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Review

Development of a Chemical Sensor Device for Monitoring Hazardous Gases Generated in the Semiconductor Manufacturing Process

by
My Thi Ngoc Nguyen
and
Jun Seop Lee
*
Department of Materials Science and Engineering, Gachon University, 1342 Seongnam-daero, Sujeong-gu, Seongnam-si 13120, Republic of Korea
*
Author to whom correspondence should be addressed.
Chemosensors 2024, 12(11), 233; https://doi.org/10.3390/chemosensors12110233
Submission received: 28 September 2024 / Revised: 7 November 2024 / Accepted: 8 November 2024 / Published: 9 November 2024
(This article belongs to the Special Issue Gas Sensors for Monitoring Environmental Changes, 2nd Edition)
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Abstract

:
The semiconductor industry plays a crucial role in various fields but also contributes to environmental degradation. Throughout the semiconductor chip manufacturing process, hazardous gases are released at each stage, despite stringent treatment procedures. These gases can be categorized into four groups: acidic and alkaline gases, volatile organic compounds, flammable and corrosive gases, and greenhouse gases. To meet stricter emission standards, further advancements in gas sensor technology are essential. This review examines recent research on monitoring these gases, highlighting the capabilities and limitations of existing sensor technologies. Additionally, the paper discusses current challenges in gas sensing research and proposes future directions for improving technologies.

1. Introduction

The Fourth Industrial Revolution is underway, with the semiconductor industry playing a critical role due to its significant influence on manufacturing capacities across various sectors such as computing, healthcare, transportation, military systems, and clean energy [1,2]. Unfortunately, this industry uses large amounts of water and energy, and emits greenhouse gases and toxic chemicals, negatively affecting human and environmental health [3,4,5]. Alongside waste and water management, air pollution control is a pressing issue that has drawn substantial interest from stakeholders (e.g., suppliers and customers), especially as emission regulations tighten in pursuit of Net Zero objectives. Numerous customers of semiconductor companies are urging their suppliers to intensify efforts to decrease greenhouse gas (GHG) emissions and achieve net-zero carbon emissions across the supply chain [6]. For example, Amazon plans to achieve net-zero emissions by 2040 and has invested $2 billion in funds to support emission reductions, while its chip supplier, Intel, has committed to net-zero emissions by 2040 for Scope 1 and 2 emissions.
In a semiconductor factory, hazardous gases are emitted from various fabrication processes (Figure 1). Completing one circuit layer involves six fundamental steps: cleaning, deposition, photolithography, etching, ion implantation, and stripping [7,8,9]. These procedures are then repeated to create multiple circuit layers. The primary sources of exhaust gas are the raw chemical materials used, which exhibit toxic, corrosive, or flammable properties. Exhaust gases must be properly classified before grouping and connecting to specific local scrubbers. They are then further processed in various central terminal facilities before being released into the atmosphere [10,11,12,13]. Despite stringent treatment processes, several pollutants remain, categorized into four types: volatile organic compounds (VOC); acid gases (e.g., H2SO4, HF, HCl, HNO3, and H3PO4); alkaline gases (such as NH3); and flammable and corrosive gases (such as AsH3, SiH4, and SiCl4), as well as greenhouse gases (such as CF4, C4F6, and SF6).
Exhausted gases must be continuously monitored when exposed to the ambient environment to safeguard employee health and safety, protect valuable equipment, and comply with regulations. Numerous attempts have been made using various analytical methods to detect hazardous gases, including mass spectrometry, spectrophotometry, high-performance liquid chromatography, and gas chromatography [14,15,16,17,18]. Although these techniques are highly precise, using them for in situ detection presents significant challenges. Since the last century, advancements in gas monitoring, both scientific and commercial, have utilized diverse sensing principles, including physical (e.g., photo-ionization detection, photoacoustic spectroscopy, photoelectric photometry) and chemical methods (e.g., chemosensors, colorimetric sensors, electrochemical sensors) [19,20,21,22,23,24,25,26] (Figure 2). However, each method has distinct advantages and limitations depending on the measurement conditions and specific gases targeted (Table 1) [27,28,29,30]. These methods continue to be applied and improved upon. Many researchers are focused on developing advanced materials or combining these methods to leverage the unique strengths of each. This approach has resulted in the development of advanced sensors capable of real-time monitoring of toxic gases and detecting extremely low concentrations. To align with advancements in gas processing technology and to meet increasingly stringent emission standards, gas sensors must improve their detection limits and be integrated into networks featuring low power consumption, reduced costs, long-term stability, and strong resistance to environmental factors such as humidity, temperature, and pressure.
This review identifies the gases emitted at each stage of the semiconductor manufacturing process and classifies them into four categories of pollutants. It also covers recent research efforts aimed at controlling these gas concentrations, highlighting the potential and limitations of their sensing performance. Furthermore, the manuscript discusses current challenges in gas sensing research and explores future directions for enhancements.

