Injection molded parts

Abstract

The present invention relates to an injection-molded part comprising a composition comprising: a. polyarylene sulfide (PAS) in an amount of 50% to 90% by weight; and b. glass fiber in an amount of 10% to 50% by weight, wherein the composition has a sodium content of up to 3500 ppm as measured by inductively coupled plasma atomic emission spectroscopy (ICP-AES); and the composition has an iodine content of up to 100 ppm as measured by X-ray fluorescence (XRF), wherein the weight percentages and ppm are based on the total weight of the composition. The present invention also relates to a fuel cell comprising the injection-molded part.

Description

Detailed Description of the Invention

[0001] The present invention relates to injection molded parts comprising a composition containing polyarylene sulfide and glass fibers. In particular, the present invention relates to fuel cell applications including injection molded parts. The present invention also relates to a method for preparing a composition containing polyarylene sulfide and glass fibers and a method for preparing an injection molded part containing said composition.

[0002] A fuel cell, particularly a proton exchange membrane fuel cell (PEMFC), is an electrochemical device that combines hydrogen fuel with oxygen to generate electricity, heat, and water. A plurality of fuel cells is called a fuel stack. A fuel stack can also include hundreds of individual fuel cells together with various components made from various materials such as, for example, polymer compositions and / or metals. Each of the individual fuel cells has a sandwich structure of a bipolar plate, a gas diffusion layer, and a proton exchange membrane and a platinum catalyst layer. The platinum catalyst oxidizes hydrogen molecules, thereby selectively allowing hydrogen ions to pass from the anode to the cathode and causing electrons to move as an electric current through an external device to the cathode. Considering the nature of the chemical reactions within a fuel cell, ions leaching from the materials utilized to manufacture the components for a fuel cell stack must be minimized and ideally prevented. Impurities and ions leaching from the components used in a fuel cell stack can be harmful to the catalyst, can clog the membrane, which can significantly reduce the efficiency of the fuel cell stack and affect its lifetime.

[0003] Any component for a fuel cell that is an injection-molded part containing a polyarylene sulfide and glass fibers must exhibit low ion leaching in order to maintain the efficiency of the fuel cell stack. Further, these injection-molded parts must exhibit sufficient hydrolysis stability, especially at elevated temperatures, particularly when in contact with water. The fuel cell operating temperature is typically 50 - 80 °C, with a peak temperature of about 110 °C, from which injection-molded parts are required that combine low ion leaching with sufficient hydrolysis stability, such as sufficient elongation at break and tensile strength, even after being exposed to water at elevated temperatures for longer periods of time.

[0004] The object of the present invention is to provide an injection-molded part that exhibits lower ion leaching and sufficient mechanical retention, such as sufficient elongation at break and / or tensile strength, especially after exposure to water or water / glycol at elevated temperatures, particularly in a hydrolytic environment. Surprisingly, this is achieved by a. a polyarylene sulfide (PAS) in an amount of 50 wt% to 90 wt%, b. glass fibers in an amount of 10 wt% to 50 wt% an injection-molded part comprising a composition containing the same, wherein the composition has a sodium content of at most 3500 ppm as measured by inductively coupled plasma atomic emission spectrometry (ICP-AES) and the composition has an iodine content of at most 100 ppm as measured by X-ray fluorescence (XRF), where the weight percent and ppm are relative to the total weight of the composition.

[0005] U.S. Patent Application Publication No. 2018 / 265701 relates to a resin composition comprising a polyarylene sulfide resin having a reduced chlorine content and a reduced sodium content and a filler. However, since polyarylene sulfide is prepared using the iodination of benzene and further reducing sulfur elements to form polyphenylene sulfide, the composition has a high iodine content. Therefore, in this polymerization process, it is difficult to fully achieve iodine recovery in this process, which results in the disadvantage of bringing about costly polyarylene sulfide. Moreover, iodine moieties accumulate in the polymer chain and / or end groups and can become more reactive in each thermal processing of polyarylene sulfide.

[0006] Injection molded parts are known per se and are obtained by an injection molding process known to those skilled in the art. Injection molding includes the steps of heating a composition containing PAS to a temperature higher than the melting temperature of PAS to obtain a melt, loading the melt into a mold, and then cooling the mold and the composition so that the composition solidifies into an injection molded part.

