Catalytic and Electronic Activity of Transition Metal Dichalcogenides Heterostructures
By: Baichang Li
Publisher: [publisher not identified]
Published: 2021
Place of publication: [New York, N.Y.?]
Language: eng
Description: The synthesis of transition metal dichalcogenides (TMDs) are crucial to realization of their real-world applications in electronic, optoelectronic and chemical devices. However, the fabrication yield in terms of material quality, crystal size, defect density are poorly controlled. In this work, by employing the up-to-date stack-and-transfer and nano fabrication techniques, synthetic TMDs that obtained from different growth methods with various crystal qualities were studied. In most of the cases, better crystals with lower defect densities and larger crystal domain sizes are preferred. Self-flux method was developed to obtain better quality crystals comparing to the traditional chemical vapor transport, as characterized by lower defect densities. BN encapsulating graphene device platform was utilized and TMDs monolayers with different defect densities was inserted in between the BN/graphene interface, where intrinsic defects from the TMDs disturbed the electronic environment of graphene.

With the better TMD crystal insertion, we obtain much better electrical performed device in terms of hysteresis, FWHM of Dirac peak and electron mobility. This device also showed advantage in quantum transport measurements . On the other hand, the presence of defects are not always undesired, especially when it comes to serve as electrocatalysts, in which most of the reactions take place at vacancy sites. However, similar to most of the MoS2 electronic devices, forming barrier-free metal semiconductor contact is the major challenge. We develop a platform that contact resistance could be monitored simultaneously with electrochemical activity. In this platform, the total device resistance is significantly reduced before electrochemical reaction happens while the intrinsic catalytic activity of the MoS₂ can be extracted. With this platform, we found the intrinsic catalytic activity of MoS₂ strongly correlated to H-coverage on its surface. By adding molecular mediator into electrolytes, H-coverage and the resulting HER activity was enhanced via “Catch and Release” mechanism. Molecular simulation was performed to support our experimental results.
Notes: Department: Mechanical Engineering.

Thesis advisor: James C. Hone.

Thesis (Ph.D.)--Columbia University, 2021.