2. Detection Method for Exhaust Gases

2.1. Acidic and Alkaline Gases

Cleaning and etching are the stages where acidic and alkaline gases are predominantly produced and emitted compared to other processes. Specifically, the immersion-type RCA (Radio Corporation of America) cleaning method uses hot liquid chemicals such as NH4OH, H2O2, and HCl [31,32]. Consequently, these processes release a significant volume of highly concentrated gaseous chemicals from cleaning systems. Therefore, these gases must be treated with scrubbers before being released into the atmosphere.
Acidic emissions exhibit many corrosive and toxic characteristics, not only causing respiratory and digestive diseases in humans but also severe environmental impacts such as acid rain, ecosystem alkalization, and climate change [33,34,35]. With increasing environmental impacts, more stringent emissions standards are being enforced. The concentration of emissions must remain below 0.5 ppm or achieve a reduction rate of 96% for acid gas emissions from semiconductor factories [36].
Moreover, ammonia (NH3) represents the primary alkaline emission and is widely used in silicon nitride deposition. According to International Financial Corporation (IFC) emission guidelines, NH3 emissions must remain below 30 mg/Nm3 (approximately 43 ppm) [37]. Additionally, the National Institute for Occupational Safety and Health (NIOSH) sets the threshold limit value for NH3 at 25 ppm, which poses a risk to human respiratory health [38]. Therefore, developing an advanced sensor to detect target gases at low concentrations is crucial for complying with stringent gas emission regulations. This section discusses studies with significant potential applications for detecting HCl and NH3 emissions.
Both alkaline and acidic gases can be detected using an electrochemical-based gas sensor, which measures gases through redox reactions in real time, generating electrical signals. In electrochemical cells, gases such as NH3 (alkaline) and HCl, SO2 (acidic) undergo oxidation or reduction on specific electrode materials. These reactions produce electrons that generate an electric current proportional to the gas concentration [39]. Additionally, optical-based sensors using various sensing layer materials, such as metal oxides and polymers, also can detect alkaline or acidic gases [40,41,42].
For example, Qiao et al. proposed a study to improve the HCl gas sensitivity of light-induced thermoelastic spectroscopy (LITES) sensors by integrating a low-frequency quartz tuning fork (QTF) and a fiber-coupled multi-pass cell into the system (Figure 3a) [43]. Since LITES is a non-contact technique, the QTF does not require direct contact with the gases being detected, which enhances its lifespan and makes it suitable for corrosive gases such as HCl. LITES functions by projecting a laser onto the target gas sample and the surface of the QTF [44]. The gas partially absorbs the laser beam, and the remaining energy is converted into thermal energy, inducing thermal expansion and mechanical vibrations in the QTF. The resonance frequency of commercially available QTFs is typically around 32 kHz. Higher frequencies lead to shorter energy accumulation times in the system, decreasing the modulation period and diminishing the piezoelectric signal. In pursuit of more sensitive detection, Qiao et al. used low-frequency QTFs as detectors by altering the tuning fork’s physical dimensions; longer and thinner prongs generally result in lower resonance frequencies. Their findings demonstrate that employing a low-frequency QTF (2.89 kHz) notably extends the energy accumulation time, effectively doubling the signal output compared to standard commercial QTFs. The specialized low-frequency QTF achieved a minimum detection limit of 148 ppb, representing a substantial enhancement in sensitivity compared to previous approaches. Additionally, the incorporation of a fiber-coupled multi-pass cell with an optical length of 40 m increases the gas absorption path length and simplifies optical alignment, thereby improving the overall performance of the sensor. Despite the high sensitivity, the selectivity of the device has not been evaluated. Moreover, a single sensor is often insufficient to monitor the myriad of toxic gases present in semiconductor manufacturing environments. Therefore, developing gas sensors capable of detecting multiple gases with distinct selectivity, minimal interferences, long-term stability, and cost-effectiveness remains crucial.
Recently, Li et al. proposed a fluorescent nanofilm based on imine bonds that serves as a multifunctional material, effectively detecting and removing HCl and NH3 (Figure 3b) [45]. The dynamic imine bonds at the interface interact with exposed HCl gas through hydrogen bonding, causing the film to shift color from green to red under UV light. Upon exposure to NH3, it reacts with the pre-absorbed HCl, reverting the film’s color back to green. A homemade gas circuit system for the quartz crystal microbalance sensor is utilized to assess the sensing performance. When the analyte is captured by the nanofilm, it induces a frequency variation signal that corresponds to the mass of the adsorbed gas. The results display rapid response times of less than 1 s for HCl and under 0.5 s for NH3. The nanofilms show high sensitivity to both HCl and NH3, achieving detection limits of less than 150 ppb for HCl and less than 1.5 ppm for NH3. Additionally, the sensor displays high selectivity for NH3 and HCl, even when tested alongside a variety of saturated vapors including benzene, alcohols, alkanes, amines, other common VOCs, and water. Since these chemicals minimally impact the reactivity of the imine group, they do not significantly influence the response signal. Moreover, the color change feature of the nanofilms upon gas adsorption supports their application in practical scenarios, thus enhancing user-friendliness in real-world environments. However, this selective approach facilitates the creation of color-variable flexible films but does not support concurrent detection of both analytes.
To address this limitation, Kondratev et al. explored sensors based on silicon nanowires (Si NWs) using electrochemical impedance spectroscopy (EIS) for simultaneous detection of NH3 and HCl (Figure 3c) [46]. A pool containing NH3 and HCl solutions was placed beneath the sensors and allowed to evaporate naturally under ambient conditions, enabling the sensors to detect gas presence. The setup was situated in a Faraday cage to ensure precise measurements. The sensing mechanism is based on the interaction of analyte molecules with the Si NWs surface, altering their electronic properties. These sensors exhibit significant changes in resistance and impedance when exposed to NH3 and HCl. The protonation of surface hydroxyl groups by NH3 molecules forms NH4+ ions, reducing resistance through increased electron concentration in the Si NWs. Conversely, exposure to HCl results in Cl- ions occupying adsorption sites on the Si NWs surface, sequestering electrons and reducing carrier density. The electrodes are assembled, and the Si NWs synthesized as in previous work (which detected only one analyte), but simultaneous sensing is achieved by distinguishing between the two analytes using characteristic frequency (F) and resistance (R). Nyquist plots from EIS measurements are employed to simultaneously determine the R and F parameters. Further insights into the selectivity of the fabricated sensors were gained by investigating the sensor responses to acetone and isopropanol, and comparing these with data for NH3 and HCl. Due to differences in the electronegativity of the analyte species, the sensors show opposite responses upon exposure to NH3 and HCl. Furthermore, the sensor showcased a minimum detection limit of 4 μmol·L−1 (approximately 0.08 ppm) for both HCl and NH3. This technique introduces a novel approach for detecting multiple analytes concurrently with a single sensor. Recently reported gas sensors for detecting acidic and alkaline gases are documented in Table 2.

