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

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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 NO ₂gas are studied. The results show that the graphene oxide reduced by hydrazine hydrate can detect the NO ₂gas 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 NO ₂at 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 NO ₂molecule 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 NO ₂acts as an electron acceptor. Therefore, the adsorption of NO ₂gas 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.

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Authors and contacts

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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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, $\Delta R={R_{\rm{a}}} - {R_{\rm{g}}}.$

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Vol. 68, Issue 11 - 2019-06-05

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