Adsorption of NO<sub>2</sub> by hydrazine hydrate-reduced graphene oxide

Li Chuang; Cai Li; Li Wei-Wei; Xie Dan; Liu Bao-Jun; Xiang Lan; Yang Xiao-Kuo; Dong Dan-Na; Liu Jia-Hao; Li Cheng; Wei Bo

doi:10.7498/aps.68.20182242

Abstract

Reduced graphene oxide, as a candidate for gas detection due to its unique atomic structure, is arousing the wide interest of researchers. In this paper, hydrazine hydrate is used to reduce graphene oxide prepared by the modified Hummers method. A chemical resistance gas sensor is fabricated. The prepared reduced graphene oxide is used as a gas sensitive layer of Au planar interdigital electrode. The gas sensing characteristics such as responsivity, recovery and repeatability of NO₂ gas are studied. The results show that the graphene oxide reduced by hydrazine hydrate can detect the NO₂ gas at a concentration of 1−40 ppm under room temperature. It has good responsivity and repeatability. The recovery rate can reach more than 71%. However, the sensitivity is only 0.00201 ppm^–1, and there is much room for improvement. In addition, the response time and recovery time for NO₂ at 5 ppm concentration are 319 s and 776 s, respectively. The sensing mechanism of the hydrazine hydrate-reduced graphene oxide gas sensor can be attributed to charge transfer between the NO₂ molecule and the sensing material. The outstanding electrical properties of the reduced graphene oxide promote the electron transfer process. This allows the sensor to exhibit excellent gas sensing performance at room temperature. The reduced graphene oxide appears as a typical p-type semiconductor and the oxidizing gas NO₂ acts as an electron acceptor. Therefore, the adsorption of NO₂ gas leads to the enhancement of the hole density and conductivity of the reduced graphene oxide. Another reason is the presence of defects and oxygen-containing functional groups on graphene sheets. Some oxygen-containing groups remain on the graphene surface after an incomplete reduction reaction. Compared with pure graphene, the reduced graphene oxide has hydroxyl groups and epoxy groups remaining on the surface. These functional groups will functionalize the material and promote the adsorption of gases. At the same time, the reduction reaction will further produce vacancies and structural defects. This will provide more reaction sites and thus conduce to the material further adsorbing the gas. In summary, the experimental research in this paper is of significance for studying the mechanism and characteristics of the reduced graphene oxide by using hydrazine hydrate as a reducing agent, and it can provide reference and lay a foundation for the applications of future graphene sensors.

Keywords:

Authors and contacts

1.
Department of Basic Science, Air Force Engineering University, Xi’an 710051, China
2.
Tsinghua National Laboratory for Information Science and Technology, Institute of Microelectronics, Tsinghua University, Beijing 100084, China
3.
The First Aeronautic Institute, Air Force Engineering University, Xinyang 464000, China
4.
Department of Chemical Engineering, Tsinghua University, Beijing 100084, China

Corresponding author: Cai Li, qianglicai@163.com ; Xie Dan, xiedan@tsinghua.edu.cn ;

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 51672154, 51774191, 11405270), the National Key Research and Development Plan, China (Grant No. 2016YFA0200200), and the Natural Science for Basic Research Program of Shaanxi Province, China (Grant No. 2017JM6072).

