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Application of boron doped diamond electrodes to electrochemical gas sensors (本文)

Triana, Yunita 慶應義塾大学

2022.03.23

概要

1. Development of Gas Sensor
　A device, module or machine that detects events or changes and relays the information to other electronics is called sensor. A sensor reads physical phenomena and converts into a measurable digital signal, which can then be displayed, read, or processed further[1]. There is a range of sources, including light, temperature, movements, and pressure etc. Sensors are embedded in everything we come into contact with in our everyday lives. Subsequent subsections show some of the critical sensors used in our daily life are level, temperature, proximity, pressure, chemical, infra-red, and many other sensors[2].
　Among them, there is gas sensor which similar to chemical sensors, except that they monitor air quality and detect various gases. Gas sensor provides a vital way to monitor gas concentration and gives safety information. Gas sensor technologies have improved the everyday life of human beings through their applications in almost all fields[3]. They are used for air quality monitoring, toxic or combustible gas detection, hazardous gas monitoring and medical application.

1.1 Application of Gas Sensor to Improve Environmental Monitoring
　Biotic and abiotic factors are the composition of our atmosphere. In fact, abiotic factor is quite essential for life on the planet. The abiotic factors are such as gases, moisture, humidity, and temperature. The hazardous gases should not increase beyond a critical level shoud be maintained to keep oxygen in an adequate level. Atmospheric pollution can create a high level of health and life loss within the short span of time. Environmental pollution, urbanization, use of automobiles, fuel burning, and industrial wastes are the main source for the increasing of hazardous gas concentration in the air. Six pollutants have been identified as the main source of air pollution. The particulate matter consists of lead and gases like oxides of carbon and oxides of nitrogen[4]. There are several diseases which result from pollution and threaten human health. Seven million deaths take place due to pollution[5]. This is because respiratory organ diseases are mainly ascribed to poor air quality. The major diseases resulting from air pollution are stroke, ischemic heart diseases, lower respiratory infections and lung cancer[6]. For the environmental effect may cause acid rain. Air quality control is the main aspect in the field of environmental monitoring. Gas sensing devices are used to protect plants and personnel from inflammable and toxic gases. They can cause hazard to human and their belongings due to its toxic nature such as hydrogen sulfide and nitrogen dioxide.

a. Hydrogen Sulfide (H2S)
　Today the rapid expansion of industries gives contribution as a serious problem to the environment and human health safety. Especially, waste gas such as hydrogen sulfide (H2S) attracts much interest due to the dangerous characteristics. Hydrogen sulfide (H2S) is known to be a corrosive, poisonous, and gaseous compound. Hydrogen sulfide is basically a gas state chemical that also found in the dissolved form[7].
　It is widely found in several water pollutant resources such as sewage treatment plants, electric power waste, coal processing plants, sulfur production processes, commercial hydrogen sulfide production, and other resources[8]. At concentrations greater than 500 parts per million, inhalation of hydrogen sulfide can lead to immediate collapse and unconsciousness. Unconsciousness and death have occurred in situations of prolonged exposure to hydrogen sulfide at concentrations of 50 ppm. The estimated global release of hydrogen sulfide from saline marshes into the atmosphere is 8.3 × 105 ton per year. The Occupational Safety and Health Administration (OSHA) define Permissible Exposure Limits (PELs) to H2S gas: 20 ppm for ceiling industry, 50 ppm (up to 10 minutes if no other exposure during shift) for general industry, 10 ppm for construction and shipyard[9].
　The strict implementation of industrial gas waste regulations is required the highly reliable and accurate gas sensors devices. High-performance liquid chromatography[10,11] and gas chromatography[12,13] are used to detect H2S. There are some weaknesses of the methods such as long incubation times due to the process in the column and these instruments are expensive.
　Recently, electrochemical sensor has been growing interest to detect H2S due to the sensitivity, selectivity, real-time detection and low detection limit[14]. By electrochemical method, there are potentiometric[15] and amperometric[16] techniques to detect H2S. However, the main problem is durability of the working electrode (eg. glassy carbon and platinum electrodes) due to sulfur (S0) layer as an oxidation product via 2 electrons can degrade the analytical performance. Therefore, a redox mediator is needed to prevent sulfur deposited on the surface of working electrodes such as room temperature ionic liquids (RTILs), hydroxyl- functionalized ionic liquids, phenol, phenylenediamine, and eugenol. However, organic solutions are expensive and harmful for the environment. Therefore, researches on high sensitivity, selectivity and high durability material for electrochemical H2S sensor have become a hot issue.

