify the cathode-electrolyte interphase (CEI) for blocking the undesirable side reaction. The preferential decomposition of MSTFA results in silicon and NO x -containing CEI, which greatly enhances the highvoltage stability of the LMO cathode. Moreover, the designed CEI enables providing a homogeneous interphase within 5 nm, which is responsible for the long-time stability of the cathode. Herein, the assembled LMO||Li battery yields a high-capacity retention of 93.1% after 200 cycles at a current density of 100 mA g −1 .

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Section: Resultsmentioning

confidence: 92%

Section: Resultsmentioning

confidence: 99%

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Stabilizing the Lithium-Rich Manganese-Based Oxide Cathode via Regulating a CEI Film

Feng,

Guo,

Liu

et al. 2024

ACS Appl. Energy Mater.

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“…[94,95] Among these methods, extensive research has demonstrated the effectiveness of trimethylsilane in eliminating H 2 O/HF from the electrolyte, as shown in Table 1. Wang et al [87] designed an additive called 2,2,2-trifluoro-Nmethyl-N-(trimethylsilyl)acetamide (MSTFA), which connects multiple functional groups using amide units. Among many similar compounds, MSTFA stands out with its rational molecular structure and the synergistic complementarity of amide, trifluoromethyl, and trimethylsilane groups.…”

Section: Silicone Additivesmentioning

confidence: 99%

Recent Progress on Multifunctional Electrolyte Additives for High‐Energy‐Density Li Batteries – A Review

Lei,

Wang,

Jiang

et al. 2024

ChemElectroChem

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The improvement of the safety, specific energy, cycle life and the cost reduction of Li‐ion batteries are hot research topics. Now, in the pursuit of high energy density, the employed high‐energy‐density cathode/anode materials and the increased operation voltage challenge the prevalent electrolyte formula, like the existing ester and ether electrolytes cannot withstand the high‐voltage operation and high‐capacity anode such as lithium (Li), silicon (Si) and silicon‐graphite (Si−C) composite anode. It is recognized that stable electrolyte‐electrode interfaces can avoid the electrolytes side reactions and protect the electrode materials. Up to now, various additives have been developed to modify the electrode‐electrolyte interfaces, such as famous 4‐fluoroethylene carbonate, vinylene carbonate and lithium nitrate, and the LIBs and lithium metal batteries (LMBs) performances have been improved greatly. However, the lifespan of the higher‐energy‐density batteries with Li/Si/Si−C anode and high‐nickel layer oxides cathode materials cannot meet the request due to the lack of ideal electrolyte formula. In this review, we present a comprehensive and in‐depth overview on the electrolyte additives, especially focused on multifunctional additives, the reaction mechanisms of various additives and fundamental design. Finally, novel insights, promising directions and potential solutions for the multifunctional electrolyte additives are proposed to motivate high‐energy‐density Li battery chemistries.

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“…17,18 It is proposed that fluorine-based electrolyte additives can preferentially form stable interfacial layers on the electrodes which enhance the overall electrochemical performance. [19][20][21][22][23][24][25] In this study we explore a novel strategy aimed at improving the electrochemical performance of LMBs with the addition of ∼1% w/v of zinc triflate (Zn(Otf) 2 ) as an additive into commercial electrolyte. Via X-ray photoelectron spectroscopy analysis, we concluded that the decomposition of Zn(Otf) 2 results in fluorination at the cathode electrolyte interface (CEI).…”

mentioning

confidence: 99%

The Role of Zinc Triflate Additive for Improved Electrochemical Performance of Nickel-Rich Layered Oxide Lithium Battery Cathode via Suppression of Interfacial Parasitic Reactions

Akella,

Blanga,

Zysler

et al. 2024

J. Electrochem. Soc.

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Nickel-rich layered oxide cathode materials with low cobalt content, such as LiNi0.90Mn0.05Co0.05O2 (NMC90), have the potential to enable cost-effective, high-energy-density lithium-metal batteries. However, NMC90 cathode materials are prone to severe parasitic reactions at higher voltages during prolonged cycling. The addition of small percentages of electrolyte additives to the neat commercial electrolyte can significantly enhance the overall electrochemical performance of lithium-metal batteries. This study investigates the effects of zinc triflate (Zn(Otf)2) as an electrolyte additive on the enhancement of the electrochemical performances of lithium-metal batteries comprising nickel-rich layered oxide cathode materials. X-ray photoelectron spectroscopy analysis revealed that Zn(Otf)2 decomposition leads to enhanced fluorination at the interfacial layers, which contributes to improved chemical stability. Utilizing operando electrochemical mass spectroscopy, we demonstrate that Zn(Otf)2 additives effectively suppress the electrolyte degradation, which is otherwise detrimental to electrochemical performance. Electrochemical studies show that the inclusion of only ~1% Zn(Otf)2 as additive in neat commercial electrolyte enhances the electrochemical performance indicated by a 10% improvement in capacity retention after 150 cycles. This study paves the way for researchers to develop novel fluorinated triflate based electrolyte additives aimed at enhancing the stabilization of interfaces for lithium ion, and potentially also Li-metal batteries.

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Developing multifunctional amide additive by rational molecular design for high-performance Li metal batteries

Cited by 13 publications

References 55 publications

Stabilizing the Lithium-Rich Manganese-Based Oxide Cathode via Regulating a CEI Film

Stabilizing the Lithium-Rich Manganese-Based Oxide Cathode via Regulating a CEI Film

Recent Progress on Multifunctional Electrolyte Additives for High‐Energy‐Density Li Batteries – A Review

The Role of Zinc Triflate Additive for Improved Electrochemical Performance of Nickel-Rich Layered Oxide Lithium Battery Cathode via Suppression of Interfacial Parasitic Reactions

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