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JOURNAL OF SENSOR SCIENCE AND TECHNOLOGY - Vol. 34 , No. 3
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JOURNAL OF SENSOR SCIENCE AND TECHNOLOGY - Vol. 34, No. 3, pp. 163-173
Abbreviation: J. Sens. Sci. Technol.
ISSN: 1225-5475 (Print) 2093-7563 (Online)
Print publication date 31 May 2025
Received 17 Mar 2025 Revised 09 Apr 2025 Accepted 15 Apr 2025
DOI: https://doi.org/10.46670/JSST.2025.34.3.163

Development of In-Situ Hydrogen Permeation Measurement Technology Based on Volumetric and Manometric Analysis of Polymer Specimen under High Pressure Hydrogen Environment
Ji Hun Lee1, +
1Department of Measurement Science, University of Science and Technology, Daejeon 34113, Korea

Correspondence to : +gghoon0625@gmail.com


This is an Open Access article distributed under the terms of the Creative Commons Attribution Non-Commercial License(https://creativecommons.org/licenses/by-nc/3.0/) which permits unrestricted non-commercial use, distribution, and reproduction in any medium, provided the original work is properly cited.
Funding Information ▼
Abstract

Two in situ high-pressure permeation measurement systems were developed to assess the hydrogen permeation properties of the polymer sealing materials in high-pressure hydrogen environments. These systems enable real-time monitoring of hydrogen permeation after the injection of high-pressure hydrogen using both volumetric and manometric analyses for the precise quantification of hydrogen gas moles. With the integration of a custom-designed diffusion-permeation analysis program, systems can accurately calculate the key properties such as hydrogen diffusivity, permeability, and solubility. Hydrogen permeation tests were performed on Ethylene Propylene Diene Monomer (EPDM) materials with carbon black fillers, which are commonly used as O-ring seals in high-pressure hydrogen applications, to validate the system performance. The tests were performed across a pressure range of 1–10 MPa, and the results showed a decrease in hydrogen permeability and diffusivity as the pressure increased, whereas the solubility remained constant. This implies that hydrogen permeation in the polymer is mainly influenced by diffusion rather than solubility. In both systems, the H2 uptake of the EPDM specimen conformed to Henry's law. The measurement results of the two systems were consistent with the uncertainties, which confirms the reliability of the two systems for evaluating hydrogen permeability under high-pressure conditions.

Keywords: Hydrogen permeation, Diffusivity, Manometric analysis, In-situ, Diffusion-permeation analysis program
1. INTRODUCTION

Owing to its clean energy and high energy density, hydrogen is essential for fuel cells, storage, transportation, and industrial applications [1-8]. However, because of its small molecular size and high diffusivity, hydrogen can permeate materials, posing the risk of leakage and explosion during storage and transport [9,10]. Moreover, hydrogen permeation can cause material embrittlement and degradation, compromising the structural integrity. Therefore, accurate measurement of hydrogen permeability is critical for ensuring the safety and reliability of hydrogen infrastructure [11-20].

Hydrogen permeability measurements are particularly important for assessing the materials used in hydrogen technologies. For example, in storage and transportation systems, O-rings with strong hydrogen barrier properties are essential to prevent leaks in high-pressure tanks, pipelines, and valves [21-30]. Similarly, in fuel cells and hydrogen energy systems, evaluating the permeability of proton exchange membranes (PEMs) and components in fuel cell vehicles (FCEVs) helps improve their efficiency, durability, and safety [31-35].

The increase in the demand for hydrogen necessitates the development of advanced hydrogen barrier materials. Research has focused on enhancing polymer membranes, metal-polymer composites, and hydrogen-resistant coatings to prevent embrittlement and improve material stability [36-39].

Current methods for measuring hydrogen permeability include the differential pressure method, gas chromatography (GC), electrochemical methods, and gravimetric analysis. Despite its widespread use, it detecting low permeation rates is difficult using the differential pressure method [40-43]. Gas chromatography [44-51] offers high precision; however, it is complex and costly. The electrochemical method [51-55] is sensitive, but limited to conductive materials and requires frequent recalibration, whereas the gravimetric method [56-63] is simple but lacks precision for low permeation rates. Optical spectroscopy, catalytic combustion, and semiconductor-based gas sensors offer distinct advantages for permeability measurements. However, optical spectroscopy requires sophisticated instrumentation, catalytic combustion is constrained by selectivity and stability issues, and semiconductor-based sensors are prone to sensitivity drift over time [64-71]. These challenges highlight the necessity for versatile and precise measurement techniques.

