DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Tuning oxidation level, electrical conductance and band gap structure on graphene sheets by cyclic atomic layer reduction technique

Abstract

The present work develops an atomic layer reduction (ALR) method to accurately tune oxidation level, electrical conductance, band-gap structure, and photoluminescence (PL) response of graphene oxide (GO) sheets. The ALR route is carried out at 200 °C within ALR cycle number of 10–100. The ALR treatment is capable of striping surface functionalities (e.g., hydroxyl, carbonyl, and carboxylic groups), producing thermally-reduced GO sheets. The ALR cycle number serves as a controlling factor in adjusting the crystalline, surface chemistry, electrical, optical properties of GO sheets. With increasing the ALR cycle number, ALR-GO sheets display a high crystallinity, a low oxidation level, an improved electrical conductivity, a narrow band gap, and a tunable PL response. Finally, on the basis of the results, the ALR technique offers a great potential for accurately tune electrical and optical properties of carbon materials through the cyclic removal of oxygen functionalities, without any complicated thermal and chemical desorption processes.

Authors:
 [1];  [2];  [3];  [4]; ORCiD logo [5]; ORCiD logo [6]
  1. Xiamen Univ. of Technology, Xiamen, Fujian (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. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Nuclear Science and Engineering and Dept. of Materials Science and Engineering; National Central Univ., Taoyuan (Taiwan). Inst. of Materials Science and Engineering
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Energy and Transportation Science Division
  6. Univ. of Tennessee, Knoxville, TN (United States). Dept. of Mechanical, Aerospace, and Biomedical Engineering
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1439927
Grant/Contract Number:  
AC05-00OR22725; MOST 105-2628-E-155-002-MY3; MOST 105-2221-E-155-014-MY3
Resource Type:
Accepted Manuscript
Journal Name:
Carbon
Additional Journal Information:
Journal Volume: 137; Journal Issue: C; Journal ID: ISSN 0008-6223
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Gu, Si-Yong, Hsieh, Chien-Te, Lin, Tzu-Wei, Chang, Jeng-Kuei, Li, Jianlin, and Gandomi, Yasser Ashraf. Tuning oxidation level, electrical conductance and band gap structure on graphene sheets by cyclic atomic layer reduction technique. United States: N. p., 2018. Web. doi:10.1016/j.carbon.2018.05.024.
Gu, Si-Yong, Hsieh, Chien-Te, Lin, Tzu-Wei, Chang, Jeng-Kuei, Li, Jianlin, & Gandomi, Yasser Ashraf. Tuning oxidation level, electrical conductance and band gap structure on graphene sheets by cyclic atomic layer reduction technique. United States. https://doi.org/10.1016/j.carbon.2018.05.024
Gu, Si-Yong, Hsieh, Chien-Te, Lin, Tzu-Wei, Chang, Jeng-Kuei, Li, Jianlin, and Gandomi, Yasser Ashraf. Sat . "Tuning oxidation level, electrical conductance and band gap structure on graphene sheets by cyclic atomic layer reduction technique". United States. https://doi.org/10.1016/j.carbon.2018.05.024. https://www.osti.gov/servlets/purl/1439927.
@article{osti_1439927,
title = {Tuning oxidation level, electrical conductance and band gap structure on graphene sheets by cyclic atomic layer reduction technique},
author = {Gu, Si-Yong and Hsieh, Chien-Te and Lin, Tzu-Wei and Chang, Jeng-Kuei and Li, Jianlin and Gandomi, Yasser Ashraf},
abstractNote = {The present work develops an atomic layer reduction (ALR) method to accurately tune oxidation level, electrical conductance, band-gap structure, and photoluminescence (PL) response of graphene oxide (GO) sheets. The ALR route is carried out at 200 °C within ALR cycle number of 10–100. The ALR treatment is capable of striping surface functionalities (e.g., hydroxyl, carbonyl, and carboxylic groups), producing thermally-reduced GO sheets. The ALR cycle number serves as a controlling factor in adjusting the crystalline, surface chemistry, electrical, optical properties of GO sheets. With increasing the ALR cycle number, ALR-GO sheets display a high crystallinity, a low oxidation level, an improved electrical conductivity, a narrow band gap, and a tunable PL response. Finally, on the basis of the results, the ALR technique offers a great potential for accurately tune electrical and optical properties of carbon materials through the cyclic removal of oxygen functionalities, without any complicated thermal and chemical desorption processes.},
doi = {10.1016/j.carbon.2018.05.024},
journal = {Carbon},
number = C,
volume = 137,
place = {United States},
year = {Sat May 12 00:00:00 EDT 2018},
month = {Sat May 12 00:00:00 EDT 2018}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 10 works
Citation information provided by
Web of Science

