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Title: Atomic layer oxidation on graphene sheets for tuning their oxidation levels, electrical conductivities, and band gaps

Journal Article · · Nanoscale
DOI: https://doi.org/10.1039/C8NR04013C · OSTI ID:1468151
ORCiD logo [1]; ORCiD logo [2];  [3];  [3];  [4]; ORCiD logo [5]; ORCiD logo [6]
  1. Xiamen Univ. of Technology (China). Fujian Provincial Key Lab. of Functional Materials and Applications. Inst. of Material Preparation and Applied Technology. School of Materials Science and Engineering
  2. Yuan Ze Univ., Taoyuan (Taiwan). Dept. of Chemical Engineering and Materials Science; Univ. of Tennessee, Knoxville, TN (United States). Dept. of Mechanical, Aerospace, and Biomedical Engineering
  3. Yuan Ze Univ., Taoyuan (Taiwan). Dept. of Chemical Engineering and Materials Science
  4. Univ. of Tennessee, Knoxville, TN (United States). Dept. of Mechanical, Aerospace, and Biomedical Engineering
  5. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Nuclear Science and Engineering. Dept. of Materials Science and Engineering; National Chiao Tung Univ., Hsinchu (Taiwan). Dept. of Materials Science and Engineering
  6. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Energy and Transportation Science Division
+ Show Author Affiliations

Graphene sheets that can exhibit electrical conducting and semiconducting properties are highly desirable and have potential applications in fiber communications, photodetectors, solar cells, semiconductors, and broadband modulators. However, there is currently no efficient method that is able to tune the band gap of graphene sheets. This paper adopts an efficient atomic layer oxidation (ALO) technique to cyclically increase the oxidation level of graphene sheets, thus, tuning their electrical conductance, band-gap structure, and photoluminescence (PL) response. The O/C atomic ratio as an increasing function of the ALO cycle number reflects two linear regions: 0.23% per cm2 per cycle (0–15 cycles) and 0.054% per cm2 per cycle (15–100 cycles). The excellent correlation coefficients reveal that the ALO process follows a self-limiting route to step-by-step oxidize graphene layers. The interlayer distance of ALO-graphene sheets shows an obvious increase after the ALO treatment, proved by X-ray diffraction. As analyzed by X-ray photon spectroscopy, the hydroxyl or epoxy group acts as a major contributor to the interlayer spacing distance and oxidation extent in the initial ALO stage, as compared to carbonyl and carboxyl groups. The ALO mechanism, based on Langmuir–Hinshelwood and Eley–Rideal models, is proposed to clarify the formation of oxygen functionalities and structural transformation from pristine graphene sheets to oxidized ones during the ALO cycle. With a tunable oxidation level, the electrical resistivity, semiconductor character, and PL response of ALO-graphene samples can be systematically controlled for desired applications. Finally, the ALO approach is capable of offering a straightforward route to tune the oxidation level of graphene sheets or other carbons.

Research Organization:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Yuan Ze Univ., Taoyuan (Taiwan); National Chiao Tung Univ., Hsinchu (Taiwan)
Sponsoring Organization:
USDOE; Ministry of Science and Technology of Taiwan
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1468151
Journal Information:
Nanoscale, Journal Name: Nanoscale Journal Issue: 33 Vol. 10; ISSN 2040-3364
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English

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Cited By (2)

Linear control of the oxidation level on graphene oxide sheets using the cyclic atomic layer reduction technique journal January 2019
Amino-functionalization on graphene oxide sheets using an atomic layer amidation technique journal January 2020

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