期刊
ACS APPLIED MATERIALS & INTERFACES
卷 13, 期 51, 页码 61139-61153出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c18777
关键词
Raman probing the surface effects; solvent blocking interface; charge-storage process; WiSE; salt-in-water electrolytes; impedance study of blocked interfaces
资金
- Brazilian funding agency CNPq [310544/2019-0]
- Brazilian funding agency FAPESP [2014/02163-7, 2017/11958-1, 2018/20756-6]
- FAPEMIG
- CNPq (PQ-2 Grant) [301095/2018-3]
- Shell
- ANP (Brazil's National Oil, Natural Gas and Biofuels Agency) through the R&D levy regulation
Comprehensive electrochemical and operando Raman studies were conducted to investigate the electrochemical stability window of supercapacitors using normal and highly concentrated electrolytes. The presence of a solvent blocking interface was confirmed to inhibit water-splitting, while a specific electrolyte was found to prevent water-splitting up to a certain voltage threshold. Additionally, the reversible nature of the charge-storage process was assessed under different polarization conditions.
Comprehensive electrochemical and operando Raman studies are performed to investigate the electrochemical stability window (ESW) of supercapacitors filled with normal (salt-in-water) and highly concentrated (water-in-salt, WiSE) electrolytes. Impedance and chronoamperometric experiments are employed and combined with cyclic voltammetry to correctly define the ESW for a WiSE-based device. The total absence of water-splitting resulted in phase angles close to -90 degrees in the impedance data. It is verified that a 17 m NaClO4 electrolyte avoids the water-splitting up to 1.8 V. Furthermore, Raman studies under dynamic and static polarization conditions corroborate the existence of a solvent blocking interface (SBI), which inhibits the occurrence of water-splitting. Also, the reversible nature of the charge-storage process is assessed as a function of the applied voltage. At extreme polarization, the SBI structure is disrupted, thus allowing the occurrence of water-splitting and anionic (ClO4-) intercalation between the graphene sheets.
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