Figures / Tables:

Fig. 1 Fig. 1: Flowchart (upper) and mechanism (lower) for describing one ALR cycle, including (i) H2-containing pulse (10 s), (ii) N2 purge (10 s), and (iii) pumping (10 s). (A colour version of this figure can be viewed online.)

Save / Share:

Works referenced in this record:

Thermal Conductance of an Individual Single-Wall Carbon Nanotube above Room Temperature
journal, January 2006

  • Pop, Eric; Mann, David; Wang, Qian
  • Nano Letters, Vol. 6, Issue 1
  • DOI: 10.1021/nl052145f

Novel Pyrolyzed Polyaniline-Grafted Silicon Nanoparticles Encapsulated in Graphene Sheets As Li-Ion Battery Anodes
journal, April 2014

  • Li, Zhe-Fei; Zhang, Hangyu; Liu, Qi
  • ACS Applied Materials & Interfaces, Vol. 6, Issue 8
  • DOI: 10.1021/am501239r

Shape-Tailorable Graphene-Based Ultra-High-Rate Supercapacitor for Wearable Electronics
journal, May 2015


Carbon Nanohorn-Derived Graphene Nanotubes as a Platinum-Free Fuel Cell Cathode
journal, October 2015

  • Unni, Sreekuttan M.; Illathvalappil, Rajith; Bhange, Siddheshwar N.
  • ACS Applied Materials & Interfaces, Vol. 7, Issue 43
  • DOI: 10.1021/acsami.5b07802

2D Hybrid Nanostructure of Reduced Graphene Oxide–CdS Nanosheet for Enhanced Photocatalysis
journal, June 2015

  • Bera, Rajesh; Kundu, Simanta; Patra, Amitava
  • ACS Applied Materials & Interfaces, Vol. 7, Issue 24
  • DOI: 10.1021/acsami.5b03800

Photogenerated Carriers Transfer in Dye–Graphene–SnO 2 Composites for Highly Efficient Visible-Light Photocatalysis
journal, December 2013

  • Zhuang, Shendong; Xu, Xiaoyong; Feng, Bing
  • ACS Applied Materials & Interfaces, Vol. 6, Issue 1
  • DOI: 10.1021/am4047014

Enhanced adsorption and photodegradation of phenol in aqueous suspensions of titania/graphene oxide composite catalysts
journal, October 2016

  • Fu, Chun-Chieh; Juang, Ruey-Shin; Huq, Mohammad Mahmudul
  • Journal of the Taiwan Institute of Chemical Engineers, Vol. 67
  • DOI: 10.1016/j.jtice.2016.07.043

Nanoelectronic circuits based on two-dimensional atomic layer crystals
journal, January 2014


Thermal conductivity from hierarchical heat sinks using carbon nanotubes and graphene nanosheets
journal, January 2015

  • Hsieh, Chien-Te; Lee, Cheng-En; Chen, Yu-Fu
  • Nanoscale, Vol. 7, Issue 44
  • DOI: 10.1039/C5NR04993H

Thermal transport in stereo carbon framework using graphite nanospheres and graphene nanosheets
journal, September 2016


Preparation of Graphitic Oxide
journal, March 1958

  • Hummers, William S.; Offeman, Richard E.
  • Journal of the American Chemical Society, Vol. 80, Issue 6, p. 1339-1339
  • DOI: 10.1021/ja01539a017

Functionalization of Graphene via 1,3-Dipolar Cycloaddition
journal, May 2010

  • Quintana, Mildred; Spyrou, Konstantinos; Grzelczak, Marek
  • ACS Nano, Vol. 4, Issue 6
  • DOI: 10.1021/nn100883p

