Faculty Advisor or Committee Member

Pratap M. Rao, Advisor

Faculty Advisor or Committee Member

Jamal Yagoobi, Committee Member

Faculty Advisor or Committee Member

Danielle L. Cote, Committee Member

Faculty Advisor or Committee Member

Adam C. Powell, Committee Member

Faculty Advisor or Committee Member

Lyubov V. Titova, Committee Member

Faculty Advisor or Committee Member

Ronald L. Grimm, Committee Member

Identifier

etd-3691

Abstract

Tin disulfide (SnS2) is a two-dimensional (2D) material with excellent properties and high prospects for low-cost solutions to catalytic and optoelectronic applications. In this work, vertical nanoflakes of SnS2 have been synthesized using custom-designed close space sublimation (CSS) system and investigated for applications in photoelectrochemical (PEC) water oxidation and metal-semiconductor-metal (MSM) photodetector. For the PEC application, vertical SnS2 nanoflakes grown directly on transparent conductive substrates have been used as photoanodes, which produce record photocurrents of 4.5 mA cm−2 for oxidation of a sulfite hole scavenger and 2.6 mA cm−2 for water oxidation without any hole scavenger, both at 1.23 VRHE in neutral electrolyte under simulated AM1.5G sunlight, and stable photocurrents for iodide oxidation in acidic electrolyte. This remarkable performance has been attributed to three main reasons: (1) high intrinsic carrier mobility of 330 cm2 V−1 s−1 and long photoexcited carrier lifetime of 1.3 ns in the nanoflakes, (2) the nanoflake height that balances the competing requirements of light absorption and charge transport, and (3) the unique stepped morphology of these nanoflakes that improves photocurrent by exposing multiple edge sites in every nanoflake. In another application, these SnS2 nanoflakes have been used to enhance the performance of lead sulfide quantum dot (PbS QDs) photodetectors by providing a high-mobility channel for photoexcited charges from PbS QDs, which results in 2 orders of magnitude enhancement in responsivity. The physical models and experimental findings presented in this dissertation can help engineer more cost-effective solutions for PEC water splitting and optoelectronics based on 2D metal dichalcogenides.

Publisher

Worcester Polytechnic Institute

Degree Name

PhD

Department

Mechanical Engineering

Project Type

Dissertation

Date Accepted

2020-05-07

Accessibility

Unrestricted

Subjects

2D Metal Dichalcogenides, Tin disulfide (SnS2) Nanoflakes, Photoelectrochemical Water Splitting, Photodetectors, Close Space Sublimation, Nanotechnology

Available for download on Friday, May 07, 2021

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