Zhefan Wang, Bin Zhao, Bing Xiao, Yang Li, Ming Cai, Chenglong Yang, Guangwen Cheng, Song Yang, Zhongxu Guo, Jian Cheng, Xiaogang Han
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引用次数: 0
Abstract
Nitrogen-doped porous carbon has been widely used in electrochemical energy storage, particularly in electrochemical double-layer capacitors (EDLCs), where it demonstrates excellent capacitance performance. However, the impact of nitrogen doping on the migration of electrolyte ions and the rapid decay of electrochemical performance at high temperatures has been rarely reported. In this work, a series of advanced characterizations, such as electrochemical quartz crystal microbalance (EQCM), time-of-flight secondary ion mass spectrometry (TOF-SIMS), and synchrotron radiation-based X-ray absorption near edge structure (XANES), were employed to analyze ion migration, deposition, and decomposition. Combining first-principles calculations, it was proved that the high-energy state lone pair electrons of amine and pyrrole-N trigger the continuous deposition/decomposition of anions BF4-, and prevent the deposition of cations SBP+. The deposited and decomposed cations further formed a passivation interface, which hindered ion migration. This interface led to dramatic fluctuations in electrode mass changes during charging and discharging, and reduced the total amount of ion migration. This work provides a novel kinetic study of ion migration within the electrochemical interface of nitrogen-doped porous carbon, which could contribute to enhancing the specific capacitance and cycle life of supercapacitors.
期刊介绍:
Electrochimica Acta is an international journal. It is intended for the publication of both original work and reviews in the field of electrochemistry. Electrochemistry should be interpreted to mean any of the research fields covered by the Divisions of the International Society of Electrochemistry listed below, as well as emerging scientific domains covered by ISE New Topics Committee.