Large-Area Synthesis of High-Quality and Uniform Graphene Films on Copper Foils
journal, May 2009


High-yield production of graphene by liquid-phase exfoliation of graphite
journal, August 2008

  • Hernandez, Yenny; Nicolosi, Valeria; Lotya, Mustafa
  • Nature Nanotechnology, Vol. 3, Issue 9, p. 563-568
  • DOI: 10.1038/nnano.2008.215

Honeycomb Carbon: A Review of Graphene
journal, January 2010

  • Allen, Matthew J.; Tung, Vincent C.; Kaner, Richard B.
  • Chemical Reviews, Vol. 110, Issue 1, p. 132-145
  • DOI: 10.1021/cr900070d

A green approach to the synthesis of high-quality graphene oxide flakes via electrochemical exfoliation of pencil core
journal, January 2013

  • Liu, Jilei; Yang, Huanping; Zhen, Saw Giek
  • RSC Advances, Vol. 3, Issue 29
  • DOI: 10.1039/c3ra41366g

Electrochemical exfoliation of graphite for producing graphene using saccharin
journal, January 2015

  • M. K., Punith Kumar; Shanthini, S.; Srivastava, Chandan
  • RSC Advances, Vol. 5, Issue 66
  • DOI: 10.1039/C5RA07846F

Low defect concentration few-layer graphene using a two-step electrochemical exfoliation
journal, February 2015


In Situ Synthesis of Metal Nanoparticles on Single-Layer Graphene Oxide and Reduced Graphene Oxide Surfaces
journal, May 2009

  • Zhou, Xiaozhu; Huang, Xiao; Qi, Xiaoying
  • The Journal of Physical Chemistry C, Vol. 113, Issue 25
  • DOI: 10.1021/jp903821n

Electrochemical Capacitors Based on Graphene Oxide Sheets Using Different Aqueous Electrolytes
journal, June 2011

  • Hsieh, Chien-Te; Hsu, Shu-Min; Lin, Jia-Yi
  • The Journal of Physical Chemistry C, Vol. 115, Issue 25
  • DOI: 10.1021/jp2032687

High-Yield Synthesis of Few-Layer Graphene Flakes through Electrochemical Expansion of Graphite in Propylene Carbonate Electrolyte
journal, June 2011

  • Wang, Junzhong; Manga, Kiran Kumar; Bao, Qiaoliang
  • Journal of the American Chemical Society, Vol. 133, Issue 23
  • DOI: 10.1021/ja203725d

Semiconducting nature of the oxygen-adsorbed graphene sheet
journal, June 2008

  • Ito, Jun; Nakamura, Jun; Natori, Akiko
  • Journal of Applied Physics, Vol. 103, Issue 11
  • DOI: 10.1063/1.2939270

Optimal preparation of Pt/TiO2 photocatalysts using atomic layer deposition
journal, November 2010


Atomic Layer Deposition of Iridium Thin Films
journal, January 2004

  • Aaltonen, Titta; Ritala, Mikko; Sammelselg, Väino
  • Journal of The Electrochemical Society, Vol. 151, Issue 8
  • DOI: 10.1149/1.1761011

Area-Selective Atomic Layer Deposition of Platinum on YSZ Substrates Using Microcontact Printed SAMs
journal, January 2007

  • Jiang, Xirong; Bent, Stacey F.
  • Journal of The Electrochemical Society, Vol. 154, Issue 12
  • DOI: 10.1149/1.2789301

Size-controlled platinum nanoparticles prepared by modified-version atomic layer deposition for ethanol oxidation
journal, February 2015


Ultralow Loading Pt Nanocatalysts Prepared by Atomic Layer Deposition on Carbon Aerogels
journal, August 2008

  • King, Jeffrey S.; Wittstock, Arne; Biener, Juergen
  • Nano Letters, Vol. 8, Issue 8, p. 2405-2409
  • DOI: 10.1021/nl801299z

Atomic Layer Deposition of Platinum Nanoparticles on Carbon Nanotubes for Application in Proton‐Exchange Membrane Fuel Cells
journal, June 2009


Platinum electrocatalysts attached to carbon nanotubes by atomic layer deposition with different cycle numbers
journal, January 2014