[0007] The injection molded parts according to the present invention comprise a composition containing polyarylene sulfide (PAS) in an amount of 50% to 90% by weight, where the weight percentages are based on the total weight of the composition. Preferably, PAS is present in an amount of 55% to 85% by weight, more preferably 60% to 80% by weight, and most preferably 60% to 70% by weight. In a preferred embodiment, PAS is poly(p-phenylene) sulfide (PPS) because PPS has the advantage of being readily available.

[0008] The injection molded parts according to the present invention comprise a composition having a sodium content of at most 3500 ppm, preferably at most 3000 ppm, even more preferably at most 2500 ppm, and most preferably at most 2000 ppm, based on the total weight of the composition. The sodium content can be measured by inductively coupled plasma atomic emission spectrometry (ICP-AES) as follows. The sodium content of the composition can be as low as about 20 ppm.

[0009] Preferably, the injection molded part according to the present invention comprises a composition having a crystallization temperature (Tc) of at least 230 °C, more preferably at least 235 °C, most preferably at least 240 °C, measured by DSC according to the method of ISO 11357-1 / 3 (2009), heating the composition at a scan rate of 10 °C / min up to 320 °C, holding the composition at 320 °C for 3 minutes under nitrogen, and then cooling the composition at the same scan rate and recording the crystallization temperature in the first cooling cycle. This has the advantage that it improves the hydrolysis stability of the injection molded part.

[0010] Preferably, the injection molded part according to the present invention comprises a PAS, more preferably PPS, having a sodium content in an amount of at most 500 ppm, more preferably at most 400 ppm, most preferably at most 300 ppm, even more preferably at most 250 ppm, where ppm is relative to the total weight of the respective PAS or PPS. The sodium content can be as low as about 5 ppm.

[0011] The injection-molded parts according to the present invention include, as a repeating unit, a composition in which PAS is mainly composed of -(Ar-S)- (where Ar is an arylene group). Examples of arylene groups are p-phenylene group, m-phenylene group, substituted phenylene group, p,p'-diphenylene ether group, p,p'-diphenylene carbonyl group, and naphthalene group. PAS can be polymerized by processes known to those skilled in the art. A particularly preferred manufacturing process includes a polymerization step of polymerizing a sulfur source and a dihaloaromatic compound in an organic polar solvent to produce a polyarylene sulfide. The said manufacturing process is disclosed by U.S. Patent No. 3,919,177 with respect to PPS. The said manufacturing process does not generate any chain bonds and / or any free iodine in the PAS. The obtained PAS such as PPS does not contain iodine, or if present, the iodine content is less than 10 ppm, preferably less than 5 ppm. The low sodium content of the above PAS can be achieved by acid washing. Acid washing is a procedure known per se. After polymerization of PAS, PAS is preferably treated by washing with an acid, washing with hot water, washing with an organic solvent, or a combination thereof to change the end groups of PAS from -SNa to -SH. Preferably, the washing solution has a pH value of 2 to 7, and suitable washing solutions can be acetic acid (CH3COOH), phosphoric acid (H3PO4), and oxalic acid (C2H2O4) or other organic acids, and more preferably acetic acid is used.

[0012] In addition, preferably, the crystallization temperature (Tc) of PAS, preferably PPS, is measured by DSC according to the method of ISO 11357-1 / 3 (2009), heating the composition at a scan rate of 10 °C / min up to 320 °C, holding the composition at 320 °C for 3 minutes under nitrogen, and then cooling the composition at the same scan rate, and recording the cold crystallization temperature in the first cooling cycle, and is at least 230 °C, more preferably at least 235 °C, most preferably at least 240 °C, thereby improving the hydrolysis stability of the injection-molded parts.

[0013] Preferably, the PAS has a weight average molecular weight (Mw) in the range of 10,000 to 100,000 g / mol, more preferably in the range of 20,000 to 80,000 g / mol, even more preferably in the range of 30,000 to 80,000 g / mol, and most preferably in the range of 30,000 to 70,000 g / mol.

[0014] Preferably, the polyarylene sulfide suitable in the present application has a PDI (weight average molecular weight / number average molecular weight; Mw / Mn) of less than 3, preferably less than 2.5, and more preferably less than 2.1.

