US EPA

4767746 

Journal Article 

Kinetics-Controlled Degradation Reactions at Crystalline LiPON/Lix CoO2 and Crystalline LiPON/Li-Metal Interfaces 

Leung, K; Pearse, AJ; Talin, AA; Fuller, EJ; Rubloff, GW; Modine, NA 

2018 

Yes 

ChemSusChem
ISSN: 1864-5631
EISSN: 1864-564X 

11 

12 

1956-1969 

English 

29603655 

10.1002/cssc.201800027 

WOS:000435934200010 

Detailed understanding of solid-solid interface structure-function relationships is critical for the improvement and wide deployment of all-solid-state batteries. The interfaces between lithium phosphorous oxynitride (LiPON) solid electrolyte material and lithium metal anode, and between LiPON and Lix CoO2 cathode, have been reported to generate solid-electrolyte interphase (SEI)-like products and/or disordered regions. Using electronic structure calculations and crystalline LiPON models, we predict that LiPON models with purely P-N-P backbones are kinetically inert towards lithium at room temperature. In contrast, transfer of oxygen atoms from low-energy Lix CoO2 (104) surfaces to LiPON is much faster under ambient conditions. The mechanisms of the primary reaction steps, LiPON structural motifs that readily reacts with lithium metal, experimental results on amorphous LiPON to partially corroborate these predictions, and possible mitigation strategies to reduce degradations are discussed. LiPON interfaces are found to be useful case studies for highlighting the importance of kinetics-controlled processes during battery assembly at moderate processing temperatures.