Additive engineering for robust interphases to stabilize high-Ni layered structures at ultra-high voltage of 4.8 V

Tan, Sha; Shadike, Zulipiya; Li, Jizhou; Wang, Xuelong; Yang, Yiying; Lin, Ruoqian; Cresce, Arthur v.; Hu, Jiangtao; Hunt, Adrian; Waluyo, Iradwikanari; Ma, Lu; Monaco, Federico; Cloetens, Peter; Xiao, Jie; Liu, Yijin; Yang, Xiao‐Qing; Xu, Ke; Hu, Enyuan

doi:10.1038/s41560-022-01020-x

Cited by 242 publications

(201 citation statements)

References 47 publications

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“…4 Moreover, dissolved TMs eventually waft to the anode side where they can destruct the SEI layer. 37 In contrast, LiDFOB exhibits the lowest LUMO, demonstrates a high electron a nity and can be expected to be reduced rstly, hence it can dominate the formation of the outer-layer SEI; while FDMA with strong electron-withdrawing -CF 3 and -N-groups shows the second-lowest LUMO energy, it can contribute to form LiF-rich and Li 2 CO 3 -less inner-layer SEI (Fig. 1d).…”

Section: Resultsmentioning

confidence: 99%

Tailoring polymer electrolyte for high-voltage solid-state Li metal batteries working at ultra-low temperatures

Weng

et al. 2022

Preprint

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Stable operation of batteries at low temperatures is critical for applications in cold-climates; however, low-temperature operations are plagued by low ionic conductivity of electrolytes, slow interfacial kinetics and unstable solid–electrolyte interphases (SEIs). We report a polymer electrolyte with an ionic conductivity of 2.2⋅10− 4 S cm− 1 and an ionic transference number of 0.8 at − 20 °C; the electrolyte is synthesized by in-situ polymerizing 1,3,5-trioxane (TXE), 2-2-2-trifluoro-N, N-dimethylacetamide (FDMA), fluoroethylene carbonate (FEC) and lithium difluoro(oxalate)borate (LiDFOB). The polymer electrolyte enables a dual-layered SEI on the Li metal anode and strongly stabilizes the LiNi0.8Co0.1Mn0.1O2 cathode, thus defining fast interfacial charge-transfer at low temperatures. Consequently, the galvanic Li corrosion and the dendritic growth are suppressed, stable Li metal anode and LiNi0.8Co0.1Mn0.1O2 cathode are achieved, and the operation temperatures of polymer-based batteries are decreased to below − 30°C. From − 30°C to room temperature, the Li||LiNi0.8Co0.1Mn0.1O2 battery achieves long cycle lifetime and high capabilities. Even at − 20°C, the Li||LiNi0.8Co0.1Mn0.1O2 battery realizes > 75% (~ 151 mAh g− 1) of its room-temperature capacity, and presents stable cycling over 200 cycles. Outstandingly, the Li||LiNi0.8Co0.1Mn0.1O2 pouch cell successfully powers an electric fan at − 58.3°C.

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Section: Resultsmentioning

confidence: 99%

Tailoring polymer electrolyte for high-voltage solid-state Li metal batteries working at ultra-low temperatures

Weng

et al. 2022

Preprint

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“…This work shows it is a simple strategy for stabilizing the surface and bulk of both Ni-rich cathodes at high-voltage operation. Recently, Hu et al [ 124 ] found that lithium difluorophosphate (LiDFP) is a serviceable electrolyte additive for maintaining the cyclic stability of Ni-rich cathode materials at an ultra-high voltage (4.8 V). With 1% LiDFP, the polycrystalline LiNi 0.76 Co 0.10 Mn 0.14 O 2 (NCM76) cathode upcycling 200 cycles possesses an impressive capacity retention of 97% in 2.8–4.8 V. The excellent cycling stability is attributed to the stable interface formed by the decomposition of LiDFP, which contributes to the rapid transmission of lithium-ions at the interface.…”

Section: Modificationsmentioning

confidence: 99%

Challenges and Modification Strategies of Ni-Rich Cathode Materials Operating at High-Voltage

Liao

Liu

2022

Nanomaterials

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Ni-rich cathode materials have become promising candidates for lithium-based automotive batteries due to the obvious advantage of electrochemical performance. Increasing the operating voltage is an effective means to obtain a higher specific capacity, which also helps to achieve the goal of high energy density (capacity × voltage) of power lithium-ion batteries (LIBs). However, under high operating voltage, surface degradation will occur between Ni-rich cathode materials and the electrolytes, forming a solid interface film with high resistance, releasing O2, CO2 and other gases. Ni-rich cathode materials have serious cation mixing, resulting in an adverse phase transition. In addition, the high working voltage will cause microcracks, leading to contact failure and repeated surface reactions. In order to solve the above problems, researchers have proposed many modification methods to deal with the decline of electrochemical performance for Ni-rich cathode materials under high voltage such as element doping, surface coating, single-crystal fabrication, structural design and multifunctional electrolyte additives. This review mainly introduces the challenges and modification strategies for Ni-rich cathode materials under high voltage operation. The future application and development trend of Ni-rich cathode materials for high specific energy LIBs are projected.

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“…33,34,[36][37][38] Interestingly, Tan et al recently reported that a stable cycling of LiNi 0.76 Mn 0.14 Co 0.1 O 2 up to 4.8 V can be achieved by adding lithium difluorophosphate as a functional electrolyte additive to passivate the surface of the cathode material. 39 Without any doubt, the above examples have made clear statements on the issues associated with the bulk properties of oxide materials, and innovative solutions were also successfully proposed and implemented to address the intended issues. However, the major discrepancy among these examples is the underlying mechanism that oxide materials are armed to sense the change of the chemical environment around the oxide particles, either in an electrolyte solution or as a surface coating, so that the materials can alternate their bulk behaviour accordingly to reflect the change of the chemical environment.…”

Section: Role Of Protonsmentioning

confidence: 99%

Chasing protons in lithium-ion batteries

Chen

2022

Chem. Commun.

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Additive engineering for robust interphases to stabilize high-Ni layered structures at ultra-high voltage of 4.8 V

Cited by 242 publications

References 47 publications

Tailoring polymer electrolyte for high-voltage solid-state Li metal batteries working at ultra-low temperatures

Tailoring polymer electrolyte for high-voltage solid-state Li metal batteries working at ultra-low temperatures

Challenges and Modification Strategies of Ni-Rich Cathode Materials Operating at High-Voltage

Chasing protons in lithium-ion batteries

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