[0015] Regarding the present invention, the molar mass of the polyarylene sulfide was determined by high-temperature size exclusion chromatography in accordance with the general guidelines for SEC analysis and subsequently in accordance with ASTM D5296-06. A PAS (or PPS if applicable) sample was dissolved in 1-chloronaphthalene at about 2 mg / ml at 230 °C. An Agilent PL-GPC 220 chromatograph equipped with a differential refractive index (RI), a differential viscometer (DV), and a multi-angle light scattering detector operating at scattering angles of 15° and 90° was used. In the calculation of the light scattering data, dn / dc was applied for PPS in 1-chloronaphthalene of 0.167. For polymer separation, a Three Polymer Laboratories PLgel Mixed-B column with a particle size of 10 μm and a size of 300×7.5 mm was utilized. The injection volume of the polymer solution was equal to 200 μl. The eluent used was 1-chloronaphthalene having 100 ppm of DBPC (BHT). The analysis temperature was set at 210 °C, and a flow rate of 1 ml / min was applied. The molar mass was calculated using a triple approach in which the light scattering detector was calibrated with a well-defined linear sample. The latter was also used to measure the multi-detector offset.

[0016] The linearity of the PAS of the present application preferably has a Mark-Houwink parameter of 0.70 ± 0.03, as taught and determined by C.J. Stacy, Molecular weight distribution of polyphenylene sulfide by high temperature gel permeation chromatography, Journal of Applied Polymer Science, 32 (1986) 3, pp3959-3969.

[0017] PAS, preferably PPS, preferably has a melt flow of 50 to 1000 g / 10 minutes, preferably 150 to 1000 g / 10 minutes, more preferably 200 to 800 g / 10 minutes, and most preferably 300 to 600 g / 10 minutes, as measured at 5 kg at 316°C and determined by the method of ISO 1133.

[0018] The injection molded parts containing the composition according to the present invention contain glass fibers in an amount of 10% to 50% by weight, and the weight percentage is based on the total weight of the composition. "Glass fiber" is understood herein to be glass particles having an aspect ratio L / D defined as the average ratio between the length (L) and the maximum of the width and thickness (D) of at least 5. Preferably, the aspect ratio of the glass fiber is at least 10, more preferably at least 20. Suitable glass fibers have a diameter of about 6 to 25 μm. Glass fibers generally have a length of 1 to 10 mm and a diameter of 6 to 15 μm, and may have a flat shape and a non-circular cross-sectional area with the width of the longer cross-sectional axis in the range of 6 to 40 μm and the width of the shorter cross-sectional axis in the range of 3 to 20 μm. The glass fiber is preferably selected from the group of E glass fiber, A glass fiber, C glass fiber, D glass fiber, S glass fiber and / or R glass fiber. Glass fibers such as DS8800-11P 4mm available from 3B are particularly suitable.

[0019] Preferably, the glass fiber is present in an amount of 20% to 45% by weight, more preferably 20% to 40% by weight, even more preferably 25% to 40% by weight, and most preferably 30% to 40% by weight, and the weight percentage is based on the total weight of the composition. Preferably, the glass fiber has a sodium content of less than 5000 ppm based on the total weight of the glass fiber when measured by ICP - AES. Preferably, the glass fiber has a sodium content of at most 3000 ppm, more preferably at most 1000 ppm, even more preferably at most 800 ppm, and ppm is based on the total weight of the glass fiber. The minimum sodium content can be as low as about 50 ppm.

[0020] The form in which the glass fiber is present in the composition can be that of continuous filament fibers or chopped or milled glass fibers. The fibers can include a suitable sizing system, and preferably, among others, particularly include a silane - based coupling agent. For example, suitable silanes include γ - aminopropyltriethoxysilane, γ - aminopropyltrimethoxysilane, γ - aminopropylmethyldiethoxysilane, γ - aminopropylmethyldimethoxysilane, N - β(aminoethyl)-γ - aminopropyltriethoxysilane, N - β(aminoethyl)-γ - aminopropyl - trimethoxysilane, N - β(aminoethyl)-γ - aminopropylmethyldiethoxysilane, N - β(aminoethyl)-γ - aminopropylmethyldimethoxysilane, N - phenyl - γ - aminopropyltriethoxysilane, and N - phenyl - γ - aminopropyltrimethoxysilane, and preferably, the aminoalkoxysilane is γ - aminopropyltriethoxysilane and / or γ - aminopropyltrimethoxysilane.

