期刊
NANO LETTERS
卷 16, 期 7, 页码 4082-4086出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.6b00773
关键词
Photoelectrochemistry; graphene; 2D materials; solar energy conversion; anticorrosion
类别
资金
- NSF [CHE-1214152]
- Link Energy Foundation
- Amgen Scholars program
- NSF MRSEC program through Columbia in the Center for Precision Assembly of Superstratic and Superatomic Solids [DMR-1420634]
- Nanoelectronics Research Initiative (NRI) through the Institute for Nanoelectronics Discovery and Exploration (INDEX)
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [1214152] Funding Source: National Science Foundation
The behavior of n-Si(111) photoanodes covered by monolayer sheets of fluorinated graphene (F-Gr) was investigated under a range of chemical and electrochemical conditions. The electrochemical behavior of n-Si/F-Gr and np(+)-Si/F-Gr photoanodes was compared to hydride-terminated n-Si (n-Si-H) and np(+)-Si-H electrodes in contact with aqueous Fe(CN)(6)(3/-4-) and Br-2/HBr electrolytes as well as in contact with a series of outer-sphere, one-electron redox couples in nonaqueous electrolytes. Illuminated n-Si/F-Gr and np(+)-Si/F-Gr electrodes in contact with an aqueous K-3(Fe(CN)(6)/K-4(Fe(CN)(6) solutions exhibited stable short-circuit photocurrent densities of similar to 10 mA cm(-2) for 100,000 s (>24 h), in comparison to bare Si electrodes, which yielded nearly a complete photocurrent decay over similar to 00 s. X-ray photoelectron spectra collected before and after exposure to aqueous anodic conditions showed that oxide formation at the Si surface was significantly inhibited for Si electrodes coated with F-Gr relative to bare Si electrodes exposed to the same conditions. The variation of the open-circuit potential for n-Si/F-Gr in contact with a series of nonaqueous electrolytes of varying reduction potential indicated that the n-Si/F-Gr did not form a buried junction with respect to the solution contact. Further, illuminated n-Si/FGr electrodes in contact with Br-2/HBr(aq) were significantly more electrochemically stable than n-Si-H electrodes, and n-Si/F-Gr electrodes coupled to a Pt catalyst exhibited ideal regenerative cell efficiencies of up to 5% for the oxidation of Br- to Br-2.
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