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References

[1]	Novoselov K S, Geim A K, Morozov S V, Jiang D, Zhang Y, Dubonos S V, Grigorieva I V, Firsov A A 2004 Science 306 666 Google Scholar
[2]	孙建平, 缪应蒙, 曹相春 2013 物理学报 62 036301 Google Scholar Sun J P, Liao Y M, Cao X C 2013 Acta Phys. Sin. 62 036301 Google Scholar
[3]	魏晓林, 陈元平, 王如志, 钟建新 2013 物理学报 62 057101 Google Scholar Wei X L, Chen Y P, Wang R Z, Zhong J X 2013 Acta Phys. Sin. 62 057101 Google Scholar
[4]	Choudhuri I, Patra N, Mahata A, Ahuja R, Pathak B 2015 J. Phys. Chem. C 119 24827 Google Scholar
[5]	Gavgani J N, Hasani A, Nouri M, Mahyari M, Salehi A 2016 Sens. Actuator B: Chem. 229 239 Google Scholar
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[33]	Wan W B, Zhao Z B, Hu H, Zhou Q, Fan Y R, Qiu J S 2011 Carbon 8 2878
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[35]	Li D, Müller M B, Gilje S, Kaner R B, Wallace G G 2008 Nat. Nanotechnol. 3 101 Google Scholar
[36]	Cho B, Hahm M G, Choi M, Yoon J, Kim A R, Lee Y J, Park S G, Kwon J D, Kim C S, Song M 2015 Sci. Rep. 5 8052 Google Scholar
[37]	Jin C, Tang X, Tan X, Smith S C, Dai Y, Kou L 2019 J. Mater. Chem. A 7 1099 Google Scholar
[38]	Yang L, Cai Z, Hao L, Ran L, Xu X, Dai Y, Pan S, Jing B, Zou J 2018 Electrochim. Acta 283 448 Google Scholar
[39]	Ko K Y, Song J G, Kim Y, Choi T, Shin S, Lee C W, Lee K, Koo J, Lee H, Kim J 2016 ACS Nano 10 9287 Google Scholar
[40]	Lu G, Ocola L E, Chen J 2009 Appl. Phys. Lett. 94 083111 Google Scholar
[41]	Pearce R, Iakimov T, Andersson M, Hultman L, Spetz A L, Yakimova R 2011 Sens. Actuator B: Chem. 155 451 Google Scholar
[42]	Yavari F, Castillo E, Gullapalli H, Ajayan P M, Koratkar N 2012 Appl. Phys. Lett. 100 203120 Google Scholar
[43]	Qazi M, Nomani M W, Chandrashekhar M, Shields V B, Spencer M G, Koley G 2010 Appl. Phys. Express 3 075101 Google Scholar

Cited By

图 1 对1—40 ppm NO₂的实时响应曲线

Figure 1. Real-time response curves to 1−40 ppm NO₂.

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图 2 响应与浓度的关系

Figure 2. The plot of response vs. concentration.

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图 3 恢复率与浓度的关系图

Figure 3. The plot of recovery vs. concentration.

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图 4 传感器对10 ppm二氧化氮气体响应的重复性测试

Figure 4. Repeatability of the sensor after exposure to 10 ppm NO₂.

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图 5 传感器对5 ppm NO₂气体的响应和恢复时间

Figure 5. Response and recovery times of the sensor to 5 ppm NO₂.

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表 1 不同石墨烯基气体传感器检测NO₂性能对比

Table 1. Graphene based gas sensors for NO₂ detection.

敏感材料	浓度	响应度	响应时间	恢复时间	文献
rGO	5 ppm	$1.03\left( {{R_{\rm{a}}}/{R_{\rm{g}}}} \right)$	~5.3 min	~13 min	本文
低温热还原rGO	2 ppm	$1.56\left( {{G_{\rm{g}}} - {G_{\rm{a}}}} \right)/{G_{\rm{a}}}$	~30 min	> 30 min	[40]
机械剥离石墨烯	2.5 ppm	$0.005\left( {{R_{\rm{g}}}/{R_{\rm{a}}}} \right)$	~1 h	~2.5 h	[41]
CVD石墨烯	10 ppm	15% $\left( {\Delta R/{R_{\rm{a}}}} \right)$	~30 min	~45 min	[42]
外延生长的石墨烯	15 ppm	7.50%$ \left[ {\left( {{G_{\rm{g}}} - {G_{\rm{a}}}} \right)/{G_{\rm{a}}}} \right]$	~7.5 min	~17 min	[43]
注: a) 1 ppb = 10^－9; b) G_a, 在干燥空气中的电导; G_g, 在测试气体中的电导; c) R_a, 在干燥空气中的电阻; R_g, 在测试气体中的电阻; d) $\Delta R$, 由气体浓度变化导致的电阻的相对改变, $\Delta R={R_{\rm{a}}} - {R_{\rm{g}}}.$

