The impact of electrode conductivity on electrolyte interfacial structuring and its implications on the Na<sup>0/+</sup> electrochemical performance

Rakov, Dmitrii; Sun, Ju; Cherepanov, Pavel V.; Araño, Khryslyn; Howlett, Patrick C.; Simonov, Alexandr N.; Chen, Fangfang; Forsyth, Maria

doi:10.1039/d3ee00864a

Cited by 9 publications

(1 citation statement)

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“… 25 Therefore, the introduction of an additional concept, referred to as the EDL, becomes imperative as it considerably impacts the chemical properties and morphology of the SEI through the arrangement of molecular and ionic assemblies in close proximity to the anode. 115 However, numerous additives merely adsorb onto the ZMA surface to generate a EDL without undergoing subsequent reduction to form an SEI. In response to this issue, Huang et al conducted a comprehensive evaluation of 15 organic additives and identified the pivotal determinant of these additives' protective effectiveness as their capacity to generate an SEI layer.…”

Section: Electrolyte Engineering-induced Protective Mechanismsmentioning

confidence: 99%

Rescuing zinc anode–electrolyte interface: mechanisms, theoretical simulations and in situ characterizations

Liu,

Zhang,

Liu

et al. 2024

Chem. Sci.

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Section: Electrolyte Engineering-induced Protective Mechanismsmentioning

confidence: 99%

Rescuing zinc anode–electrolyte interface: mechanisms, theoretical simulations and in situ characterizations

Liu,

Zhang,

Liu

et al. 2024

Chem. Sci.

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An Electrolyte with Less Space‐Occupying Diluent at Cathode Inner Helmholtz Plane for Stable 4.6 V Lithium‐Ion Batteries

Fang,

Du,

Zhang

et al. 2023

Angewandte Chemie

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Reasonably elevating the working voltage (≥4.4 V vs. Li/Li+) of the cathode is one of the efficient approaches to maximize the energy density of lithium‐ion batteries (LIBs). As a preferred partner for high‐voltage LIB systems, localized high‐concentration electrolyte (LHCE), characterized by a stronger Li solvation structure, less free solvent, and robust electrode/electrolyte interphase has attracted much attention in academic circles. Herein, we systematically studied the role of the diluent in LHCE on the formation of the cathode electrolyte interphase (CEI) and elucidated that the existing anion‐diluent pairing in the inner Helmholtz plane (IHP) results in an uneven CEI and subsequent battery degradation under high voltage. A m‐fluorotoluene (mFT) diluent was further employed in the LHCE containing lithium difluoro(oxalato)borate (LiDFOB) to facilitate a uniform and rich‐anion‐derived CEI, since the weaker interaction of HmFT−BDFOB−, as compared to the HHhydrofluoroether−BDFOB−, reduces the influence of mFT in IHP or initial CEI formation. Consequently, the mFT‐dominated LHCE propels the high‐voltage performance of LIBs one step forward, endowing a 4.6 V‐class 1.2‐Ah graphite||LiNi0.8Co0.1Mn0.1O2 pouch cells a 90.4 % capacity retention after 130 cycles. Our study thus describes a new index affecting the CEI formation and proposes novel strategies to deeply optimize the high‐voltage LIBs.

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Carbonate Ester‐Based Sodium Metal Battery with High‐Capacity Retention at −50 °C Enabled by Weak Solvents and Electrodeposited Anode

Hu,

Guo,

Huang

et al. 2024

Angewandte Chemie

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Sodium metal batteries (SMBs) have received increasing attention due to the abundant sodium resources and high energy density, but suffered from the sluggish interfacial kinetic and unstable plating/stripping of sodium anode at low temperature, especially when matched with ester electrolytes. Here, we develop a stable ultra‐low‐temperature SMBs with high‐capacity retention at −50°C in a weak solvated carbonate ester‐based electrolyte, combined with an electrodeposited Na (Cu/Na) anode. The Cu/Na anode with electrochemically activated “deposited sodium” and stable inorganic‐rich solid electrolyte interphase (SEI) was favor for the fast Na+ migration, therefore accelerating the interfacial kinetic process. As a result, the Cu/Na || NaCrO2 battery exhibited the highest capacity retention (compared to room‐temperature capacity) in carbonate ester‐based SMBs (98.05% at −25°C, 91.3% at −40°C, 87.9% at −50°C, respectively). The cyclic stability of 350 cycles at −25°C with a high energy efficiency of 96.15% and 70 cycles at −50°C can be achieved. Even in chill atmospheric environment with the fluctuant temperature, the battery can still operate over one month. This work provides a new opportunity for the development of low‐temperature carbonate ester‐based SMBs.

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The impact of electrode conductivity on electrolyte interfacial structuring and its implications on the Na^0/+ electrochemical performance

Abstract: The molecular and ionic assemblies at an electrode/liquid electrolyte interface, i.e., electric double layer (EDL), define battery performance by directing the formation of stable interphases. An unstable interphase can hamper...

Cited by 9 publications

References 70 publications

Rescuing zinc anode–electrolyte interface: mechanisms, theoretical simulations and in situ characterizations

Rescuing zinc anode–electrolyte interface: mechanisms, theoretical simulations and in situ characterizations

An Electrolyte with Less Space‐Occupying Diluent at Cathode Inner Helmholtz Plane for Stable 4.6 V Lithium‐Ion Batteries

Carbonate Ester‐Based Sodium Metal Battery with High‐Capacity Retention at −50 °C Enabled by Weak Solvents and Electrodeposited Anode

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The impact of electrode conductivity on electrolyte interfacial structuring and its implications on the Na0/+ electrochemical performance

Abstract: The molecular and ionic assemblies at an electrode/liquid electrolyte interface, i.e., electric double layer (EDL), define battery performance by directing the formation of stable interphases. An unstable interphase can hamper...

Cited by 9 publications

References 70 publications

Rescuing zinc anode–electrolyte interface: mechanisms, theoretical simulations and in situ characterizations

Rescuing zinc anode–electrolyte interface: mechanisms, theoretical simulations and in situ characterizations

An Electrolyte with Less Space‐Occupying Diluent at Cathode Inner Helmholtz Plane for Stable 4.6 V Lithium‐Ion Batteries

Carbonate Ester‐Based Sodium Metal Battery with High‐Capacity Retention at −50 °C Enabled by Weak Solvents and Electrodeposited Anode

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Product

Resources

About

The impact of electrode conductivity on electrolyte interfacial structuring and its implications on the Na^0/+ electrochemical performance