Ultrasensitive gas detection of large-area boron-doped graphene
- Ruitao Lva,b,c1,
- Gugang Chend1,
- Qing Lie1,
- Amber McCrearyb,c1,
- Andrés Botello-Méndezf1,
- S. V. Morozovg,
- Liangbo Liangh,
- Xavier Declerckf,
- Nestor Perea-Lópezb,c,
- David A. Culleni,
- Simin Fengb,c,
- Ana Laura Elíasb,c,
- Rodolfo Cruz-Silvaj,
- Kazunori Fujisawab,c,
- Morinobu Endoj,
- Feiyu Kanga,
- Jean-Christophe Charlierf,
- Vincent Meunierh,
- Minghu Pank,
- Avetik R. Harutyunyand,
- Konstantin S. Novoselovg, and
- Mauricio Terronesb,c,j,l,m,2
- aKey Laboratory of Advanced Materials of Ministry of Education of China, School of Materials Science and Engineering, Tsinghua University, Beijing, 100084, China;
- bDepartment of Physics, The Pennsylvania State University, University Park, PA 16802;
- cCenter for 2-Dimensional and Layered Materials, The Pennsylvania State University, University Park, PA 16802;
- dHonda Research Institute USA Inc., Columbus, OH 43212;
- eInstitute of Functional Nano and Soft Materials and Collaborative Innovation Center of Suzhou Science and Technology, Soochow University, Jiangsu 215123, China;
- fInstitute of Condensed Matter and Nanosciences, Université catholique de Louvain, 1348 Louvain-la-Neuve, Belgium;
- gSchool of Physics & Astronomy, University of Manchester, Manchester, M13 9PL, United Kingdom;
- hDepartment of Physics, Applied Physics and Astronomy, Rensselaer Polytechnic Institute, Troy, NY 12180;
- iMaterials Science & Technology Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831;
- jResearch Center for Exotic Nanocarbons, Shinshu University, Wakasato 4-17-1, Nagano 380-8553, Japan;
- kSchool of Physics, Huazhong University of Science and Technology, Wuhan 430074, China;
- lDepartment of Chemistry, The Pennsylvania State University, University Park, PA 16802;
- mDepartment of Materials Science & Engineering, The Pennsylvania State University, University Park, PA 16802
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Edited by Manish Chhowalla, Rutgers, Piscataway, NJ, and accepted by the Editorial Board September 28, 2015 (received for review March 26, 2015)
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Fig. 1.Morphology of BG sheets. (A) Photograph of BG sheet (1.6 cm × 1.2 cm) transferred onto SiO2/Si substrate. (B and C) Aberration-corrected medium-angle annular dark-field STEM images of BG sheets. The monolayer region is shown in green. (D) SAED pattern depicting the hexagonal characteristic of the doped graphene lattice. Both C and D show that the hexagonal lattice of graphene is not perturbed even with substitutional boron doping. (E) XPS B1s fine scan of BG and PG samples.
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Fig. 2.Atomic-scale structure of boron dopants in as-synthesized BG sheets. (A) Large-area STM image of the BG illustrating the presence of numerous B dopants with similar croissant-like configuration (highlighted by white arrows). (B) Highly resolved experimental STM image of a croissant-like feature. (C) Simulated STM image and corresponding ball–stick structural model of B3 dopant. (D) Simulated STS of the B3-doping region shown in C. (E) dI/dV curves measured on B3 dopants (blue solid curve) and on nondoped graphene region (red dot curve).
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Fig. 3.Raman analysis of as-transferred BG sheets on SiO2/Si substrate. (A) Typical Raman spectra of PG (nondoped) and BG sheets. The Raman laser line is 514 nm. (B) D-peak over G-peak intensity ratio (ID/IG) mapping of BG. (C) Position distributions of G peak and (D) Two-dimensional peak with the corresponding ID/IG ratios of BG sheets.
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Fig. 4.Comparison of sensor response between PG (nondoped) and BG sheets. (A and B) Sensor response of PG sheets versus time recorded with the sensor exposed to NO2 (A) and NH3 (B). (C and D) Corresponding gas sensing on BG sheets when the sensor was exposed to NO2 (C) and NH3 (D). All experiments were carried out under in situ UV light illumination. Successive experiments were done after the device had been recovered. E and F demonstrate the difference of charge density with respect to the isolated atoms for the B3-doped graphene with NO2 and NH3 molecules, respectively.