DownLoad: CSV

[1]	Novoselov K S, Geim A K, Morozov S V, Jiang D, Zhang Y, Dubonos S V, Grigorieva I V, Firsov A A 2004 Science 306 666 Google Scholar
[2]	孙建平, 缪应蒙, 曹相春 2013 物理学报 62 036301 Google Scholar Sun J P, Liao Y M, Cao X C 2013 Acta Phys. Sin. 62 036301 Google Scholar
[3]	魏晓林, 陈元平, 王如志, 钟建新 2013 物理学报 62 057101 Google Scholar Wei X L, Chen Y P, Wang R Z, Zhong J X 2013 Acta Phys. Sin. 62 057101 Google Scholar
[4]	Choudhuri I, Patra N, Mahata A, Ahuja R, Pathak B 2015 J. Phys. Chem. C 119 24827 Google Scholar
[5]	Gavgani J N, Hasani A, Nouri M, Mahyari M, Salehi A 2016 Sens. Actuator B: Chem. 229 239 Google Scholar
[6]	Ye Z, Tai H, Xie T, Yuan Z, Liu C, Jiang Y 2016 Sens. Actuator B: Chem. 223 149 Google Scholar
[7]	Matsuba K, Wang C, Saruwatari K, Uesusuki Y, Akatsuka K, Osada M, Ebina Y, Ma R, Sasaki T 2017 Sci. Adv. 3 e1700414 Google Scholar
[8]	Pour M M, Lashkov A, Radocea A, Liu X, Sun T, Lipatov A, Korlacki R A, Shekhirev M, Aluru N R, Lyding J W 2017 Nat. Commun. 8 820 Google Scholar
[9]	Singh E, Meyyappan M, Nalwa H S 2017 ACS Appl. Mater. Interfaces 9 34544 Google Scholar
[10]	Liu J H, Yang X K, Zhang M L, Wei B, Li C, Dong D N, Li C 2019 IEEE Electron Device Lett. 40 220 Google Scholar
[11]	Liu J H, Yang X K, Cui H Q, Wang S, Wei B, Li C, Li C, Dong D N 2019 J. Magn. Magn. Mater. 474 161 Google Scholar
[12]	Zhang T, Ma Y D, Huang B B, Dai Y 2019 ACS Appl. Mater.Interfaces 11 6104
[13]	Schedin F, Geim A, Morozov S, Hill E, Blake P, Katsnelson M, Novoselov K 2007 Nat. Mater. 6 652 Google Scholar
[14]	Venugopal G, Krishnamoorthy K, Mohan R, Kim S J 2012 Mater. Chem. Phys. 132 29 Google Scholar
[15]	Yasaei P, Kumar B, Hantehzadeh R, Kayyalha M, Baskin A, Repnin N, Wang C, Klie R F, Chen Y P, Král P 2014 Nat. Commun. 5 4911 Google Scholar
[16]	Chung M G, Kim D H, Lee H M, Kim T, Choi J H, Kyun Seo D, Yoo J B, Hong S H, Kang T J, Kim Y H 2012 Sens. Actuator B: Chem. 166 172
[17]	Yavari F, Koratkar N 2012 J. Phys. Chem. Lett. 3 1746 Google Scholar
[18]	Novoselov K, Jiang D, Schedin F, Booth T, Khotkevich V, Morozov S, Geim A 2005 Proc. Natl. Acad. Sci. U. S. A. 102 10451 Google Scholar
[19]	Park S, Ruoff R S 2009 Nat. Nanotechnol. 4 217 Google Scholar
[20]	Berger C, Song Z, Li X, Wu X, Brown N, Naud C, Mayou D, Li T, Hass J, Marchenkov A N 2006 Science 312 1191 Google Scholar
[21]	韩林芷, 赵占霞, 马忠权 2014 物理学报 63 248103 Google Scholar Han L Z, Zhao Z X, Ma Z Q 2014 Acta Phys. Sin. 63 248103 Google Scholar
[22]	Dua V, Surwade S P, Ammu S, Agnihotra S R, Jain S, Roberts K E, Park S, Ruoff R S, Manohar S K 2010 Angew. Chem. 122 2200 Google Scholar
[23]	Li W, Li X, Cai L, Sun Y, Sun M, Xie D 2018 J. Nanosci. Nanotechnol. 18 7927 Google Scholar