This study introduces two novel volumetric and manometric analysis techniques integrated with the differential pressure method and an advanced diffusion-permeation analysis program [72-75]. These methods significantly enhance the measurement accuracy by compensating for temperature and pressure fluctuations. Furthermore, the hydrogen diffusivity, permeability, and solubility of Ethylene Propylene Diene Monomer (EPDM) polymers were assessed, validating the approach through a comparative analysis of the measurement results obtained from two distinct systems. The consistency between the two sets of results within the estimated uncertainties further confirms the reliability of both the systems for evaluating hydrogen permeability under high-pressure conditions. This enhanced measurement method refines the precision of hydrogen permeability assessments and contributes to the development of safer and more efficient sealing materials, such as O-rings, for the hydrogen economy.

2. SPECIMEN PREPARATION AND CHEMICAL COMPOSITION WITH KEY PROPERTY

Ethylene propylene diene monomer (EPDM) is known for its excellent chemical resistance, superior performance at low temperatures, and stable elasticity over a wide temperature range of -40 to 150°C, which makes it ideal for various industrial applications [76]. The addition of fillers such as silica or carbon black significantly improves the durability and hydrogen barrier properties of EPDM, particularly in high-pressure hydrogen environments [77,78]. Furthermore, high-hardness rubber materials are recognized for their exceptional resistance to degradation.

To develop a high-hardness rubber sample suitable for high-pressure hydrogen applications, an EPDM with a substantial carbon-black filler content was chosen for the measurement. The chemical composition and key properties of the EPDM are listed in Table 1. Permeability tests were performed using disk-shaped specimens, each with an effective diameter of 35 mm and a thickness of 2.2 mm, to ensure a sufficient permeation area while maintaining the mechanical stability under high-pressure conditions.

Table 1. 
Chemical composition and key properties of carbon blackfilled EPDM (Ethylene Propylene Diene Monomer) polymer. phr: parts per hundred rubber.
Chemical Compositions EPDM composite
Polymer EPDM 100 phr
Filler carbon black (N774) 90 phr
Cure agent Peroxide 5 phr
Key properties Density (g/cm3) 1.192
Hardness (Shore A) 90
Tensile strength (kgf/cm2) 230

3. PRINCIPLE FOR MEASURING HYDROGEN DIFFUSIVITY, PERMEABILITY AND SOLUBILITY
3.1. Measurement of the permeated hydrogen moles by volumetric and manometric analyses
3.1.1. Volumetric analysis

The molar quantity of hydrogen gas permeating through the polymer in the permeation cell after high-pressure hydrogen injection was measured in real time using the volumetric gas collection method [77-79]. As shown in Fig. 1 (a) and (b), the measurement from the permeation cell was performed within a specially designed cylinder, where variations in the water level were analyzed using an image brightness processing program. As the hydrogen diffused and permeated through the specimen in the permeation cell, it displaced the water inside the cylinder, which resulted in a gradual decrease in the water level, as shown in Fig. 1 (b).


Fig. 1. 
Permeation cell and volumetric/manometric method for evaluating the permeation characteristics of disc-shaped polymer specimen. (a) Internal structure of the high-pressure hydrogen permeation cell assembly, (b) volumetry analysis method with graduated cylinder, and (c) manometry analysis method with data logger and logger container. The red line illustrates the flow path of the injected high-pressure hydrogen, while the blue line indicates the release pathway of the permeated hydrogen, which is measured using volumetric analysis by image analysis algorithm or manometric analysis by data logger. The blue area in (b) is the distilled water.

Based on the principles of manometry, the internal pressure of the empty space within the cylinder, P(t), at a given time after pressure injection can be determined as the difference between the atmospheric and hydrostatic pressures, expressed as ρgh(t)[80-82].

Pt=Pot-ρght(1) 

where, Po(t) indicates the time-varying atmospheric pressure outside the cylinder,ρ is the density of distilled water at room temperature,g is the acceleration owing to gravity, andh(t) is the measured water level inside the cylinder, taken from the surface of the water container as a function of time. By measuring h(t), the volume of hydrogen gas (△V) permeated from the sample in the permeation cell can be determined. Thereafter, using the ideal gas law (PV = nRT), the number of moles of hydrogen gas permeated (△n ) can be calculated as follows [81,82].

Δnmol=PtΔVtRTt=Pot-ρghtΔVtRTt,ΔVt=Aht(2) 

where, R is the gas constant (8.20544 × 10-5 m3·atm/(mol·K)), T(t) is the temperature inside the cylinder as a function of time, and A is the inner cross-sectional area of the cylinder. The molar quantity of permeated H2, based on the change in the water level owing to hydrogen permeation from the sample, was obtained from Eq. (2).

