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Title: Boron Doping and Defect Engineering of Graphene Aerogels for Ultrasensitive NO 2 Detection

Abstract

In this study, boron-doped and defect-engineered graphene aerogels are prepared using triphenyl boron as a boron precursor and subsequent heat treatments. The boron chemistry and concentration in the graphene lattice are found to be highly dependent on the temperature used to activate boron. At 1500 °C, boron is incorporated at 3.2 atom % through a combination of B–C, B–N, and B–O bonds. At 1750 °C, the boron concentration decreases to 0.7 atom % and is predominantly incorporated through B–N bonding. Higher temperatures result in complete expulsion of boron from the lattice, leaving behind defects that are found to be beneficial for NO 2 gas detection. The gas sensing properties are explored to gain insight into the impact of boron chemistry on the sensing performance. A highly sensitive and selective conductometric NO 2 sensor is fabricated on a low-power microheater. Defect-engineered graphene aerogels with no boron remaining have superior gas detection properties. At an optimum sensing temperature of 240 °C, the defect-engineered aerogel has a theoretical detection limit of 7 ppb for NO 2 and response and recovery times of 100 and 300 s, respectively, with excellent selectivity over ammonia and hydrogen. Lastly, the superior gas sensing performance of defect-engineered graphenemore » aerogels has remarkable implications for their performance in catalysis and energy storage applications.« less

Authors:
ORCiD logo [1];  [2];  [1];  [3];  [3];  [3]; ORCiD logo [4];  [3];  [4];  [1]
  1. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Univ. of California, Berkeley, CA (United States); Hangzhou Dianzi University (China)
  3. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
  4. Univ. of California, Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
OSTI Identifier:
1548340
Report Number(s):
LLNL-JRNL-752424
Journal ID: ISSN 1932-7447; 938636
Grant/Contract Number:  
AC52-07NA27344; AC02-05-CH11231
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 122; Journal Issue: 35; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Turner, Sally, Yan, Wenjun, Long, Hu, Nelson, Art J., Baker, Alex, Lee, Jonathan R. I., Carraro, Carlo, Worsley, Marcus A., Maboudian, Roya, and Zettl, Alex. Boron Doping and Defect Engineering of Graphene Aerogels for Ultrasensitive NO 2 Detection. United States: N. p., 2018. Web. doi:10.1021/acs.jpcc.8b05984.
Turner, Sally, Yan, Wenjun, Long, Hu, Nelson, Art J., Baker, Alex, Lee, Jonathan R. I., Carraro, Carlo, Worsley, Marcus A., Maboudian, Roya, & Zettl, Alex. Boron Doping and Defect Engineering of Graphene Aerogels for Ultrasensitive NO 2 Detection. United States. doi:10.1021/acs.jpcc.8b05984.
Turner, Sally, Yan, Wenjun, Long, Hu, Nelson, Art J., Baker, Alex, Lee, Jonathan R. I., Carraro, Carlo, Worsley, Marcus A., Maboudian, Roya, and Zettl, Alex. Tue . "Boron Doping and Defect Engineering of Graphene Aerogels for Ultrasensitive NO 2 Detection". United States. doi:10.1021/acs.jpcc.8b05984. https://www.osti.gov/servlets/purl/1548340.
@article{osti_1548340,
title = {Boron Doping and Defect Engineering of Graphene Aerogels for Ultrasensitive NO 2 Detection},
author = {Turner, Sally and Yan, Wenjun and Long, Hu and Nelson, Art J. and Baker, Alex and Lee, Jonathan R. I. and Carraro, Carlo and Worsley, Marcus A. and Maboudian, Roya and Zettl, Alex},
abstractNote = {In this study, boron-doped and defect-engineered graphene aerogels are prepared using triphenyl boron as a boron precursor and subsequent heat treatments. The boron chemistry and concentration in the graphene lattice are found to be highly dependent on the temperature used to activate boron. At 1500 °C, boron is incorporated at 3.2 atom % through a combination of B–C, B–N, and B–O bonds. At 1750 °C, the boron concentration decreases to 0.7 atom % and is predominantly incorporated through B–N bonding. Higher temperatures result in complete expulsion of boron from the lattice, leaving behind defects that are found to be beneficial for NO2 gas detection. The gas sensing properties are explored to gain insight into the impact of boron chemistry on the sensing performance. A highly sensitive and selective conductometric NO2 sensor is fabricated on a low-power microheater. Defect-engineered graphene aerogels with no boron remaining have superior gas detection properties. At an optimum sensing temperature of 240 °C, the defect-engineered aerogel has a theoretical detection limit of 7 ppb for NO2 and response and recovery times of 100 and 300 s, respectively, with excellent selectivity over ammonia and hydrogen. Lastly, the superior gas sensing performance of defect-engineered graphene aerogels has remarkable implications for their performance in catalysis and energy storage applications.},
doi = {10.1021/acs.jpcc.8b05984},
journal = {Journal of Physical Chemistry. C},
issn = {1932-7447},
number = 35,
volume = 122,
place = {United States},
year = {2018},
month = {8}
}

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