Organic-inorganic composite SEI for a stable Li metal anode by in-situ polymerization

Cao, Wenzhuo; Lu, Jiaze; Zhou, Kun; Sun, Guochen; Zheng, Jieyun; Zhang, Geng; Li, Hong

doi:10.1016/j.nanoen.2022.106983

Cited by 148 publications

(74 citation statements)

References 54 publications

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“…Together with the F 1s spectra revealing the Li x PO y –1 F z +1 group in the ester-based electrolyte, one can conclude that the decomposition of LiPF 6 (which usually produces HF and corrodes both the cathode and anode) is avoided by using the PCE. The SEI in the PCE combines organic and inorganic components, which endows it with high robustness and flexibility. − The long-term Li||Li cell cycling performance and rate tests are shown in Figures S17 and S18. The symmetric cell in the PCE can run stably for over 1200 h at 0.2 mA cm –2 , and the overpotential remains ∼35 mV at the 850th cycle, which proves the long-time stability with lithium.…”

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confidence: 99%

Solvation Structure-Tunable Phase Change Electrolyte for Stable Lithium Metal Batteries

Yan

et al. 2022

ACS Energy Lett.

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Li + solvation structure (LSS) is considered to be the decisive factor in determining the electrochemical performance of lithium metal batteries. Herein, we propose a phase change electrolyte (PCE) whose LSS can be in operando regulated by changing the physical state of the electrolyte. The primary solvent of a PCE is dimethyl dodecanedioate (DDCA), which stands out among a series of solvents, exhibiting excellent comprehensive performance. The PCE shows high ionic conductivity, lithium transference number, and a wide electrochemical stability window in the solid and liquid states. Moreover, the LSS of the obtained PCE can reversibly transform between the solventseparated ion pair (SSIP) and contact ion pair (CIP) structure according to its physical state. This characteristic enables PCE to outperform conventional liquid electrolytes in suppressing lithium dendrite growth and dissolution of active anodic materials, especially at varying temperatures. The assembled Li-LiMn 2 O 4 full cells display outstanding electrochemical performance, high Coulombic efficiency, and capacity retention.

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confidence: 99%

Solvation Structure-Tunable Phase Change Electrolyte for Stable Lithium Metal Batteries

Yan

et al. 2022

ACS Energy Lett.

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“…Notably, the peak in the O 1s spectrum located at 528.3 eV (Figure b) may be associated with Li 2 O, which originates from the LiClO 4 additive that facilitates Li + transport and presents a more uniform electric field intensity distribution on the Li anode surface. , Furthermore, the existence of LiCl is further evidenced by the Li 1s spectrum in Figure c, the LiCl peak located around 56.3 eV, the Cl 2p spectrum in Figure d, the LiCl 2p 1/2 peak at 200.5 eV, and the LiCl 2p 3/2 peak at 198.9 eV. The F 1s spectrum in Figure S5 of the Supporting Information found that the LiF content on the surface of the negative electrode containing the most additive additions is relatively low, indicating that the additive addition can effectively reduce the decomposition of the electrolyte. − More importantly, the electrochemical performance is effectively improved by benefiting from a stable and homogeneous SEI layer. The cycling CE in Li||Cu cells and cycle stability in complete cells are used to evaluate the reversibility of the Li metal anode in practical application, which is encouraged by the impressive interfacial strength in symmetric cells. − The CEs of Li||Cu cells are shown in Figure a at current densities of 0.5 and 2 mA cm –2 , respectively, with a fixed deposition capacity of 1 mAh cm –2 .…”

Section: Resultsmentioning

confidence: 92%

Lithium Perchlorate Additive for Dendritic-Free and Long-Life Li Metal Batteries

Deng

et al. 2022

Energy Fuels

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Nowadays, lithium (Li) metal is regarded as the most prospective electrode for the next generation of rechargeable batteries. Regrettably, poor coulombic efficiency (CE) and dendritic lithium development after repeated lithium electroplating/exfoliation treatments significantly restrict Li metal battery applications. To prevent dendrite growth of the Li metal during the reaction, an adequate amount of lithium perchlorate (LiClO4) is added to the ether-based electrolyte as an additive. When this additive is combined with lithium metal, a homogeneous and dense solid electrolyte interphase (SEI) layer rich in lithium chloride and lithium oxide can be created in situ. As a result of the general synergistic protection of LiCl and Li2O, the produced SEI has high ionic conductivity, allowing Li+ mobility, resulting in a more homogeneous distribution of electric field strength, helping to uniform Li deposition, and preventing the development of Li dendrites. As a result, the superior electrochemical performances are demonstrated by an ultralong cycling lifetime (>1500 h) in Li||Li symmetrical cells, coupled with a relatively low hysteresis voltage of 60 mV at 1 mA cm–2, a sufficiently high-quality CE (approximately 96% for 200 cycles at the current density of 0.5 mA cm–2 in Li||Cu cells), and an improved cycling stability in the Li||LiFePO4 complete cell.