[0021] The injection - molded part is a. Polyarylene sulfide (PAS) in an amount of 50% to 90% by weight, b. Glass fiber in an amount of 10% to 50% by weight Comprising a composition, where the weight percentages are relative to the total weight of the composition, and the composition has a sodium content of at most 3500 ppm when measured by ICP - AES. The sodium content of the composition is preferably at most 3000 ppm, more preferably at most 2500 ppm, and even more preferably at most 2000 ppm. The sodium content of the composition can be as low as about 20 ppm.

[0022] The sodium content of PAS in the mixed composition or in the injection - molded part is measured by ICP - AES according to the following method. Since sodium remains stable during combustion, the sample is prepared by the ash residue method.

[0023] Step 1: Accurately weigh about 5 grams of the sample into a ceramic crucible and slowly combust it using a Bunsen burner. Then, place the combusted residue in a muffle furnace at 600 °C for 3 hours to ensure complete incineration. Since the percentage of ash is used for recalculating the actual sodium concentration in the original sample, weigh the crucible again and quantify the ash content.

[0024] Step 2: Using platinum laboratory equipment, melt about 1 gram of the ash residue at 1250 °C together with 5 grams of lithium metaborate. Weigh both amounts accurately.

[0025] Step 3: Dissolve about 1 gram of the melted material, which has been accurately weighed, in 10 ml of H2SO4 and 10 ml of H2O using a shaker for 16 hours.

[0026] Step 4: Further dilute the dissolved solution to 100 ml with H2O.

[0027] Step 5: Analyze the resulting solution by ICP - AES using an iCAP6500 spectrometer from Thermo Scientific. The measurement is performed against a calibration line prepared with a certified Specpure® standard solution from Alfa Aesar.

[0028] The injection-molded part contains a composition having a maximum iodine content of 100 ppm when measured by X-ray fluorescence (XRF). Preferably, the iodine content is at most 80 ppm, more preferably at most 70 ppm, and most preferably at most 50 ppm. The iodine content of the composition may be very low and thus may be lower than the detection limit of the XRF method, which is typically about 20 ppm.

[0029] The iodine content is measured by X-ray fluorescence (XRF). Due to its instability, iodine cannot be measured by the sample combustion method. Therefore, iodine is analyzed by XRF directly in the first polymer or in the composition. Parts such as flat plaques, for example tensile test specimens, are drilled in such a way that the bottom of the weighing cup is completely covered (diameter 40 mm, thickness 4 mm). The plaque is then analyzed by XRF using an AXIOS mAX Advanced WDXRF spectrometer from Panalytical equipped with a Rh X-ray tube. A reference sample is analyzed simultaneously to confirm the correct position of the iodine signal.

[0030] In a preferred embodiment, the injection-molded part contains a composition further comprising a coupling agent in an amount of 0.1 wt% to 1.0 wt% based on the total weight of the composition. Surprisingly, this leads to an improvement in the further hydrolysis stability of the composition.

[0031] The coupling agent is known per se and has the general formula (I): (X-(CH2) x ) y -Si-(O-C n H (2n+1) ) (4-y) Formula (I) wherein the definitions of the substituents are as follows. X is NH2. x is an integer from 1 to 10, preferably 2 or 3, y is an integer from 0 to 3, preferably 0 or 3, n is an integer from 1 to 3, preferably 1 or 2.

[0032] Suitable coupling agents include, for example, γ-aminopropyltriethoxysilane, γ-aminopropyltrimethoxysilane, γ-aminopropylmethyldiethoxysilane, γ-aminopropylmethyldimethoxysilane, N-β(aminoethyl)-γ-aminopropyltriethoxysilane, N-β(aminoethyl)-γ-aminopropyl-trimethoxysilane, N-β(aminoethyl)-γ-aminopropylmethyldiethoxysilane, N-β(aminoethyl)-γ-aminopropylmethyldimethoxysilane, N-phenyl-γ-aminopropyltriethoxysilane and N-phenyl-γ-aminopropyltrimethoxysilane. Preferably, the aminoalkoxysilane is γ-aminopropyltriethoxysilane and / or γ-aminopropyltrimethoxysilane. The coupling agent can be added during the preparation of the composition, which is usually carried out by mixing in an extruder. Preferably, the coupling agent is added by side feeding together with the glass fiber. Other suitable coupling agents are, for example, ureidopropyltrimethoxysilane or ureidopropyltriethoxysilane as disclosed in US Patent Application Publication No. 2015 / 0166731A1. Surprisingly, the addition of the coupling agent leads to a composition that exhibits further hydrolysis stability.

