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Division of Radiation Research for Industry and Environment, Korea Atomic Energy Research Institute, 1266 Sinjeong-dong, Jeongeup-si, Jeollabuk-do 580-185, Korea
Received: January 20, 2015 / Revised: March 13, 2015 / Accepted: March 30, 2015 / Published: April 8, 2015
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Polyurethane (PU) is a very popular polymer used in a variety of applications due to its excellent mechanical, thermal, and chemical properties. However, PU recycling has received significant attention due to environmental concerns. In this research, we developed a recycling method for PU waste that uses the radiation grafting technique. Grafting of PU waste is carried out using polyethylene-graft-maleic anhydride (PE-g-MA) radiation technique. The PE-g-MA-grafted PU / high density polyethylene (HDPE) composite was prepared by melt-blending in various concentrations (0-10 phr) PE-g-MA-grafted PU. The composites were characterized using fourier transform infrared (FT-IR) spectroscopy, and the surface morphology and thermal/mechanical properties were reported. For 1 phr PU, PU can be easily introduced into HDPE during melt processing in a blender after radiation-induced grafting of PU with PE-g-MA. PE-g-MA easily reacts with PU according to the increase in radiation dose and is located at the interface between PU and HDPE during melting processing in the blender, which increases the interface interaction and the mechanical properties of the resulting composite. However, the elongation at break for PU content > 2 phr was drastically reduced.
Polyurethane (PU) is a very popular polymer used in various applications, such as in vehicles, furniture, and construction materials, due to its excellent mechanical, thermal, and chemical properties [1, 2]. However, PU recycling has received significant attention due to environmental concerns. Increasing landfill costs and decreasing landfill space have facilitated the consideration of alternative options for PU disposal. Therefore, there is a need to recycle or modify PU waste into some useful materials [3, 4]. PU can be recycled by various methods, such as mechanical recycling, advanced chemical and thermochemical recycling, energy recovery and product recycling [3]. Among these methods, mechanical recycling is done by grinding polyurethane foam into powder, allowing the converted material to be reused as filler [3].
Recently, nanofillers, such as nanoclay, nanosilica, carbon nanotubes and grapheme, have been used as commercial fillers for polymer composites [5]. However, this material is too expensive for mass production. In addition, the compatibility between the polymer and the filler significantly affects the quality of the composite [5].
PU is added as a reinforcing filler to increase the strength and thermal properties of commodity polymers [6]. However, the main disadvantage of incorporating PU into commodity polymers is its compatibility. PU is hydrophilic, while most commodity polymers are hydrophobic [7, 8].
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Surface modification or grafting polymerization is a good way to improve the adhesion of immiscible polymers or the adhesion between polymers and fillers [5, 9]. Radiation-induced grafting, compared to classical chemical grafting, provides several advantages such as uniform grafting and room temperature processing, and freedom from residuals of the initiator or catalyst [4, 10, 11]. In particular, radiation techniques can transfer energy to the solid state to create free radicals [12].
Here, we developed a recycling method for PU waste that uses a radiation grafting technique. Grafting of PU waste is carried out using polyethylene-graft-maleic anhydride (PE-g-MA) radiation technique. The PE-g-MA-grafted PU / high density polyethylene (HDPE) composite was prepared through melt-blending. Improved compatibility was obtained, and the mechanical properties of the composite were determined.
Commercial grade high-density polyethylene (HDPE; 5305E) was used throughout this study and was provided by Lotte Chemical Corporation (Yeosu, Korea). Polyurethane (PU) with yellow color was collected from railway waste disposal Envista, Inc. (Chungju, Korea). Polyethylene-graft-maleic anhydride (PE-g-MA) was purchased from Sigma Aldrich (St. Louis, MO, USA). Dimethylformamide was purchased from Samchun Pure Chemicals Co., Ltd. (Pyeongtaek, Korea). All other chemicals used were reagent grade and applied as purchased without further purification.
Waste PU particles (15 wt%) and PE-g-MA (5 wt%) were dipped in a dimethylformamide (DMF) solution (80 wt%) and mechanically stirred at room temperature until the chemicals were completely dissolved. The prepared mixture was irradiated using an electron beam accelerator (10 MeV/1 mA, Jeongup KAERI site, Jeonbuk, Korea). The total absorbed dose ranges from 10 to 70 kGy. Then, to remove the remaining solvent and moisture, the irradiated mixture was washed 3 times with DI water and dried in a vacuum oven at 60 °C for 24 hours.
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The PE-g-MA-grafted PU / HDPE composite is prepared by melt-blending in various concentrations (0-10 phr) PE-g-MA-grafted PU. The unit “phr” is an abbreviation of parts per hundred of resin, and the basic resin used here is HDPE. Melting compounding was carried out using a lab-scale blender (Brabender D-47055, Brabender, Germany) with a screw speed of 50 rpm at 160 °C for 15 min. After blending, the mixture is prepared using a square sheet in the form of a hot mold at a temperature of 180 ° C for 10 minutes.
Mechanical properties, such as tensile strength and elongation at break, were measured using a universal testing machine (Model 4210, Instron Engineering Co., Norwood, MA, USA) according to ASTM Standard D 638 [14]. Measurements were performed at room temperature at a crosshead speed of 50 mm/min.
The radiation-induced grafting of PU to the HDPE composite was analyzed via FT-IR (Tensor 37, Bruker, Billerica, MA, USA).
The surface morphology of the PU/HDPE composite was observed using a scanning electron microscope (SEM, Hitachi, S-4700, Tokyo, Japan).
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The static water contact angle was measured based on the sessile drop method using a Phoenix 300 contact angle analyzer (Surface Electro Optics Co., Suwon, Korea). Regarding the water contact angle, at least five specimens were tested, and the average value was obtained.
The storage modulus was measured using a dynamic mechanical analyzer (DMA, TA Instruments Q800, New Castle, NH, USA). The temperature increased from room temperature to 130 °C at a heating rate of 5 °C/min, and the oscillation frequency was 1 Hz.
The melting behavior and crystallinity of the composite were determined based on differential scanning calorimetry (DSC) (TA Instrument Q100, New Castle, NH, USA) from 30 to 180 °C at a heating rate of 10 °C/min in nitrogen gas. . The degree of crystallinity (Xc) can be calculated by the following equation.
= 290 J/g is the enthalpy of fusion for a completely crystalline polymer and ΔHm is the enthalpy of fusion calculated from the endothermic melting peak area.
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It is well known that PU/HDPE composites show poor mechanical properties, such as tensile strength and elongation at break, due to incompatibility [15].
To make a good composite, improving the compatibility between HDPE and PU is very important. In this study, the effect of radiation grafting on PU / HDPE composites to develop composites with better properties was investigated.
Figure 1 shows the mechanical properties, including the tensile strength and elongation at break of the PU/HDPE composite at various absorption doses. During this experiment, the PU content was 1 phr. The mechanical properties of the samples were tested at least five times, and the average value at the maximum point was recorded.
Tensile strength increased slightly with increasing radiation dose. As shown in Figure 1a, in a doe of 70 kGy irradiation, the tensile strength was 24 MPa. In addition, elongation at break drastically increased with increasing absorbed dose. When the absorbed dose was 70 kGy, the elongation at break of the PU/HDPE composite reached a maximum average value of 300%, which is about twice as large as the non-irradiated PU/HDPE composite (150%). These results show a significant improvement in the interface conditions between HDPE and
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