Sensitive Detection of H₂S Using Gold Nanoparticle Decorated Single-Walled Carbon Nanotubes

Abstract

Herein, we demonstrate that highly sensitive conductometric gas nanosensors for H 2 S can be synthesized by electrodepositing gold nanoparticles on single-walled carbon nanotube (SWNT) networks. Adjusting the electrodeposition conditions allowed for tuning of the size and number of gold nanoparticles deposited. The best H 2 S sensing performance was obtained with discrete gold nanodeposits rather than continuous nanowires. The gas nanosensors could sense H 2 S in air at room temperature with a 3 ppb limit of detection. The sensors were reversible, and increasing the bias voltage reduced the sensor recovery time, probably by local Joule heating. The sensing mechanism is believed to be based on the modulation of the conduction path across the nanotubes emanating from the modulation of electron exchange between the gold and carbon nanotube defect sites when exposed to H 2 S.Sensitive detection and monitoring of gaseous reduced sulfur compounds such as hydrogen sulfide (H 2 S) is important because of toxicity, corrosion, and odor nuisance concerns. H 2 S is generated in large amounts in coal and natural gas processing, petroleum industries, biogas production, and sewage treatment plants. 1 The odor threshold of H 2 S is around 3 ppb in air which is well below any known toxic effects, while the threshold limit value (TLV) was set to 10 ppm; at concentrations exceeding 150 ppm, H 2 S is extremely toxic and hazardous. 2 Hence, it is important to develop sensors that can monitor H 2 S in real time and can detect concentrations from as low as a few parts per billion to the several hundred parts per million in air. A number of H 2 S detection techniques have been developed in the past few decades, with electrochemical detection as the most widely utilized method in compact and portable H 2 S gas monitors. 3,4 These devices often rely on solid state sensors made of semiconducting metal oxides such as tungsten oxide and tin oxide or metals such as gold. H 2 S detection is usually based on determining conductivity changes of thin films upon exposure to H 2 S gas. 4,5 While there are a number of successful devices available commercially, drawbacks of existing H 2 S monitors include high power consumption (e.g., in metal oxide sensors that require high operating temperatures); low sensitivity, making them unsuitable for environmental monitoring; short lifetime (usually less than one year); short linear dynamic range; interference from other gases (e.g., NH 3 , NO x , etc); and high cost. 6 Recently, chemical sensors based on one-dimensional nanostructures such as bare or functionalized semiconducting singlewalled carbon nanotubes (SWNTs), 6,7 metal oxides, and conducting polymer nanowires 8 have attracted a great deal of attention because of their superior sensing performance. In particular, these sensors offer promising perspectives for real-time monitoring of gases or vapors with high sensitivity and low-power consumption and potentially at a low cost. 6 Their small size will also allow future integration with low-pow...

Investigation of interaction hydrogen sulfide with (5,0) and (5,5) single-wall carbon nanotubes by density functional theory method

“…Despite low and positive values of the Gibbs free energies of H 2 S adsorption on the external wall of (5,0) and (5,5) nanotubes, the adsorption energies are negative. It confirms no interaction between H 2 S gas and nanotube [15]. For obtaining more information, the optical properties under rotation of H 2 S molecule and natural bond orbital (NBO) analysis of H 2 S fluid-nanotube systems are studied.…”

“…Wei et al [14] demonstrated that multi-walled carbon nanotubes have extraordinarily highcurrent carrying capacity, sustaining current densities greater than 109 A/cm 2 . These novel electrical properties have generated substantial interest in utilizing carbon nanotubes in nanoelectronics [15].…”

Computational investigation of single-wall carbon nanotube functionalized with palladium nanoclusters as hydrogen sulfide gas sensor

“…It is shown that functionalization with metal 1 3 nanoparticles, play a crucial role in producing gas sensors with high sensitivity [19][20][21][22][23][24][25][26][27][28]. Different experimental and theoretical studies have been performed for functionalization of carbon nanotubes and graphene, with metal nanoparticles, as the gas sensor [29][30][31][32][33][34][35]. For example, Yoosefian theoretically showed that intrinsic single wall carbon nanotube (SWCNT), cannot adsorb NH 3 gas molecules suitably, but SWCNT functionalized with palladium (Pd), facilitate adsorption of NH 3 gas, leading to the high selectivity and fast response of the device [33].…”

Adsorbing H2S onto a single graphene sheet: A possible gas sensor

“…43 Several industrial processes generate a huge amount of H 2 S, including natural gas processing, petroleum refining, coal gasification, biogas fermentation, and the activity of petrochemical plants, Kraft mills, and coke ovens. 43 During the process of the biogas fermentation, a huge amount of H 2 S is produced [44][45][46] because the biogas must be purified from H 2 S. Inhaled H 2 S is very harmful and can cause death depending on the concentration and the exposure duration. From the above, it is clear that the adsorption of H 2 S on graphene is a very important problem.…”