First, Valve 2 is closed, Valve 1 is opened, and a hydrogen tank pressurizes hydrogen up to 10 MPa and stores it in a buffer tank. Considering the maximum storage pressure of the hydrogen tank (12 MPa), as shown in Fig. 2, the experimental pressure was set to a maximum of 10 MPa. Next, Valve 1 was closed and Valve 2 was opened, which allowed hydrogen to be injected into the specimen in the permeation cell up to the target pressure within a few seconds. The measurement began by recording the time from the moment Valve 2 was opened (t = 0). The quantitative measurement of the permeated hydrogen was recorded using the VM with the cylinder shown in Fig. 2 (b) and the MM with data logger 2 (c).


Fig. 2. 
Overall schematic representation of two high-pressure hydrogen permeation measuring systems. (a) Diagram illustrating the high-pressure hydrogen injection process with high pressure H2 tank and the permeation cell (b) volumetric method (VM) setup utilized for the precise quantification of permeated H2 using graduated cylinder. (c) manometric method (MM) setup utilized for the precise quantification of permeated H2 using portable manometer in logger container. The red line illustrates the flow path of the injected high-pressure hydrogen, while the blue line indicates the release pathway of the permeated hydrogen, which is measured using volumetric analysis or manometric analysis by data logger.

3.1.2. Manometric analysis

Fig. 1 (a) and (c) depicts the setup of the hydrogen permeation measurement, which employs a manometric sensor to quantify the molar amount of permeated hydrogen at room temperature. The measurement apparatus comprises a high-pressure permeation cell, as shown in Fig. 1 (a), a logger container featuring a rubber seal, and an integrated commercial USB-type data logger (Fig. 1 (c)). The ELP manometer sensor employed in this study is a commercially available data logger capable of simultaneously recording atmospheric pressure and temperature. Following the injection of high-pressure hydrogen to the permeation cell, the gas permeating through the sample induced a gradual pressure increase within the logger container. Consequently, the pressure (P) and temperature (T) inside the container vary over time. The gas behavior within the container adheres to the ideal gas law. The number of moles of H2 that permeated from the sample was determined by measuring the increase in pressure P(t), over time through manometric measurements at a constant container volume. The total number of moles n(t), corresponding to the pressure increase P(t), in the container can be expressed as follows [81,82]:

nt=PtV0RTt=PtV0RTt=P0+ΔPtV0RT01+αt≅P0V0+ΔPtV0RT01-αt=n0+Δnt,with n0=P0V0RT0, Δnt=V0RT0ΔPt-αtP0-αtΔPtαt=Tt-T0T0(3) 

where, T0, V0, and P0 represent the initial temperature, volume, and pressure of the air inside the container at the starting time, respectively; P(t) is the total pressure, consisting of the initial air pressure (Po) and the time-dependent pressure increase [ΔP(t)] caused by the permeated hydrogen, that is, P(t) = Po + ΔP(t). n0 is the number of moles of the remaining initial air, while Δn(t) corresponds to the time-dependent change in hydrogen moles owing to the pressure increase from the permeated hydrogen. α(t) denotes the rate of change in temperature relative to the initial temperature (T0).

3.2. Overall volumetric and manometric systems for measuring hydrogen diffusivity, permeability and solubility

Fig. 2 shows the two developed H2 permeation measurement systems, which enable both volume and pressure measurements of hydrogen permeated through the specimen. The system includes a high-pressure hydrogen tank, permeation cell, graduated cylinder, portable manometer (ELP logger), temperature sensor (UA10, DEKIST Co., Ltd., Yongin, Korea), pressure sensor (UA52, DEKIST Co., Ltd.), digital camera (D800, Nikon Co., Tokyo, Japan), and a computer running the developed program. The temperature and pressure data collected from the USB-based temperature and pressure sensors were used to calculate the amount of hydrogen that permeated through the sample using Eq. (2) for the volumetric method (VM) and Eq. (3) for the manometric method (MM).

The high-pressure hydrogen injection process using the system shown in Fig. 2 (a) is as follows.

3.3. Development of H2 diffusion–permeation analysis program

The molar amount of hydrogen permeating the specimen was measured using the permeation measurements illustrated in Fig. 2. The molar amount of the diffusing gas per unit area (A), denoted as Q(t), can be expressed as follows [83]:

Qt=ntA=lC1×Dtl2-l6-2π2Σ1∞-1nn2exp⁡⁡-Dn2π2t/l2(4) 

where, C1 represents the concentration at x = 0 in the high-pressure region while l denotes the thickness of the specimen. Considering the experimental setup of the permeation cell, Eq. (4) was derived based on the assumption that the polymer specimen initially had zero concentration within the range of 0 < x < l, and that the concentration at the diffusion exit face (x = l) was effectively maintained at zero.