[0033] The present invention also relates to a fuel cell including injection molded parts according to any of the embodiments disclosed above. These injection molded parts include, for example, but not limited to, media distribution plates, manifolds, insulating plates, media connectors, air flow control valves, air flow shut-off devices, hydrogen injectors, hydrogen supply valves, hydrogen regulating valves, pressure control valves, hydrogen circulation pumps, humidifiers, thermostats, electrically controlled cooling valves, and electrically controlled coolant pumps.

[0034] One embodiment of the present invention is the injection molded part disclosed above, wherein the composition exhibits a tensile strength of at least 170 MPa, preferably at least 175 MPa, more preferably at least 180 MPa on an injection molded tensile test specimen 4 mm thick, measured at 23°C according to ISO 527-1A 5 mm / min after exposure to a water glycol (W / G) mixture (50% / 50% volume% / volume%) at a temperature of 135°C for 1000 hours. In another embodiment, the present invention is the injection molded part disclosed above, wherein the composition exhibits an elongation at break of at least 1.5%, preferably at least 1.6%, more preferably at least 1.7% on an injection molded tensile test specimen 4 mm thick, measured at 23°C according to ISO 527-1A 5 mm / min after exposure to a water glycol (W / G) mixture (50% / 50% volume% / volume%) at a temperature of 135°C for 1000 hours. In a preferred embodiment, the injection molded part exhibits the combination of tensile strength and elongation at break disclosed above. All individual ranges can be explicitly combined. Surprisingly, the injection molded part combines sufficient tensile strength and elongation at break after exposure to water / glycol at high temperature while reducing ion leaching. This enables applications where the injection molded part can come into contact with fluids containing water, in particular.

[0035] In a preferred embodiment, the present invention is an injection molded part as disclosed above, wherein the composition exhibits a tensile strength of at least 160 MPa, preferably at least 165 MPa, more preferably at least 170 MPa on an injection molded tensile test specimen 4 mm thick measured at 23°C according to ISO 527-1A 5 mm / min after exposure to steam at 110°C for 1000 hours in an autoclave. In another embodiment, the present invention is an injection molded part as disclosed above, wherein the composition exhibits an elongation at break of at least 1.2%, preferably at least 1.3%, more preferably at least 1.4%, even more preferably at least 1.5%, most preferably at least 1.6% on an injection molded tensile test specimen 4 mm thick measured at 23°C according to ISO 527-1A 5 mm / min after exposure to water at 110°C for 1000 hours. In a preferred embodiment, the injection molded part exhibits the combination of tensile strength and elongation at break as disclosed above. All individual ranges are explicitly combinable. In fuel cell applications, the injection molded part can come into contact with water at high temperatures, and surprisingly, the injection molded part according to the present invention exhibits sufficient elongation at break and tensile strength while reducing ion leaching.

[0036] The present invention relates to a composition comprising polyarylene sulfide and glass fibers, having a sodium content of at most 3500 ppm when measured by inductively coupled plasma atomic emission spectrometry (ICP - AES) and an iodine content of at most 100 ppm when measured by X - ray fluorescence (XRF), wherein the weight percentages and ppm are based on the total weight of the composition, and to a method for preparing the composition, the method comprising heating the PAS to a temperature above its melting temperature, for example using an extruder, and then adding the glass fibers to obtain a mixture, which mixture can then be cooled and preferably pelletized. Preferably, when the composition further comprises a coupling agent, the coupling agent is added to the PAS in a side feed together with the glass fibers, and more preferably, the coupling agent is an aminoalkoxysilane, γ - aminopropyltriethoxysilane and / or γ - aminopropyltrimethoxysilane. All the preferred ranges disclosed above are also applicable to the method for preparing the composition.

[0037] The present invention relates to a. polyarylene sulfide (PAS) in an amount of 50 wt% to 90 wt%, b. glass fibers in an amount of 10 wt% to 50 wt% The composition has a sodium content of at most 3500 ppm when measured by inductively coupled plasma atomic emission spectrometry (ICP - AES) and an iodine content of at most 100 ppm when measured by X - ray fluorescence (XRF), wherein the weight percentages and ppm are based on the total weight of the composition. All the preferred ranges disclosed above with respect to injection - molded parts comprising the composition are also applicable to the present invention relating to the composition.