2.2. Volatile Organic Compounds (VOC)

VOC emissions primarily arise from wafer cleaning, photolithography, and photoresist stripping processes [52,53,54]. Solvents such as methanol, isopropyl alcohol (IPA), acetone, propylene glycol, monomethyl ether acetate, and ethyl acetate are major sources of these emissions [55,56,57]. Exposure to VOC can cause eye, nose, and throat irritation, breathing difficulties, nausea, and damage to the central nervous system and other organs, with potential cancer risks [58]. Under sunlight, VOC react with nitrogen oxides (NOx) and carbon monoxide (CO) to form tropospheric ozone (O3), also known as ground-level smog [59,60]. In response to environmental concerns about VOC emissions, significant nations (EU, USA, China, South Korea, etc.) have established ambitious Net-Zero goals for 2050. Taiwan Semiconductor Manufacturing Company Limited, the largest semiconductor manufacturer globally, has implemented stricter regulations to lower exhaust VOC concentrations to below 14 ppm [36]. Methanol is particularly crucial among the solvents used in various semiconductor manufacturing processes such as furnace cleaning, wet sawing of ingots, silicon wafer washing, and quality control [61,62]. The United States Environmental Protection Agency (EPA) identified methanol as one of five chemicals accounting for over 90% of total hazardous air pollutants from semiconductor manufacturing, along with HCl, hydrogen fluoride (HF), glycol ethers, and xylene [63]. This section examines the detection of low methanol gas concentrations, which has significant implications for emission control systems in semiconductor manufacturing.
PID is a widely used technology for VOC detection. In PID, VOC molecules are ionized by UV light, with most VOC possessing ionization energies within the typical UV range of approximately 10.6 eV, enabling PID to ionize and detect VOC efficiently [64]. Furthermore, metal oxide semiconductor gas sensors are highly effective in directly monitoring VOC concentrations down to sub-ppb levels [65,66]. Owing to their extensive detection range, these sensors are extensively employed in both consumer devices and industrial applications for indoor air quality monitoring.
Commercial sensors often require high operating temperatures, whereas VOC have low flash points that limit their detection capabilities. To address this issue, Sáaedi et al. combined polyaniline (PAni) with zinc oxide (ZnO) to create a nanocomposite that significantly enhances the sensitivity of methanol detection (Figure 4a) [67]. ZnO/PAni nanocomposites were deposited on SiO2/Si substrates, and gold electrodes were introduced to these films to collect resistance signals. The sensor was then placed in a test chamber with controlled temperature and humidity. The study underscored the role of magnetic fields in enhancing the structural and chemical properties of PAni composites, thus improving their gas sensing performance. By increasing the magnetic field intensity to 0.5 T, the protonation level of PAni increased to 36.32%, over three times the 11.59% achieved at 0.0 T. This enhanced protonation increases the interaction between PAni and gas molecules, thus advancing gas sensing performance and enabling the nanocomposite to operate at just 60 °C instead of 150 °C for pristine ZnO thin films. To assess selectivity, the device was exposed to 100 ppm of methanol as well as other gases including ethanol, acetone, liquefied petroleum gas, and CO2. The response signals for methanol exceeded those for other gases, even across varying operating temperatures (ranging from 60 °C to 140 °C). Compared to other gas sensing technologies, these sensors are more viable for various applications due to their low manufacturing costs and simple design.
In another study, Xuan et al. introduced an in situ pyrolytic coating technique to produce core-shell CsPbBr3@ZnO nanocrystals by coating perovskite structures with metal oxides (Figure 4b) [68]. This design leverages the stability of the ZnO shell and the sensitivity of perovskites to polar molecules, facilitating electron transfer from the conduction band minimum of CsPbBr3 to that of ZnO. This transfer enhances the surface activity of ZnO and improves its gas detection capabilities. Additionally, the strong adsorption properties of the core-shell structure enhance its gas response performance. Consequently, the sensor exhibits a rapid response and recovery time (approximately 3.27 s for the response and 3.11 s for recovery when detecting 10 ppm methanol at room temperature). The sensor’s detection threshold for methanol is 1 ppm, enabling accurate identification of low concentrations in mixed environments. The selectivity of the sensor was tested using 10 ppm of various gases (methanol, butyl acetate, n-heptane, toluene, isopropanol, heptanal, and ethanol). The results demonstrated that the sensitivity of the CsPbBr3@ZnO sensor to methanol was approximately three times higher than to other gases. The sensor utilizes a molecular fingerprint sensing mechanism, where the crystal structure, density of states, and band structure of the sensing material are altered by different gases, resulting in distinct response/recovery properties and thus enabling differentiation of methanol from other gases. It should be noted that the configuration of the sensing material plays a crucial role in the performance of sensor systems.
Mishra et al. proposed an alternative configuration of the sensing material wherein a 2D semiconducting Cu(I) coordination polymer (CP1) serves as a chemiresistive sensor for methanol (Figure 4c) [69]. The CP1 sensing device was fabricated by simply drop-casting a CP1/ethanol solution onto a commercial interdigitated electrode. Its sensing performance was observed using a dynamic flow-through gas sensing setup at room temperature. The 2D configuration significantly enhances the interaction between the analyte and the active sites of the polymer. The study indicates that the electron-rich nature of the Cu(I) coordination polymer facilitates enhanced charge transfer interactions with the analyte, vital for effective sensing. Upon exposure to methanol, the Fermi level of CP1 slightly increases by 0.26 eV, attributed to the recombination of hole-electron pairs and a decrease in overall charge carriers, resulting in increased resistance. In selectivity investigations, compared to other volatiles (acetone, ethanol, benzene, and toluene), methanol’s smaller size enables it to access the active centers more readily. Consequently, the sensor demonstrates ultrahigh selectivity for methanol over other volatile organic compounds, with detection and quantification limits of 1.22 ppb and 4.02 ppb, respectively. Additionally, the CP1 sensor features rapid response and recovery times, recorded at 17.5 s and 34.2 s, respectively, making it well-suited for real-time applications. However, the synthesis of MOF membranes on an industrial scale is challenging due to its complexity and time-consuming nature. Moreover, research on bimetallic conducting MOF-based chemical resistors is still in its early stages, necessitating further exploration to enable industrial applications. Recently reported gas sensors for VOC detection are detailed in Table 3.