[24]	Li W, Teng C, Sun Y, Cai L, Xu J L, Sun M, Li X, Yang X, Xiang L, Xie D 2018 ACS Appl. Mater. Interfaces 10 34485 Google Scholar
[25]	Hu N, Wang Y, Chai J, Gao R, Yang Z, Kong E S W, Zhang Y 2012 Sens. Actuator B: Chem. 163 107 Google Scholar
[26]	Brodie B 1860 Ann. Chim. Phys. 59 e472
[27]	Staudenmaier L 1898 Ber. Dtsch. Chem. Ges. 31 1481 Google Scholar
[28]	Hummers Jr W S, Offeman R E 1958 J. Am. Chem. Soc. 80 1339 Google Scholar
[29]	洪菲, 周立群, 黄莹, 宋荷娟, 王婷, 罗辛茹, 伍珍 2012 化学与生物工程 29 31 Google Scholar Hong F, Zhou L Q, Huang Y, Song H J, Wang T, Luo X R, Wu Z 2012 Chem. Bioeng. 29 31 Google Scholar
[30]	Compton O C, Nguyen S T 2010 Small 6 711 Google Scholar
[31]	Lipatov A, Varezhnikov A, Wilson P, Sysoev V, Kolmakov A, Sinitskii A 2013 Nanoscale 5 5426 Google Scholar
[32]	Ren P G, Yan D X, Ji X, Chen T, Li Z M 2010 Nanotechnology 22 055705
[33]	Wan W B, Zhao Z B, Hu H, Zhou Q, Fan Y R, Qiu J S 2011 Carbon 8 2878
[34]	Alizadeh T, Soltani L H 2016 Sens. Actuator B: Chem. 234 361 Google Scholar
[35]	Li D, Müller M B, Gilje S, Kaner R B, Wallace G G 2008 Nat. Nanotechnol. 3 101 Google Scholar
[36]	Cho B, Hahm M G, Choi M, Yoon J, Kim A R, Lee Y J, Park S G, Kwon J D, Kim C S, Song M 2015 Sci. Rep. 5 8052 Google Scholar
[37]	Jin C, Tang X, Tan X, Smith S C, Dai Y, Kou L 2019 J. Mater. Chem. A 7 1099 Google Scholar
[38]	Yang L, Cai Z, Hao L, Ran L, Xu X, Dai Y, Pan S, Jing B, Zou J 2018 Electrochim. Acta 283 448 Google Scholar
[39]	Ko K Y, Song J G, Kim Y, Choi T, Shin S, Lee C W, Lee K, Koo J, Lee H, Kim J 2016 ACS Nano 10 9287 Google Scholar
[40]	Lu G, Ocola L E, Chen J 2009 Appl. Phys. Lett. 94 083111 Google Scholar
[41]	Pearce R, Iakimov T, Andersson M, Hultman L, Spetz A L, Yakimova R 2011 Sens. Actuator B: Chem. 155 451 Google Scholar
[42]	Yavari F, Castillo E, Gullapalli H, Ajayan P M, Koratkar N 2012 Appl. Phys. Lett. 100 203120 Google Scholar
[43]	Qazi M, Nomani M W, Chandrashekhar M, Shields V B, Spencer M G, Koley G 2010 Appl. Phys. Express 3 075101 Google Scholar

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Adsorption of NO₂ by hydrazine hydrate-reduced graphene oxide

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Corresponding author: Cai Li, qianglicai@163.com ; Xie Dan, xiedan@tsinghua.edu.cn ;

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Adsorption of NO2 by hydrazine hydrate-reduced graphene oxide

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Corresponding author: Cai Li, qianglicai@163.com ; Xie Dan, xiedan@tsinghua.edu.cn ;

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Adsorption of NO₂ by hydrazine hydrate-reduced graphene oxide