[0038] [Examples:] [Materials used:] [Glass fibers:] NEG ECS03T - 747H / R available from NEG, having a sodium content of 4500 ppm with respect to the glass fibers. The iodine content was below the detection limit. DS8800-11P 4mm available from 3B, having a sodium content of 400 ppm with respect to the glass fiber. The iodine content was below the detection limit.

[0039] [PPS:] PPS A and PPS 1 were manufactured according to the process described in U.S. Patent No. 3,919,177. In this process, para-dichlorobenzene was reacted with NaHS in an N-methyl-2-pyrrolidone solvent at a high temperature of about 250 °C until the desired Mw was reached. For PPS 1, after polymerization, a washing step with water at a temperature of 80 °C was further performed to partially convert -SH to lead to a low sodium content, thereby reducing the amount of -SNa end groups.

[0040] The molecular characteristics, crystallization temperature, sodium and iodine contents of PPS A and PPS 1 were determined by the methods described hereinabove.

[0041] The results are shown below.

[0042]

Table 1

[0043] PPS A having a sodium content of 1500 ppm, which is 0.15% by weight based on the total weight of PPS. PPS 1 having a sodium content of 400 ppm. PPS A and PPS 1 have an iodine content below the detection limit.

[0044] Comparative material B: A504X90(C) available from Toray. This contains PPS having a sodium content of 1700 ppm based on the total weight of PPS and 40% by weight of glass fiber. The iodine content of comparative material B is below the detection limit.

[0045] Comparative Material C: 1140L4 available from Celanese. This composition contains 40 wt% glass fiber based on the total weight of the composition and has a sodium content of 0.47 wt% (4700 ppm). The iodine content of Comparative Material C is below the detection limit.

[0046]

Table 2

[0047] Compositions were prepared by mixing the materials shown in Table 1, except for Comparative B obtained from Toray and Comparative C obtained from Celanese.

[0048] To avoid breakage of the glass fiber, a mixture of PPS and a coupling agent was combined with the glass fiber and melt-mixed using a twin-screw extruder at a temperature of about 315 °C to about 420 °C. The melted composition was extruded to form strands, which were passed through a water bath and cut into pellets. The resulting pellets were dried at 140 °C for at least 4 hours and then molded into test articles by injection molding at a melting temperature of 315 °C to 345 °C at a mold cavity surface temperature of 135 °C to 150 °C, and tested for, for example, tensile strength test, tensile modulus test, and tensile strain.

[0049] For all tensile tests in the case of Table 2, they were carried out in accordance with the standard test method ISO 527-2. The test articles were subjected to tensile tests to obtain the initial characteristic values (T0 time values). The data are shown in Tables 2-1 to 2-6. The test articles were subjected to a water glycol (W / G) mixture (50% / 50% volume% / volume%). The W / G aging of the test articles was carried out in a closed stainless steel pressure vessel heated to 135 ± 2 °C using steam heating for various periods (e.g., 1 week, 2 weeks, and 6 weeks) as shown in Tables 2-1 to 2-3, by completely immersing the test articles (e.g., molded test pieces) in W / G to obtain aged test articles. Then, the aged test articles were recovered and subjected to tensile tests to obtain the final characteristic values. The data are shown in Tables 2-1 to 2-3 (tensile properties aged at 135 °C and tested at 23 °C). "n.m." in the table means not measured.

[0050]

Table 3

[0051]

Table 4

[0052]

Table 5

[0053] [Autoclave aging at 110 °C] The test articles were subjected to tensile tests to obtain the initial characteristic values described as T0 in the table. The data are shown in Tables 2-4 to 2-6. The test articles were subjected to steam at 110 °C in an autoclave for various periods as shown in Tables 2-4 to 2-6, that is, after 500 hours and 1000 hours, to obtain aged test articles. Then, the aged test articles were recovered and subjected to tensile tests to obtain the final characteristic values. The data are shown in Tables 2-4 to 2-6. This shows the tensile properties aged at 110 °C and measured at 23 °C.

[0054]

Table 6

[0055]

Table 7

[0056]

Table 8

[0057] Tables 2-1 to 2-3 clearly show that the elastic moduli of the various samples are similar. The tensile strength and EAB are the highest for Example 1 and remain higher even after long-term exposure to W / G. Comparative B shows a dramatic decrease in tensile strength and EAB, and these were no longer measurable after 1008 hours.