b. Nitrogen Dioxide (NO2)
　Nowadays, road traffic and automobiles activities are sources of pollution released into the atmosphere since the beginning of the twentieth century. Our urban and rural areas are currently subject to pollution peaks such as ozone, nitrogen dioxide, and carbon monoxide. One of six criteria air pollutants designated by the United States Environmental Protection Agency (USEPA) is nitrogen dioxide (NO2). It is formed in the atmosphere from nitrogen monoxide (NO), which is mainly released during the combustion of fossil fuels[17].
　NO2 is a reddish-brown flammable gas with a characteristic odor. At low concentrations of NO2, medical consequences include difficulty in breathing, chest pain and chronic respiratory problems. This gas is extremely toxic at high concentrations above 360 ppb. From an environmental point of view, nitrogen dioxide is converted into nitric acid in the presence of water molecules and contributes to form as acid rain. Therefore, the monitoring of air quality and gaseous pollutants is the goal of several researchers around the world. The most difficult pollutants to control is NO2[18].
　Maximum 30-minute or 1-hour average and maximum 24-hour average outdoor nitrogen dioxide concentrations of up to 0.5 ppm and 0.21 ppm, respectively. In Japan, the short-term exposure limit for NO2 gas is 500 ppb, and the environmental standard value is 40 to 60 ppb[19].
　It leads to urgent needs for sensitive, selective, and responsive NO2 sensors. High performance liquid chromatography (HPLC)[20] and gas chromatography[21] are used for NO2 detection. However, it caused cost ineffectiveness, insufficient sensitivity for detection, and time consuming sample incubation. Chemiluminescence[22,23] combined with HPLC and gas chromatography is also widely used but the response time is limited.
　In the last decades, electrochemical sensors have presented a promising way forward for the detection of NO2 gas, since they offer real time measurement, simplicity with a low limit of detection (LOD) and good selectivity[24,25]. By electrochemical technique, metal electrodes such as Pt (platinum) and gold (Au) are modified with nafion[26], yttria-stabilized zirconia (YSZ)[27], and teflon[25] to increase the performance. However, surface modification is difficult and many optimizations to prepare. In other hand, carbon based electrodes such as glassy carbon[28], graphite[29], and carbon nanotubes[30] have disadvantages of limited sensitivity, poor precision and lack of durability. Further investigation of good performance material for electrochemical NO2 sensor attracts much attention recently.

1.2 Application of Gas Sensor in Biomedical Diagnostic
　The intake of oxygen (O2) and the release of carbon dioxide (CO2) are the most important activities for human health. Respiration provides a constant flow of O2 molecules to our brain, organs and tissues while providing a way to remove the waste CO2 molecules that are created in the cells[31]. Without respiration, our bodies will shut down within seconds. Therefore, regardless of the procedure, wound, disease or illness, one of the first priorities of a physician is to insure continuous respiration. For this reason, gas sensor is critical instruments in medical applications. In order to measure respiration, physicians and health care workers use several O2 and CO2 gas sensors. These gases are measured in 2 areas: the breath and the blood.
　Blood O2 monitoring can play as an essential role of disease biomarker such as hypoxemia, COVID-19 infection, heart failure, cancers and other diseases related to O2 concentration in human body[32]. Oxygen is measured 3 ways, as partial pressure of oxygen (PaO2), as oxygen saturation (O2 Sat) and for oxygen content (O2CT) in the blood. Normal O2 concentration in human body is around 40 – 100 mmHg[33].
　Optical detection is commonly used for O2 concentration in daily life for example oximeter[34] and diffuse optical tomography[35]. These instruments show O2 concentration in saturated O2 in percentage (% SpO2). However, oximeter has lack of sensitivity due to its limitations of the arterial pulse strength, body movement, lipids and bilirubin, color of the skin, and other physical factors[36] from the patients. So, it cannot show the real condition of the patients. Resonance[37] methods also can detect O2 but expensive and difficult to calibrate.
　 Electrochemical sensors have been attracted much attention due the real-time measurement and sensitivity. By electrochemical methods, there are polarographic[38] and conductometry[39]. However, the techniques are difficult to be applied due to ineffectiveness and lack of accuracy. Therefore, developing of design material for electrochemical O2 gas sensor is challenging and increasing in biomedical application.

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