2.3. Flammable and Corrosive Gases

Flammable and corrosive gases are emitted during many manufacturing processes such as chemical vapor deposition, etching, thermal diffusion, and ion implantation [75,76,77]. Besides the acidic and alkaline or VOC, the process also emits an amount of inorganic gas with flammable (AsH3, SiH2Cl2, PH3, etc.) and/or corrosive (WF6, SiHCl3, SiCl4, etc.) properties [78,79,80,81,82]. Semiconductor factories prioritize the control of these gases during production and waste treatment to prevent accidents that could cause extensive damage. Nowadays, commercial detectors for gas control in semiconductor plants typically use catalytic combustion, semiconductor, and NDIR methods to detect flammable gases, and electrochemical and optical methods for corrosive gases [83]. The processing equipment is costly, and products are particularly susceptible to damage from fire, smoke, and water; hence, there is a significant risk of monetary loss from fires, even when confined to small areas. Workers face a high risk of organ damage from exposure to toxic gases such as AsH3, PH3, and WF6 during production, which can lead to respiratory diseases, convulsions, and death [84,85]. Therefore, the Occupational Safety and Health Administration (OSHA) in the United States sets maximum allowable concentrations of chemicals to protect workers during an 8-h workday [86]. It establishes permissible exposure limits to minimize health risks, such as a limit of 0.05 ppm for arsine (AsH3) and 0.3 ppm for phosphine (PH3). This section discusses studies aimed at developing effective AsH3 gas sensing devices.
To address the limitations of the tape method (inability to detect gas leaks in real-time) and electrochemical cells (risk of electrolyte leakage and high cost), Takada et al. pioneered research into solid-state gas sensors for detecting various toxic gases, including PH3, B2H6, AsH3, GeH4, and SiH4 (Figure 5a) [87]. Their investigations focused on B-doped diamond thin films, synthesized using the conventional hot filament chemical vapor deposition (CVD) technique with a gas mixture of methane (CH4) and boron hydride (B2H6), diluted in hydrogen (H2). They discovered that heat treating the diamond films at 600–700 °C during sensor assembly significantly improved sensitivity. The films treated at 700 °C exhibited a reproducible sensitivity increase to semiconductor manufacturing gases, whereas those treated at lower temperatures (e.g., 500 °C) showed reduced sensitivity. This research demonstrates that B-doped diamond thin films can detect extremely low concentrations of gases, such as 0.2 ppm PH3, 100 ppb B2H6, 50 ppb AsH3, 0.2 ppm GeH4, and 5 ppm SiH4, vital for leak detection in semiconductor manufacturing. However, the precise sensing mechanism and optimal production conditions are still undefined, with issues such as high operating temperatures and costly components yet to be resolved.
Virji et al. proposed a design for a more affordable, scalable, and inert sensing material for AsH3 detection devices (Figure 5b) [88]. The primary sensing material used in their study consists of polyaniline nanofiber-metal salt composites. These composites are produced by combining polyaniline nanofibers with copper(II) bromide to enhance their detection capabilities for AsH3. The sensing material was deposited on a self-designed interlayer electrode and then exposed to a constant flow of AsH3 gas in a chamber to assess its sensing ability. The acidic byproducts from the redox reactions dope the polyaniline, resulting in decreased resistance, which is a critical indicator of AsH3 presence. Furthermore, using nanostructured polyaniline with a high surface area enhances the sensor’s response by increasing the magnitude of resistance change and improving response time. The sensor demonstrates sensitivity to AsH3 concentrations as low as 100 ppb. However, the sensors’ sensitivity is influenced by environmental factors such as temperature and humidity, leading to variability in performance and reduced reliability under fluctuating conditions.
Furue et al. proposed an AsH3 sensor featuring a significantly low detection limit alongside an independent humidity sensor, employing gold-modified reduced graphene oxide (Au/rGO), which surmounts the challenges more effectively than previous studies (Figure 5c) [89]. The Au/rGO sensor exhibits improved reversible conductivity when exposed to AsH3, owing to the depletion of adsorbed oxygen on the gold islands, which enhances hole conduction in the rGO film. This sensor exhibited optimal response intensities at temperatures of 110 °C and 130 °C, with faster response times at 130 °C, which is established as the preferred operating temperature. To assess the material’s potential for gas control in semiconductor plants, Furue et al. investigated and compared the responses of the device to AsH3 and common gases in semiconductor plants, such as NO, NO2, NH3, and H2O2. The sensor achieved a detection limit of 10 ppb and showed selectivity for AsH3, although it also responded to NO2. However, the absence of NO2 in air-quality-controlled clean rooms does not affect its suitability for semiconductor applications.
Research on the development of sensors for flammable and corrosive gases continues, with efforts aimed at lowering operating temperatures, providing real-time signal outputs, reducing costs, and enabling detection of multiple gases [90,91]. However, experimental studies in this area have decreased significantly after 2017, as most research now primarily focuses on Density Functional Theory (DFT) methods [92,93,94,95]. This shift may be due to the risks involved in conducting experiments with toxic gases such as AsH3 and PH3. To promote the research and development of gas control devices, integrating experimental research with DFT studies can create a more comprehensive, effective, and insightful approach, thus bridging the gap between theoretical predictions and practical implementation.