[0058] Tables 2-4 to 2-6 show that the elastic moduli of the various samples are similar. Also, here, the tensile strength and EAB are the highest for Example 1 and remain higher even after long-term exposure to water vapor. In contrast to Example 1, where the values were still sufficient even after 1000 hours, Comparative A and C showed a dramatic decrease in tensile strength and EAB.

[0059] [Leaching Experiment] [Sample Information] For the leaching experiment, three compositions, namely Comparative A, Comparative B, and Example 1 described in Table 1, were used as tensile test specimens. Half of the tensile test specimens were used. The test specimens had the following characteristics: a thickness of 4.0 mm and a total surface area of 32 cm 2 . ISO 527-1A was used for the test specimens.

[0060] [Leaching Incubation Protocol] 1) The test specimens were placed in 100 ml of ultrapure water (= 32 mm 2 / ml); 2) They were oven-aged at 90 °C in a closed Teflon (trademark) FEB bottle; 3) Incubation at 90 °C for 6 weeks. 100 ml of it was subjected to ICP-AES measurement. A reference sample by 100 ml of Blanco incubation in a Teflon bottle was also included.

[0061] [ICP-AES Setup for Leaching Results] Approximately 15 ml of liquid was collected for ICP-AES screening. The sample was acidified with 0.5 ml of HNO3 before measurement. Quantitative multi-component screening was performed using certified reference standards. Measurements were carried out using an iCAP6500 ICP-AES from Thermo Scientific. The main five leaching elements of Si, Ca, Al, K, and Na are shown in Table 3. Significant differences in leaching behavior were observed among various PPS samples.

[0062]

Table 9

[0063] Comparison B clearly showed the worst leaching performance for all reported elements. Next, Comparison A was close behind. Example 1 clearly showed the lowest leaching content for all reported elements.

Claims

1. a. A polyarylene sulfide (PAS) in an amount of 50% to 90% by weight, b. Glass fibers in an amount of 10% to 45% by weight comprising an injection-molded part made of a composition, wherein the composition has a sodium content of at most 3500 ppm when measured by inductively coupled plasma atomic emission spectrometry (ICP-AES), and the composition has an iodine content of at most 100 ppm when measured by X-ray fluorescence (XRF), and the % by weight and ppm are based on the total weight of the composition, the glass fibers have a sodium content of at most 3000 ppm based on the total weight of the glass fibers, the composition further comprises a coupling agent in an amount of 0.1% to 1.0% by weight based on the total weight of the composition, the coupling agent is selected from γ-aminopropyltriethoxysilane, γ-aminopropyltrimethoxysilane, γ-aminopropylmethyldiethoxysilane, γ-aminopropylmethyldimethoxysilane, N-β(aminoethyl)-γ-aminopropyltriethoxysilane, N-β(aminoethyl)-γ-aminopropyl-trimethoxysilane, N-β(aminoethyl)-γ-aminopropylmethyldiethoxysilane, N-β(aminoethyl)-γ-aminopropylmethyldimethoxysilane, N-phenyl-γ-aminopropyltriethoxysilane and N-phenyl-γ-aminopropyltrimethoxysilane, the composition has a tensile strength of at least 160 MPa and an elongation at break of at least 1.2% on an injection-molded tensile test specimen having a thickness of 4 mm measured at 23°C according to ISO 527-1A 5 mm / min after exposure to steam at 110°C for 1000 hours in an autoclave, an injection-molded part.

2. The amount of the PAS is 60% to 80% by weight, and the amount of the glass fibers is 20% to 40% by weight, and the % by weight is based on the total weight of the composition, the injection-molded part according to Claim 1.

3. The composition has a sodium content of at most 2000 ppm when measured by inductively coupled plasma atomic emission spectrometry (ICP-AES), the injection-molded part according to Claim 1 or 2.

4. The PAS has a sodium content of at most 500 ppm based on the total weight of the PAS, and is the injection molded part according to any one of claims 1 to 3.

5. The glass fiber has a sodium content of at most 800 ppm based on the total weight of the glass fiber, and is the injection molded part according to any one of claims 1 to 4.

6. The PAS has a crystallization temperature of at least 230 °C, which is measured by DSC according to the method of ISO 11357-1 / 3 (2009), heating the composition at a scan rate of 10 °C / min to 320 °C, holding the composition at 320 °C for 3 minutes under nitrogen, and then cooling the composition at the same scan rate to record the crystallization temperature in the first cooling cycle, and is the injection molded part according to any one of claims 1 to 5.

