期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 125, 期 14, 页码 7701-7710出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.1c01265
关键词
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资金
- European Research Council (ERC) under the European Union's Horizon 2020 research and innovation programs [716539, 862453]
- Hungarian Academy of Sciences for the MTA Premium Post Doctorate Research Program [461029]
- Janos Bolyai Research Scholarship of the Hungarian Academy of Sciences
- New National Excellence Program of the Ministry for Innovation and Technology from the source of the National Research, Development and Innovation Fund [NKP-20-5]
- Ministry for Innovation and Technology [U'NKP-20-2]
The study investigates the impact of different surface domains on photoelectrochemical performance, revealing a decrease in PEC activity with thinner nanoflakes and a reduction in relative PEC activity due to introduced defects. Edge defects were found to have higher electrocatalytic activity compared to basal planes, although they also act as charge carrier recombination centers.
The exfoliation of layered materials into two-dimensional (2D) semiconductors creates new structural domains, for example, basal planes, defect-rich in-planes, and edge sites. These surface species affect the photoelectrochemical (PEC) performance, which in turn determines their applicability in solar energy conversion technologies. In this study, a custom-designed microdroplet cell-based spatially resolved PEC approach was employed to identify the structural parts and to measure the PEC activity of the mechanically exfoliated MoSe2 and WSe2 nanosheets for bulk, few-layer, and monolayer specimens. The PEC performance decreased with the decreasing thickness of nanoflakes, and the relative PEC activity (photo/total current) reduced by introducing more defects to the 2D flakes: 1-3% loss was found for in-plane defects and 30-40% for edge defects. While edge sites act as charge carrier recombination centers, their electrocatalytic activity is higher than that of the basal planes. The comparison of PEC activity of micromechanically and liquid phase exfoliated bulk and few-layer MoSe2 and WSe2 flakes further confirmed that the PEC performance of 2D flakes decreases with an increasing number of edge sites.
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