2.4. Greenhouse Gas (GHG)

Semiconductor manufacturing emits all six families of GHG outlined by the Kyoto Protocol, including CO2, SF6, CH4, N2O, hydrofluorocarbons (HFCs), and perfluorocarbons (PFCs) [96,97]. In 2021, the semiconductor industry’s global Scope 1 and Scope 2 emissions totaled 76.5 megatons of CO2 equivalent (CO2 eq.), representing approximately 0.2% of the global emissions [98]. Processes such as deposition, photolithography, and etching, which consume substantial amounts of energy, are primarily responsible for these emissions. Fluorine gases are the predominant contributors to CO2 eq. emissions due to their exceptionally high global warming potential, ranging from 6290 to 11,100 times that of CO2, and their atmospheric lifetime spans approximately 2000 to 50,000 years [99]. Several governments and industries have adopted voluntary measures like carbon pricing or cap-and-trade systems to mitigate fluorinated gas emissions within the framework of broader climate commitments. Accurate monitoring and reporting of these emissions are vital for adherence to national climate action plans and international agreements such as the Paris Agreement. Currently, the primary techniques for detecting fluorinated gases are gas chromatography (GC) and Fourier-transform infrared spectroscopy (FTIR) [100,101,102]. However, these methods cannot achieve continuous sampling and analysis, and their associated testing procedures are inherently complex. This section explores research that shows promise in detecting emissions of fluorinated gases, such as SF6, CF4, C4F6, etc.).
Zhang et al. discovered a two-node hollow fullerene, which functions as a sensing material in gas sensor devices, showing outstanding sensitivity to tetrafluoromethane (CF4) gas molecules (Figure 6a) [103]. The material’s structure is composed of a C60 fullerene molecule connected to a half-C60 fullerene, with both sharing a hexagonal carbon ring. A device equipped with Au nanochains and two probes was designed to assess the sensitivity of the two-node hollow fullerene to CF4 molecules using a combination of DFT and nonequilibrium Green’s function formalism. The contour plot of the voltage drop, at a gate voltage of Vg = 0 V, demonstrates significant voltage drops when a CF4 molecule is encapsulated. This observation implies that CF4 molecules notably reduce electrical current, particularly under slight negative bias voltages, suggesting a strong interaction between the sensor and the gas that enhances its sensitivity. Notably, the sensor maintains its selectivity for CF4 even in humid conditions, effectively differentiating CF4 from water molecules without performance degradation—a crucial feature for practical applications in real-world environments.
Hexafluoroethane (CF3CF3, PFC-116), is identified as a potent PFC and the fourth strongest greenhouse gas with a lifespan exceeding 10,000 years in the atmosphere [104]. He et al. suggested that doping with non-metallic elements such as sulfur could enhance the gas sensing properties of tin oxide (SnO2) for CF3CF3, providing a cost-effective alternative to noble metal doping (Figure 6b) [105]. The fluorine in CF3CF3 exhibits a −1 valence state and reductive properties, whereas the doped sulfur possesses a +4 valence state, indicative of strong oxidative properties. Consequently, the doped sulfur significantly improves the sensing response to CF3CF3. Furthermore, with a grain size of merely 12.5 ± 2.2 nm, the sensing material offers a larger surface area and more active sites for gas adsorption. The sensor achieved a low detection limit of 0.5 ppm and demonstrated rapid response and recovery times of 10 s and 148 s, respectively. Additionally, the sensor effectively distinguishes CF3CF3 gas from CO2 and VOC gases. The considerable electronegativity of fluorine atoms, together with the lone pairs of electrons on the doped sulfur, facilitate the adsorption of CF3CF3 more readily than other gases. These features render the sensor highly suitable for real-time monitoring applications.