7. The composition has a tensile strength of at least 165 MPa on an injection molded tensile test piece with a thickness of 4 mm, which is measured at 23 °C according to ISO 527-1A 5 mm / min after exposure to steam at a temperature of 110 °C for 1000 hours in an autoclave, and is the injection molded part according to any one of claims 1 to 6.

8. The composition has a tensile strength of at least 170 MPa on an injection molded tensile test piece with a thickness of 4 mm, which is measured at 23 °C according to ISO 527-1A 5 mm / min after exposure to steam at a temperature of 110 °C for 1000 hours in an autoclave, and is the injection molded part according to any one of claims 1 to 7.

9. The composition has an elongation at break of at least 1.3% on an injection molded tensile test piece with a thickness of 4 mm, which is measured at 23 °C according to ISO 527-1A 5 mm / min after exposure to steam at a temperature of 110 °C for 1000 hours in an autoclave, and is the injection molded part according to any one of claims 1 to 8.

10. The composition has an elongation at break of at least 1.4% on an injection molded tensile test piece with a thickness of 4 mm, which is measured at 23 °C according to ISO 527-1A 5 mm / min after exposure to steam at a temperature of 110 °C for 1000 hours in an autoclave, and is the injection molded part according to any one of claims 1 to 9.

11. The injection-molded part according to any one of claims 1 to 10, wherein the composition has an elongation at break of at least 1.5% on an injection-molded tensile test piece with a thickness of 4 mm, measured at 23°C in accordance with ISO 527-1A 5 mm / min after exposure to steam at a temperature of 110°C for 1000 hours in an autoclave.

12. The injection-molded part according to any one of claims 1 to 11, wherein the composition has an elongation at break of at least 1.6% on an injection-molded tensile test piece with a thickness of 4 mm, measured at 23°C in accordance with ISO 527-1A 5 mm / min after exposure to steam at a temperature of 110°C for 1000 hours in an autoclave.

13. The injection-molded part according to any one of claims 1 to 12, wherein the polyarylene sulfide is polyphenylene sulfide.

14. The injection-molded part according to any one of claims 1 to 13, wherein the coupling agent is aminoalkoxysilane, γ-aminopropyltriethoxysilane and / or γ-aminopropyltrimethoxysilane.

15. A fuel cell comprising the injection-molded part according to any one of claims 1 to 14.

16. A composition comprising polyarylene sulfide (PAS) and glass fibers, the composition having a sodium content of up to 3500 ppm as measured by inductively coupled plasma atomic emission spectroscopy (ICP-AES) and an iodine content of up to 100 ppm as measured by X-ray fluorescence (XRF), wherein weight percent and ppm are based on the total weight of the composition, the glass fibers having a sodium content of up to 3000 ppm based on the total weight of the glass fibers, and further comprising a coupling agent in an amount of 0.1 wt. % to 1.0 wt. % based on the total weight of the composition, the coupling agent being selected from the group consisting of γ-aminopropyltriethoxysilane, ... and N-phenyl-γ-aminopropyltrimethoxysilane, γ-aminopropylmethyldiethoxysilane, γ-aminopropylmethyldimethoxysilane, N-β(aminoethyl)-γ-aminopropyltriethoxysilane, N-β(aminoethyl)-γ-aminopropyltrimethoxysilane, N-β(aminoethyl)-γ-aminopropylmethyldiethoxysilane, N-β(aminoethyl)-γ-aminopropylmethyldimethoxysilane, N-phenyl-γ-aminopropyltriethoxysilane and N-phenyl-γ-aminopropyltrimethoxysilane, said composition having an ISO 14149 purity at 23° C. after exposure to water vapor at a temperature of 110° C. for 1000 hours in an autoclave. 527-1A 5mm / min on a 4mm thick injection-molded tensile bar of at least 160 MPa and an elongation at break of at least 1.2%, the method comprising the steps of heating the PAS to a temperature above its melting temperature and then adding glass fibers to obtain a mixture which may then be cooled and suitably pelletized.

17. 17. The method of claim 16, wherein the coupling agent, which is an aminoalkoxyl silane, gamma-aminopropyltriethoxysilane and / or gamma-aminopropyltrimethoxysilane, is added to the PAS together with the glass fibers.

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