The infinite-series expansions in Eq. (4) was computed by summing the first 50 terms, as higher-order terms were negligible with values smaller than 10-5. To ensure accuracy, a dedicated diffusion–permeation analysis program was developed to incorporate these 50 terms and calculate the diffusivity using Eq. (4). This approach demonstrated greater precision than the time lag (L) method, which relies on a simplified equation at infinite time given by L = l2 / 6D [83].

The permeability was obtained from the linear slope ΔnΔt  representing the change in moles of hydrogen over time as follows:

P=ΔnΔtlAΔP(5) 

where, A indicates the hydrogen contact area of the sample, ΔP is the pressure difference between the feed and permeate sides in the permeation cell, and Δl is the specimen thickness. H2 permeability was determined from the steady-state flow rate using Eq. (5). The H2 solubility (S) was obtained by dividing the permeability (P) by the diffusivity (D) as follows [32,36]:

S=PD(6) 

Fig. 3 shows an example of analyzing the hydrogen diffusion coefficient ( D ), permeability ( P ), and solubility ( S ) of an EPDM specimen using the developed hydrogen diffusion–permeability analysis program based on the molar amount of H2 measured at a hydrogen injection pressure of 5 MPa. The molar amount of H2 that permeated at each time point was calculated using Eq. (2) for the volumetric analysis or Eq. (3) for the manometric analysis. The analysis process is as follows.

First, after entering the thickness, effective permeation area, experimental pressure difference ( ΔP ), and permeated H2 molar amount for the disk-shaped specimen in the lower-left section of Fig. 3 (a), the curve fitting function, located in the middle-right section of Fig. 3 (a), is executed. Consequently, the lower-right section shows the diffusivity, permeability, and solubility values calculated using Eqs. (4), (5) and (6), yielding D = 2.481 × 10-10 m2/s, = 4.695 × 10-9 mol/m·s·MPa and S = 18.9295 mol/m3·MPa, respectively. Utilizing this specialized analysis program significantly reduces the measurement time and provides additional information, such as a figure of merit (FOM) of 0.8%, which indicates the deviation between the equations and the measured data, as shown in the middle section of Fig. 3 (a). Fig. 3 (b) shows the replotted results with the permeation parameters obtained using the diffusion–permeation analysis program. The blue line represents the results fitted based on Eq. (4) using the analysis program.


Fig. 3. 
Diffusion–permeation analysis program for determining H2 diffusivity, permeability and solubility using Eq. (4), (5) and (6) in EPDM polymer under injection pressure of 5 MPa. (a) graphical user interface of the program. (b) replotted result showing diffusivity (D), peameability (Pe) and solubility (S), obtained by diffusion-permeation analysis program.

4. MEASURED RESULTS AND DISCUSSIONS
4.1. Hydrogen permeation parameter versus injection pressure in two systems

Using a custom-designed high-pressure hydrogen permeation measuring system, the permeation characteristics of EPDM reinforced with a carbon black filler were investigated under high-pressure hydrogen conditions ranging from 1 to 10 MPa. Fig. 4 illustrates the pressure-dependent behavior of the permeation rate, permeability, diffusivity, and solubility in the VM and MM.


Fig. 4. 
Pressure dependence of hydrogen permeation properties in carbon black-filled EPDM polymer. (a) Permeation rate, (b) permeability, (c) diffusivity, and (d) solubility as a function of pressure, obtained using two systems (VM and MM).R2 is the squared correlation coefficient between measured data and fitted equation.

Fig. 4 (a) illustrates that the hydrogen permeation rate for both the VM and MM increased with pressure; however, the rate of increase progressively diminished at higher pressures. Theoretically, if the permeability remains independent of pressure, Eq. (5) predicts a linear relationship between the permeation rate and pressure passing through the origin. However, the observed reduction in the rate of increase suggests that permeability decreases with increasing pressure, as depicted in Fig. 4 (b).

This trend is consistent with those of previous studies on the pressure dependence of gas permeability in polymers. According to Stern et al. [84] and Naito et al. [85], gas permeation behavior in polymers can be classified based on the relationship between permeability and pressure. Condensable vapors, such as CO, N2O, and organic vapors, exhibit a positive correlation, where permeability increases with pressure. Conversely, permanent gases with extremely low liquefaction temperatures, such as N2 and He, d°isplayed a negative correlation, indicating a decrease in permeability with increasing pressure. Because hydrogen also falls into the category of permanent gases, the results presented in Fig. 4 (b) confirm a similar trend, demonstrating that the hydrogen permeability declines with increasing pressure.