Meng et al. also proposed another approach to non-metallic doping sensing material (Figure 6c) [106]. They developed a fluorinated gas sensor using N-doped tin oxide (N-SnO2), significantly enhancing gas detection technology. Nitrogen doping in the tin oxide structure increases oxygen vacancies and creates more active sites. Upon exposure to air, oxygen molecules adsorb onto the surface and capture electrons from the tin dioxide, forming negatively charged ions such as O−, O2−, or O2−. This process of electron capture reduces the number of free electrons, leading to an increased resistance in the gas sensor. When exposed to gases such as SF6, C2F6, and C2H2F4, the negatively charged ions react with these gases, releasing the captured electrons back into the conduction band, altering the sensor’s resistance. The N-SnO2 sensor achieves ultra-sensitive detection of fluorinated greenhouse gases such as SF6, C2F6, and C2H2F4, with detection limits of 44 ppb, 7 ppb, and 48 ppb, respectively. This high sensitivity makes it highly effective for detecting low concentrations. The sensor’s optimal stability through multiple cycles confirms its reliability for long-term use. However, the paper does not fully explain the mechanism for distinguishing between these gases, necessitating further investigation. Furthermore, the sensor’s response to SF6 and C2H2F4 is similar, complicating the differentiation of these gases and their concentrations. Recently reported gas sensors for detecting GHG are documented in Table 4.
Chemosensors 12 00233 g006
Figure 6. (a) A two-node hollow fullerene is used as a sensing material in gas sensor devices, exhibiting remarkable sensitivity to CF4 [103]. Copyright 2020, Wiley. (b) Non-metallic doping (sulfur) enhances the CF3CF3 gas sensing properties of SnO2 [105]. Copyright 2024, Elsevier. (c) Nitrogen doping in the SnO2 structure increases oxygen vacancies, thereby enhancing the sensor’s performance [107]. Copyright 2024, Royal Society of Chemistry.
Figure 6. (a) A two-node hollow fullerene is used as a sensing material in gas sensor devices, exhibiting remarkable sensitivity to CF4 [103]. Copyright 2020, Wiley. (b) Non-metallic doping (sulfur) enhances the CF3CF3 gas sensing properties of SnO2 [105]. Copyright 2024, Elsevier. (c) Nitrogen doping in the SnO2 structure increases oxygen vacancies, thereby enhancing the sensor’s performance [107]. Copyright 2024, Royal Society of Chemistry.
Chemosensors 12 00233 g006
Table 4. Recently reported gas sensors for GHG detection.
Table 4. Recently reported gas sensors for GHG detection.
Materials and DevicesPrinciple of
Detection		Target GasOperating Temp.ResponseResponse TimeLODRef.
S-SnO2 SensorChemiresistiveC2F6200 °C13.44 at 25 ppm10 s0.5 ppm[105]
N-SnO2 SensorChemiresistiveC2F6200 °C11.9 at 30 ppm-7 ppb[106]
DAPPI-FAIMS 1PhotoionizationSF6RT0.25 pA at 3 ppm-0.02 ppm[107]
MDP sensor 2OpticalSF6RT2748 μV at 100 ppm1 s11 ppb[108]
CuO/TiO2 sensorChemiresistiveN2ORT0.011 at 1 ppm36 s50 ppb[109]
TCN(II)– KOH-rGO/CF sensor 3ElectrochemicalN2ORT−31 μA cm2 at 2 ppm5 s1 ppm[110]
TDLAS sensor 4OpticalCO40 °C133 ppt at 0.1 Hz200 s133 ppt[111]
CaO-ZnO sensorChemiresistiveCO2150 °C1.60 at 500 ppm170 s11 ppb[112]
1 Dopant-assisted atmospheric pressure photoionization combined with high-field asymmetric waveform ion mobility spectroscopy; 2 Multi-pass differential photoacoustic sensor; 3 Tetracyanonickelate (II)/KOH/reduced graphene oxide fabricated carbon felt-based sensor; 4 Tunable diode laser absorption spectroscopy.

3. Conclusions

Advanced gas sensors are vital for risk-safety management strategies and regulatory compliance in semiconductor manufacturing due to their high sensitivity, excellent selectivity, and rapid response times. This review explores various studies that show significant promise for monitoring hazardous gas emissions in semiconductor production. It elaborates on sensor materials, operating principles, and factors to improve sensor performance, highlighting their prospects and challenges. Despite substantial progress in gas sensor technology, further enhancements are needed to meet more stringent emission standards. These improvements include developing sensors capable of detecting multiple gases simultaneously, achieving ultra-low detection limits to verify the effectiveness of new emission gas treatment technologies, and designing sensors that are energy-efficient, cost-effective, and provide long-term stability. Additionally, it is crucial to ensure that sensors can withstand environmental factors such as humidity, temperature, and pressure. A combined approach involving experimental and DFT studies is essential for advancing a robust and efficient research and development process, bridging the gap between theoretical predictions and practical applications. Integrating materials science, nanotechnology, and data analytics can significantly improve sensor performance, address existing limitations, and broaden the detectable range of gases.

Funding

This work was supported by the Gachon University Research Fund of 2023 (GCU-202301000001).

