1. In situ electrochemical Raman investigation of charge storage in rGO and N-doped rGO
- Author
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Masanori Hara, Masamichi Yoshimura, Rohit Yadav, and Prerna Joshi
- Subjects
Materials science ,Graphene ,Intercalation (chemistry) ,Oxide ,Analytical chemistry ,General Physics and Astronomy ,02 engineering and technology ,Electrolyte ,010402 general chemistry ,021001 nanoscience & nanotechnology ,Electrochemistry ,01 natural sciences ,0104 chemical sciences ,law.invention ,chemistry.chemical_compound ,symbols.namesake ,Graphite intercalation compound ,chemistry ,law ,symbols ,Graphite ,Physical and Theoretical Chemistry ,0210 nano-technology ,Raman spectroscopy - Abstract
In this study, in situ electrochemical Raman spectroscopy was applied to clarify the charge storage mechanism in three types of anodes, synthetic graphite, reduced graphene oxide (rGO), and nitrogen-doped reduced graphene oxide (N-rGO). The Li+ intercalation phenomenon was measured in LiPF6 electrolyte solution using a modified coin cell setup. The synthetic graphite anode showed the splitting of the G peak at the potential E < 0.2 V vs. Li/Li+, corresponding to the formation of a graphite intercalation compound (GIC) and its second-order 2D peak was found to be red-shifted due to charge transfer and induced strain in the potential region of 0.5 to 0.15 V vs. Li/Li+. In the case of rGO, the lattice defects assisted in large and early intercalation of electrolyte ions, which is confirmed by the red-shift in the G peak (∼36 cm−1) and its early disappearance below 0.3 V vs. Li/Li+, respectively. Unlike rGO, nitrogen vacancies in N-rGO provide active sites for Li+ intercalation, resulting in enhanced charge transfer, displayed by the large red-shift in the G peak (∼55 cm−1) and blue-shift in the D peak. In addition, a new Raman peak at 1850 cm−1 was observed in N-rGO for the first time, corresponding to the formation of a reversible intermediate species from the interaction between Li+ and nitrogen vacancies. This work demonstrates the use of a simple in situ technique to get insight into the nano-carbon electrodes during device operation and to reveal the role of doped nitrogen atoms for Li+ intercalation.
- Published
- 2021
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