Fig. 4 (c) illustrates a decline in diffusivity with increasing pressure in both the VM and MM. This trend can be attributed to free volume theory, which states that gas molecules migrate through the transient voids generated by the thermal motion of the polymer chains [86,87]. Under high-pressure conditions, the available free volume within the polymer matrix decreases, thereby restricting the molecular mobility and resulting in reduced diffusivity [22].

Fig. 4 (d) indicates that the solubility remained relatively stable in the two methods within the uncertainty range, regardless of the pressure variations. This finding suggests that the observed decrease in permeability at elevated pressures was primarily driven by reduced diffusivity owing to diminished free volume rather than changes in solubility. Additionally, the hydrogen permeation behavior of polymeric materials under high-pressure conditions is governed not only by the dissolution–diffusion mechanism but also by other complex factors, including internal pore structures, pressure-induced morphological changes, and interactions between the polymer matrix and embedded fillers [88].

4.2. Hydrogen uptake versus injection pressure in the two systems

Using the measured solubility values, the hydrogen uptake was calculated using the following equation [32]:

Hydrogen Uptake wtppm=s⋅mH2⋅Pds(7) 

where, S represents the solubility, mH2 is the molecular weight of hydrogen gas (2.016 g/mol), P denotes the pressure, and ds [g/m3] is the density of the polymer specimen. This equation was applied to all the solubility values presented in Fig. 4 (d), and the resulting H2 uptake data in both VM and MM are depicted in Fig. 5.

The behavior of hydrogen dissolution in polymers is typically interpreted using models such as Henry's law and the Langmuir adsorption model. Henry's law states that the amount of gas absorbed by a polymer matrix is directly proportional to the applied pressure, which is applicable when hydrogen is uniformly absorbed by the polymer matrix [89]. Conversely, the Langmuir adsorption model accounts for scenarios in which hydrogen molecules are adsorbed onto specific sites within the polymer or on the filler surfaces, which causes saturation at higher pressures [90-93]. In our findings, the H2 uptake results in the two systems (VM and MM) for the EPDM polymer containing carbon black filler followed Henry's law with a squared correlation coefficient of R2=0.98, indicating a good fit.


Fig. 5. 
H2 uptake versus pressure in carbon black-filled EPDM polymer obtained by the two systems (VN and MM), calculated using Eq. (7).

5. CONCLUSION

In this study, two in-situ measurement systems were developed to evaluate the H2 permeation characteristics of polymer-sealing materials under high-pressure conditions (up to 10 MPa). This system enables precise quantification of hydrogen permeation over time through volumetric and manometric analyses following high-pressure hydrogen injection. Additionally, a custom-built diffusion-permeation analysis program was used to accurately determine the key parameters, including permeability, diffusivity, and solubility.

Using integrated systems, the hydrogen permeation properties of EPDM containing carbon black fillers across a pressure range of 1 MPa to 10 MPa were systematically assessed. The results obtained for the two systems indicated that as the pressure increased, both the permeability and diffusivity exhibited decreasing trends, whereas the solubility remained largely unchanged. These findings suggest that H2 transport in polymers is predominantly governed by diffusion constraints owing to a reduction in the free volume, with the decline in diffusivity being the primary driver of reduced permeability rather than variations in solubility. Moreover, the hydrogen uptake behavior of the EPDM polymer closely followed Henry's law and exhibited a good squared correlation coefficient. The measurement results of the volumetric and manometric systems were consistent with the estimated uncertainties, confirming the reliability of the two systems for evaluating hydrogen permeability under high-pressure conditions.

In summary, the experimental system and analytical approach established in this study provide a robust framework for the quantitative evaluation of the sealing properties of polymer materials in high-pressure hydrogen environments. These advancements could significantly contribute to the optimization and development of sealing materials for hydrogen applications, such as H2 transfer pipelines.

Authorship Contribution Statement

Ji Hun Lee: Conceptualization, Investigation, Methodology, Validation, Writing - original draft, Writing - review & editing.

Declaration of Competing Interest

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Acknowledgments

This research was supported by the Korea Institute of Energy Technology Evaluation and Planning (KETEP) grant funded by the Ministry of Trade, Industry and Energy (MOTIE) of the Republic of Korea. (No. RS-2024-00449107)

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