Journal
ENERGY STORAGE MATERIALS
Volume 41, Issue -, Pages 495-504Publisher
ELSEVIER
DOI: 10.1016/j.ensm.2021.06.018
Keywords
Ni-rich layered cathode; Dendritic mesoporous silica; Electrolyte additive; Cathode/electrolyte interphase; Harsh operating conditions
Funding
- National Key R&D Program of China [2016YFB0100301]
- National Natural Science Foundation of China [21875022, 51802020]
- Natural Science Foundation of Chongqing, China [cstc2020jcyj-msxmX0654, cstc2020jcyj-msxmX0589]
- Science and Technology Innovation Foundation of Beijing Institute of Technology Chongqing Innovation Center [2020CX5100006]
- Young Elite Scientists Sponsorship Program by CAST [2018QNRC001]
- Beijing Institute of Technology Research Fund Program for Young Scholars
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In this study, a self-reconstructive cathode/electrolyte interphase (CEI) layer with good interfacial stability was designed for Ni-rich cathode by incorporating dendritic mesoporous silica (DMS) as a multifunctional electrolyte additive. The sample with a self-reconstructive CEI layer exhibited significantly superior cyclic stability under extended cut-off voltage or elevated temperature, and the flame-retardant effect of DMS additive contributed towards the thermal stability of the electrolyte and electrode, improving the safety aspect of the battery. This work provides new insights into reducing undesired self-reinforced failure process in Ni-rich cathode and reconstructing a self-healing CEI layer for high-safety, high-voltage lithium-ion batteries.
To achieve widespread adoption of Ni-rich layered oxides in commercial applications, it is highly necessary to address their cyclic stabilities and safety aspects under prolonged and harsh operating conditions, which will aggravate the simultaneous degradation of the Ni-rich cathode and electrolyte due to the more serious interfacial side reactions between them. Herein, a self-reconstructive cathode/electrolyte interphase (CEI) layer with good interfacial stability was designed and constructed for Ni-rich cathode, through the incorporation of dendritic mesoporous silica (DMS) with rich surface silicon-hydroxyl groups as a multifunctional electrolyte additive. The DMS shows the ability to reconstruct the CEI layer in real time, i.e., endowing the CEI layer with defluorination function, spontaneously formed LiPO2F2, and in-situ formed anti-fluorination protective layer with enhanced electron and Li+ diffusion. As expected, the sample with a self-reconstructive CEI layer exhibits significantly superior cyclic stability compared to the pristine one under extended cut-offvoltage (4.5 V) or elevated temperature (55 degrees C). Notably, the flame-retardant effect of DMS additive can also contribute towards the thermal stability of the electrolyte and electrode, which will effectively improve the safety aspect of the battery. Thus, this work provides new insights into reducing undesired self-reinforced failure process in Ni-rich cathode and reconstructing a self-healing CEI layer for high-safety, high-voltage lithium-ion batteries.
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