In situ monitoring of the electrochemically induced phase transition of thermodynamically metastable 1T-MoS 2 at nanoscale

• Published in: Nanoscale Vol. 12; no. 16; pp. 9246 - 9254
• Main Authors: Huang, Junxiao, Pan, Xuelei, Liao, Xiaobin, Yan, Mengyu, Dunn, Bruce, Luo, Wen, Mai, Liqiang
• Format: Journal Article
• Language: English
• Published: England 30.04.2020
• ISSN: 2040-3364; 2040-3372
• DOI: 10.1039/D0NR02161J

1T-MoS2 is widely used in the hydrogen evolution reaction (HER) due to its abundant active sites and good conductivity. However, 1T-MoS2 is thermodynamically metastable due to the distorted crystal structure. Recently, researchers have detected the J1 and A1g Raman peaks after the HER process and confirmed that the 2H-1T phase possesses good stability. Therefore, continuous HER is likely to transform 1T-MoS2 into a stable 2H-1T mixed phase. The in situ characterization of 1T-MoS2 individual nanosheets in the HER process is important to understand the intrinsic electrocatalytic behaviour at confined nanoscale, which has rarely been investigated. Herein, we built an individual 1T-MoS2 nanosheet micro-nano device by the intercalation of N-butyllithium into 2H-MoS2. Then, the device was kept at an overpotential (η) of 450 mV, which was much lower than the onset potential, for 20 minutes to ensure continuous HER. Through this electrochemical treatment, we successfully obtained a mixed phase of 2H-1T and monitored the electrochemical phase transition by in situ Raman mapping and atomic force microscopy (AFM). The HER performance of the 2H-1T phase was superior to that of 1T-MoS2 and 2H-MoS2. Additionally, computational simulations demonstrated that the 2H-1T phase exhibited optimal hydrogen adsorption energy. The presented work displays the excellent catalysis of the mixed phase obtained by the electrochemical phase transition, which provides new directions for improving the catalytic activity of TMDs.