CO2 and O2 Evolution at High Voltage Cathode Materials of Li-Ion Batteries: A Differential Electrochemical Mass Spectrometry Study

化学 阴极 电解质 电化学 电极 电池(电) 无机化学 分析化学(期刊) 锂(药物) 物理化学 色谱法 量子力学 医学 物理 内分泌学 功率(物理)
作者
Hongsen Wang,Eric D. Rus,Takahito Sakuraba,Jun Kikuchi,Yasuyuki Kiya,Héctor D. Abruña
出处
期刊:Analytical Chemistry [American Chemical Society]
卷期号:86 (13): 6197-6201 被引量:128
标识
DOI:10.1021/ac403317d
摘要

A three-electrode differential electrochemical mass spectrometry (DEMS) cell has been developed to study the oxidative decomposition of electrolytes at high voltage cathode materials of Li-ion batteries. In this DEMS cell, the working electrode used was the same as the cathode electrode in real Li-ion batteries, i.e., a lithium metal oxide deposited on a porous aluminum foil current collector. A charged LiCoO2 or LiMn2O4 was used as the reference electrode, because of their insensitivity to air, when compared to lithium. A lithium sheet was used as the counter electrode. This DEMS cell closely approaches real Li-ion battery conditions, and thus the results obtained can be readily correlated with reactions occurring in real Li-ion batteries. Using DEMS, the oxidative stability of three electrolytes (1 M LiPF6 in EC/DEC, EC/DMC, and PC) at three cathode materials including LiCoO2, LiMn2O4, and LiNi(0.5)Mn(1.5)O4 were studied. We found that 1 M LiPF6 + EC/DMC electrolyte is quite stable up to 5.0 V, when LiNi(0.5)Mn(1.5)O4 is used as the cathode material. The EC/DMC solvent mixture was found to be the most stable for the three cathode materials, while EC/DEC was the least stable. The oxidative decomposition of the EC/DEC mixture solvent could be readily observed under operating conditions in our cell even at potentials as low as 4.4 V in 1 M LiPF6 + EC/DEC electrolyte on a LiCoO2 cathode, as indicated by CO2 and O2 evolution. The features of this DEMS cell to unveil solvent and electrolyte decomposition pathways are also described.
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