Using Exciton/Trion Dynamics to Spatially Monitor the Catalytic Activities of MoS2 during the Hydrogen Evolution Reaction

Fu-He Hsiao; Cheng-Chu Chung; Chun-Hao Chiang; Wei-Neng Feng; Wen-Yen Tzeng; Hung-Min Lin; Chien-Ming Tu; Heng-Liang Wu; Yu-Han Wang; Wei-Yen Woon; Hsiao-Chien Chen; Ching-Hsiang Chen; Chao-Yuan Lo; Man-Hong Lai; Yu-Ming Chang; Li-Syuan Lu; Wen-Hao Chang; Chun-Wei Chen; Chih-Wei Luo

doi:10.1021/acsnano.1c10380

Using Exciton/Trion Dynamics to Spatially Monitor the Catalytic Activities of MoS₂ during the Hydrogen Evolution Reaction

ACS Nano. 2022 Mar 22;16(3):4298-4307. doi: 10.1021/acsnano.1c10380. Epub 2022 Mar 7.

Authors

Fu-He Hsiao¹, Cheng-Chu Chung², Chun-Hao Chiang², Wei-Neng Feng¹, Wen-Yen Tzeng¹, Hung-Min Lin², Chien-Ming Tu¹, Heng-Liang Wu^{3

4}, Yu-Han Wang^{5

6}, Wei-Yen Woon^{5

6}, Hsiao-Chien Chen^{7

8}, Ching-Hsiang Chen⁹, Chao-Yuan Lo^{3

4}, Man-Hong Lai³, Yu-Ming Chang^{3

4}, Li-Syuan Lu¹, Wen-Hao Chang^{1

10}, Chun-Wei Chen^{2

4

10}, Chih-Wei Luo^{1

10

11

12}

Affiliations

¹ Department of Electrophysics, National Yang Ming Chiao Tung University, Hsinchu 30010, Taiwan.
² Department of Materials Science and Engineering, National Taiwan University, Taipei 10617, Taiwan.
³ Center for Condensed Matter Sciences, National Taiwan University, Taipei 10617, Taiwan.
⁴ Center of Atomic Initiative for New Materials (AI-MAT), National Taiwan University, Taipei 10617, Taiwan.
⁵ Department of Physics, National Central University, Taoyuan 32001, Taiwan.
⁶ Molecular Science and Technology Program, Taiwan International Graduate Program, Institute of Atomic and Molecular Science, Academia Sinica, Taipei 10617, Taiwan.
⁷ Center for Reliability Science and Technologies, Chang Gung University, Taoyuan 33302, Taiwan.
⁸ Kidney Research Center, Department of Nephrology, Chang Gung Memorial Hospital, Linkou, Taoyuan 333, Taiwan.
⁹ Sustainable Energy Development Center, National Taiwan University of Science and Technology, Taipei 106335, Taiwan.
¹⁰ Taiwan Consortium of Emergent Crystalline Materials (TCECM), Ministry of Science and Technology, Taipei 10622, Taiwan.
¹¹ Institute of Physics and Center for Emergent Functional Matter Science, National Yang Ming Chiao Tung University, Hsinchu 30010, Taiwan.
¹² National Synchrotron Radiation Research Center, Hsinchu 30076, Taiwan.

PMID: 35254822
DOI: 10.1021/acsnano.1c10380

Abstract

The adsorption and desorption of electrolyte ions strongly modulates the carrier density or carrier type on the surface of monolayer-MoS₂ catalyst during the hydrogen evolution reaction (HER). The buildup of electrolyte ions onto the surface of monolayer MoS₂ during the HER may also result in the formation of excitons and trions, similar to those observed in gate-controlled field-effect transistor devices. Using the distinct carrier relaxation dynamics of excitons and trions of monolayer MoS₂ as sensitive descriptors, an in situ microcell-based scanning time-resolved liquid cell microscope is set up to simultaneously measure the bias-dependent exciton/trion dynamics and spatially map the catalytic activity of monolayer MoS₂ during the HER. This operando probing technique used to monitor the interplay between exciton/trion dynamics and electrocatalytic activity for two-dimensional transition metal dichalcogenides provides an excellent platform to investigate the local carrier behaviors at the atomic layer/liquid electrolyte interfaces during electrocatalytic reaction.

Keywords: exciton dynamics; hydrogen evolution reaction (HER); monolayer MoS2; time-resolved microscopy; trion dynamics.