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“…Figure 5i exhibits the Ragone plot of the NCM811|MS|PE|Ag 2 S|Li prototype in comparison with previously reported NCM811|Li cell models, all values were calculated based on the mass of electrode material. [21,[44][45][46][47][48][49][50] The NCM811|Li cell with MS|PE|Ag 2 S separator shows the highest power output of 2040 W kg −1 with the energy density of 408 Wh kg −1 at 5 C, which surpass the most values of the previously reported NCM811|Li metal batteries. Furthermore, the cycling stability of cell assembled with MS|PE|Ag 2 S separators is also superior to most previously reported metal batteries with other modified separators under lean electrolyte condition (Table S4, Supporting Information).…”

Section: Resultsmentioning

confidence: 99%

“…[19] Alternatively, the ether-based solvents ((1,3-dioxolane, ethylene glycol dimethylether) or the film-forming additives (fluoroethylene carbonate, vinylene carbonate, and lithium difluorooxalato borate) were directly adopted in the electrolyte to in situ form the favorable passivation components. [20][21][22] Upon the high-voltage cycling or at the low temperature conditions, however, the low oxidation resistance of ethers or insufficient dynamics of the derived species (LiF, poly(vinylene carbonate)) also lead to the enhanced interfacial charge transfer resistance, which inevitably jeopardized the power output of the cell. [23,24] Moreover, the "lithiophilic" seeds (e.g., Ag, Au, and Zn) were also used to induce the preferential Li + influx toward the specific location and mitigate the nucleation barrier.…”

Section: Introductionmentioning

confidence: 99%

Boosting the Temperature Adaptability of Lithium Metal Batteries via a Moisture/Acid‐Purified, Ion‐Diffusion Accelerated Separator

Zhang

Liu

Gan

et al. 2022

Advanced Energy Materials

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solutions, explorative studies of the electro-redox couples, with the concurrent high retrievable capacity, enlarged nominal voltage gap, and rapid reaction kinetics, hold the key to promote the energy-dense battery construction at the extreme power output. [1] For the lithium ion batteries, the energy densities of traditional formats (LiCoO 2 /LiFePO 4 cathodes and graphite anodes) have approached their theoretical limits. [2] Alternatively, the unit cell prototyping of the high-capacity Li metal anode with the nickel-rich cathode can achieve the enhanced level of energy densities at the device level. [3,4] When soaking this electrode couples in the conventional carbonate-based electrolytes, however, the Fermi-energy incompatibility at the multiscale interface would cause the uncontrollable dendrite growth on the metallic foil and cathode structure collapse upon the high-voltage cycling. [5] Therefore, the reliable operation of the energy-dense battery necessitates the harmony balance of the enlarged voltage gap and the interfacial stability at multiple scales, yet still remains challenging.As the most attractive cathode type of the practical relevance, nickel-rich (Ni content >0.8) layered oxides exhibit the merits of the large specific capacity (>200 mAh g −1 ), environmental benignity and relative lower cost as compared to the LiCoO 2 cathode. Despite of the dominant nickel occupancy in the layered oxides for elevating the Li storage sites, the increased nickel ratio adversely deteriorates the cycle performance. The transition metal (TM) layer of the oxide structure at the highvoltage charged states would oxidize the carbonate solvents in the presence of moisture, leading to serious self-discharge rates upon the high-temperature storage. [6] Additionally, the hydrofluoric acid (HF) formed by the decomposition of the lithium hexafluorophosphate (LiPF 6 ) salt aggravates the TM ions (Co 2+ , Ni 2+ , and Mn 2+ ) dissolution and structural collapse of the layered cathode, meanwhile the TM species would deposit on the anode surface and degrade the solid electrolyte interface (SEI). [7] So far, a plethora of mitigation strategies were implemented to insulate the direct contact of the oxide particles with the electrolyte, for instance the exquisite coatings with The reliable operation of Li metal batteries suffers from cathode collapse due to high-voltage cycling, interfacial reactivity of the Li deposits, self-discharge at the elevated temperatures, as well as the power output deterioration in low-temperature scenarios. In contrast to the individual electrode optimization, herein, a hetero-layered separator with an asymmetric functional coating on polyethylene is proposed in response to the aforementioned issues: On the face-to-cathode side, the hybrid layer of the molecular sieve and sulfonated melamine formaldehyde can scavenge the hydrofluoric acid and moisture residues from the carbonate electrolyte, maintaining the cathode robustness in both the high-voltage cycling or high-temperature storage scenarios; while...

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Organic-inorganic composite SEI for a stable Li metal anode by in-situ polymerization

Cited by 148 publications

References 54 publications

Solvation Structure-Tunable Phase Change Electrolyte for Stable Lithium Metal Batteries

Solvation Structure-Tunable Phase Change Electrolyte for Stable Lithium Metal Batteries

Lithium Perchlorate Additive for Dendritic-Free and Long-Life Li Metal Batteries

Boosting the Temperature Adaptability of Lithium Metal Batteries via a Moisture/Acid‐Purified, Ion‐Diffusion Accelerated Separator

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