Institutional Review Board Statement

Not applicable.

Informed Consent Statement

Not applicable.

Data Availability Statement

Not applicable.

Conflicts of Interest

The authors declare no conflicts of interest.

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Chemosensors 12 00233 g001
Figure 1. The basic steps to obtain a circuit layer and the corresponding exhaust gas at each step.
Figure 1. The basic steps to obtain a circuit layer and the corresponding exhaust gas at each step.
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Figure 2. Timeline chart illustrating the major developments in gas detection technologies.
Figure 2. Timeline chart illustrating the major developments in gas detection technologies.
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Figure 3. (a) The low-frequency QTF, utilized in the LITES sensor, improved signal output to about twice that of the commercial QTF [43]. Copyright 2022, Elsevier. (b) The fluorescent nanofilm based on an imine-bond sensor exhibited the ability to detect both HCl and NH3 [45]. Copyright 2023, American Chemical Society. (c) HCl and NH3 can be simultaneously detected in a mixture by evaluating two parameters: characteristic frequency (F) and resistance [46]. Copyright 2023, American Chemical Society.
Figure 3. (a) The low-frequency QTF, utilized in the LITES sensor, improved signal output to about twice that of the commercial QTF [43]. Copyright 2022, Elsevier. (b) The fluorescent nanofilm based on an imine-bond sensor exhibited the ability to detect both HCl and NH3 [45]. Copyright 2023, American Chemical Society. (c) HCl and NH3 can be simultaneously detected in a mixture by evaluating two parameters: characteristic frequency (F) and resistance [46]. Copyright 2023, American Chemical Society.
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Figure 4. (a) The structure and grain size of PAni composites lower the operating temperature of gas-sensing devices while enhancing their performance [67]. Copyright 2019, Elsevier. (b) The core-shell CsPbBr3@ZnO nanocrystals are employed as a sensing material in chemiresistive gas sensors to boost their sensing performance [68]. Copyright 2023, American Chemical Society. (c) The 2D semiconducting Cu(I) coordination polymer enhances the interaction of methanol molecules with active sites, improving sensing performance [69]. Copyright 2024, Wiley.
Figure 4. (a) The structure and grain size of PAni composites lower the operating temperature of gas-sensing devices while enhancing their performance [67]. Copyright 2019, Elsevier. (b) The core-shell CsPbBr3@ZnO nanocrystals are employed as a sensing material in chemiresistive gas sensors to boost their sensing performance [68]. Copyright 2023, American Chemical Society. (c) The 2D semiconducting Cu(I) coordination polymer enhances the interaction of methanol molecules with active sites, improving sensing performance [69]. Copyright 2024, Wiley.
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Figure 5. (a) Layers of solid-state gas sensors for detecting various toxic gases [87]. Copyright 2000, Elsevier. (b) Polyaniline nanofibers with copper(II) bromide used as a sensing material to enhance the detection capabilities for AsH3 of the gas sensor [88]. Copyright 2009, Elsevier. (c) The Au/rGO sensor exhibits reversible conductivity enhancement when exposed to AsH3 and displays the output signal in real time [89]. Copyright 2017, Elsevier.
Figure 5. (a) Layers of solid-state gas sensors for detecting various toxic gases [87]. Copyright 2000, Elsevier. (b) Polyaniline nanofibers with copper(II) bromide used as a sensing material to enhance the detection capabilities for AsH3 of the gas sensor [88]. Copyright 2009, Elsevier. (c) The Au/rGO sensor exhibits reversible conductivity enhancement when exposed to AsH3 and displays the output signal in real time [89]. Copyright 2017, Elsevier.
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Table 1. Advantages and disadvantages of some popular gas detection sensor technologies.
Table 1. Advantages and disadvantages of some popular gas detection sensor technologies.
No.Principle of
Detection		AdvantagesDisadvantages
1Catalytic
combustion		Simple operation
Fast response
Can detect mostly flammable gases
Low cost
Work in air or oxygen medium		Silicones, leaded fuels, and sulfur compounds poisoning
Environmental factors such as temperature and humidity affect accuracy
High power consumption
Requires a warm-up period
Unable to detect other types of gases
2Thermal
conductivity		Long-term stability
Not require oxygen to operate
Can detect a wide range of gases		High power consumption
Environmental factors such as temperature and humidity affect accuracy
Cross-sensitivity issues
Only gases with large differences in thermal conductivities can be distinguished
3Gas ChromatographyHigh sensitivity (ppb level)
Capable of analyzing complex multiphase separation gases		Cannot achieve continuous sampling and analysis
Complex system
4ChemiresistiveHigh sensitivity (ppm level)