  • Hsieh, Chien-Te; Liu, Yung-Ying; Tzou, Dong-Ying
  • Journal of the Taiwan Institute of Chemical Engineers, Vol. 45, Issue 1
  • DOI: 10.1016/j.jtice.2013.07.001

Atomic Layer Deposition of Platinum Nanocatalysts onto Three-Dimensional Carbon Nanotube/Graphene Hybrid
journal, December 2012

  • Hsieh, Chien-Te; Liu, Yung-Ying; Tzou, Dong-Ying
  • The Journal of Physical Chemistry C, Vol. 116, Issue 51
  • DOI: 10.1021/jp303552j

Influence of oxygen treatment on electric double-layer capacitance of activated carbon fabrics
journal, April 2002


Silver nanorods attached to graphene sheets as anode materials for lithium-ion batteries
journal, October 2013


Electrochemical Properties of Graphene Paper Electrodes Used in Lithium Batteries
journal, July 2009

  • Wang, Caiyun; Li, Dan; Too, Chee O.
  • Chemistry of Materials, Vol. 21, Issue 13
  • DOI: 10.1021/cm900764n

Surface analysis of carbon black waste materials from tire residues
journal, March 1999


Vapor adsorption on coal- and wood-based chemically activated carbons
journal, January 1999


Dye-sensitized solar cells equipped with graphene-based counter electrodes with different oxidation levels
journal, July 2012


Fabrication of Graphene-Based Electrochemical Capacitors
journal, January 2012

  • Hsieh, Chien-Te; Hsu, Shu-Min; Lin, Jia-Yi
  • Japanese Journal of Applied Physics, Vol. 51, Issue 1
  • DOI: 10.1143/JJAP.51.01AH06

Graphite Oxide with Different Oxygenated Levels for Hydrogen and Oxygen Production from Water under Illumination: The Band Positions of Graphite Oxide
journal, October 2011

  • Yeh, Te-Fu; Chan, Fei-Fan; Hsieh, Chien-Te
  • The Journal of Physical Chemistry C, Vol. 115, Issue 45
  • DOI: 10.1021/jp204856c

Tuning the Electronic Structure of Graphite Oxide through Ammonia Treatment for Photocatalytic Generation of H 2 and O 2 from Water Splitting
journal, March 2013

  • Yeh, Te-Fu; Chen, Shean-Jen; Yeh, Chen-Sheng
  • The Journal of Physical Chemistry C, Vol. 117, Issue 13
  • DOI: 10.1021/jp312613r

Photocatalytic reduction of carbon dioxide to methanol using a ruthenium trinuclear polyazine complex immobilized on graphene oxide under visible light irradiation
journal, January 2014

  • Kumar, Pawan; Sain, Bir; Jain, Suman L.
  • Journal of Materials Chemistry A, Vol. 2, Issue 29
  • DOI: 10.1039/c4ta01494d

Selective band gap manipulation of graphene oxide by its reduction with mild reagents
journal, November 2015


Deep Ultraviolet to Near-Infrared Emission and Photoresponse in Layered N-Doped Graphene Quantum Dots
journal, May 2014

  • Tang, Libin; Ji, Rongbin; Li, Xueming
  • ACS Nano, Vol. 8, Issue 6
  • DOI: 10.1021/nn501796r

Works referencing / citing this record:

Amino-functionalization on graphene oxide sheets using an atomic layer amidation technique
journal, January 2020

  • Gu, Siyong; Hsieh, Chien-Te; Mallick, Bikash Chandra
  • Journal of Materials Chemistry C, Vol. 8, Issue 2
  • DOI: 10.1039/c9tc05748j

Linear control of the oxidation level on graphene oxide sheets using the cyclic atomic layer reduction technique
journal, January 2019

  • Mallick, Bikash Chandra; Hsieh, Chien-Te; Yin, Ken-Ming
  • Nanoscale, Vol. 11, Issue 16
  • DOI: 10.1039/c8nr10118c

Graphene materials as a superior platform for advanced sensing strategies against gaseous ammonia
journal, January 2018

  • Vikrant, Kumar; Kumar, Vanish; Kim, Ki-Hyun
  • Journal of Materials Chemistry A, Vol. 6, Issue 45
  • DOI: 10.1039/c8ta07669c

Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.