Electrolyte-induced surface transformation and transition-metal dissolution of fully delithiated LiNi0.8Co0.15Al0.05O2

DOI: 10.1021/acs.langmuir.7b00863

Authors: Nicholas V. Faenza (Rutgers University) , Zachary W. Lebens-Higgins (Binghamton University) , Pinaki Mukherjee (Rutgers University) , Shawn Sallis (Binghamton University) , Nathalie Pereira (Rutgers University) , Fadwa Badway (Rutgers University) , Anna Halajko (Rutgers University) , Gerbrand Ceder (University of California) , Frederic Cosandey (Rutgers University) , Louis F. J. Piper (Binghamton University) , Glenn G. Amatucci (Rutgers University)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Langmuir

State: Published (Approved)
Published: June 2017
Diamond Proposal Number(s): 12764

Abstract: Enabling practical utilization of layered R-3m positive electrodes near full delithiation requires an enhanced understanding of the complex electrode-electrolyte interactions that often induce failure. Using Li[Ni0.8Co0.15Al0.05]O2 (NCA) as a model layered compound, the chemical and structural stability in a strenuous thermal and electrochemical environment was explored. Operando microcalorimetry and electrochemical impedance spectroscopy identified a fingerprint for a structural decomposition and transition metal dissolution reaction that occurs on the positive electrode at full delithiation. Surface sensitive characterization techniques, including X-ray absorption spectroscopy and high resolution transmission electron microscopy, measured a structural and morphological transformation of the surface and subsurface regions of NCA. Despite the bulk structural integrity being maintained, NCA surface degradation at a high state of charge induces excessive transition metal dissolution and significant positive electrode impedance development, resulting in a rapid decrease of electrochemical performance. Additionally, the impact of electrolyte salt, positive electrode surface area, and surface Li2CO3 content on the magnitude and character of the dissolution reaction was studied.

Journal Keywords: Electrical properties; Electrodes; Dissolution; Electrochemical cells; Electrolytes

Diamond Keywords: Batteries; Lithium-ion

Subject Areas: Chemistry, Materials, Energy


Instruments: I09-Surface and Interface Structural Analysis

Other Facilities: 8.0.1 at ALS

Added On: 22/06/2017 09:37

Discipline Tags:

Energy Storage Energy Physical Chemistry Energy Materials Chemistry Materials Science

Technical Tags:

Spectroscopy X-ray Absorption Spectroscopy (XAS)