Rapid response
Compact design
Capable of detecting a broad spectrum of gases (both toxic and flammable)		Susceptibility to sulfur and weak acid poisoning
Environmental factors such as temperature and humidity affect accuracy
Nonlinear feedback
Cross-sensitivity issues
5Nondispersive infrared sensor (NIDR)Capable of detecting multiple gases (CO2, GHG, etc.)
Does not involve chemical reactions
High sensitivity level
Accurate and quick measurements
Avoidance of cross-sensitivity		Only appropriate for gases with IR absorptivity (difficult to measure gases include: H2, N2, O2)
Elevated cost
Not user-friendly
Requires regular calibration
6ElectrochemicalHigh sensitivity (ppm level)
A wide range of gases can be detected (NOx, NH3, CO, etc.)
Rapid and accurate measurements
Low power consumption
Good linear output		Limited operating conditions, such as temperature ranging from −30 °C to +50 °C and relative humidity between 60% and 80%
Unable to differentiate between gas molecules from the same family
Requires regular calibration
7Surface acoustic wave (SAW)A wide range of gases can be detected, depending on the properties of the material on the sensing layer.
High sensitivity (ppb level)
Rapid and accurate measurements
Ease of integration
Small size		Environmental factors such as temperature and humidity affect accuracy
Complex electronic circuits
8Photoionization detector (PID)High sensitivity (ppb level)
A wide range of gases, including VOCs, acid, and toxic gases, can be detected		High cost
Verify the detection range before use
Accuracy is influenced by environmental factors such as humidity
Table 2. Recently reported gas sensors for detecting acidic and alkaline gases.
Table 2. Recently reported gas sensors for detecting acidic and alkaline gases.
Materials and
Devices		Principle of
Detection		Target GasOperating Temp.ResponseResponse TimeLODRef.
HCl-LITES Sensor 1OpticalHClRT711.6 μV at 500 ppm200 ms148 ppb[43]
UiO-66 Sensor 2OpticalHClRT22.75 nm at 2.5 ppm0.49 s10.9 ppb[47]
Si-NS FET Sensor 3Field-effect TransistorsHFRT1447% at 7.5 ppm333.6 s219 ppb[48]
HF-LITES sensor 4OpticalHFRT38 μV at 100 ppm110 s71 ppb[49]
Imine Bond-QCM 5 SensorOpticalHCl and NH3RT49 (a.u.) at 150 ppb (HCl)
20 (a.u.) at 1.5 ppm (NH3)		0.6 s (HCl)
0.3 s (NH3)		150 ppb (HCl)
1.5 ppm (NH3)		[45]
Si NWs-based
Sensor 6		SchottkyHCl and NH3-0.8% per μmol·L−1 (HCl) and −0.2% per μmol·L−1 (NH3) at 4 μmol·L−1 (80 ppb)1 min4 μmol·L−1
(80 ppb)		[46]
(Pt/MP-2) sensor 7ChemiresistiveNH3RT16.64 at 50 ppm15 s250 ppb[50]
PAni-Au@SiO2 sensor 8ChemiresistiveNH3RT80% at 10 ppm35 s10 ppb[51]
1 Light-induced thermoelastic spectroscopy-based sensor for hydrogen chloride; 2 UiO-66 3D photonic crystals optical sensor; 3 Silicon nanosheet-based field-effect transistor sensors; 4 Light-induced thermoelastic spectroscopy-based sensor for hydrogen fluoride; 5 Quartz Crystal Microbalance; 6 Si nanowire-based Schottky sensors; 7 Pt/MoS2/PAni gas sensor; 8 Core-shell Au@SiO2 nanocrystals doped with PAni-based sensor.
Table 3. Recently reported gas sensors for VOC detection.
Table 3. Recently reported gas sensors for VOC detection.
Materials and DevicesPrinciple of
Detection		Target GasOperating Temp.ResponseResponse TimeLODRef.
ZnO/PAni -based sensorChemiresistiveMethanol60 °C19.2 at 100 ppm18.2 s0.121 ppm[67]
CsPbBr3@ZnO sensorChemiresistiveMethanolRT0.13 at 10 ppm3.27 s1 ppm[68]
CP1 Chemiresistive sensor 1ChemiresistiveMethanolRT66.7 at 100 ppm17.5 s1.22 ppb[69]
CuO-based chemiresistive sensorsChemiresistiveAcetone200 °C610% at 500 ppm60 s125 ppm[70]
Au-SnO2 NRs 2 sensorChemiresistiveXylene400 °C170 at 10 ppm1.8 s0.1 ppm[71]
TiO2-based sensorsChemiresistiveXylene330 °C6.09 at 1 ppm<40 s5 ppb[72]
Ca-In2O3-based sensorsChemiresistiveFormaldehyde120 °C116 at 100 ppm1 s60 ppb[73]
Pt-SnO2-based sensorsChemiresistiveFormaldehyde200 °C16 at 1 ppm9 s60 ppb[74]
1 2D Copper(I) Iodide polymer chemiresistive sensor; 2 Au-coated SnO2 nanorods.
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Nguyen, M.T.N.; Lee, J.S. Development of a Chemical Sensor Device for Monitoring Hazardous Gases Generated in the Semiconductor Manufacturing Process. Chemosensors 2024, 12, 233. https://doi.org/10.3390/chemosensors12110233

AMA Style

Nguyen MTN, Lee JS. Development of a Chemical Sensor Device for Monitoring Hazardous Gases Generated in the Semiconductor Manufacturing Process. Chemosensors. 2024; 12(11):233. https://doi.org/10.3390/chemosensors12110233

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Nguyen, My Thi Ngoc, and Jun Seop Lee. 2024. "Development of a Chemical Sensor Device for Monitoring Hazardous Gases Generated in the Semiconductor Manufacturing Process" Chemosensors 12, no. 11: 233. https://doi.org/10.3390/chemosensors12110233

APA Style

Nguyen, M. T. N., & Lee, J. S. (2024). Development of a Chemical Sensor Device for Monitoring Hazardous Gases Generated in the Semiconductor Manufacturing Process. Chemosensors, 12(11), 233. https://doi.org/10.3390/chemosensors12110233

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