Degradation of low-density polyethylene to nanoplastic particles by accelerated weathering

Menzel, Teresa; Meides, Nora; Mauel, Anika; Mansfeld, Ulrich; Kretschmer, Winfried P.; Kuhn, Meike; Herzig, Eva M.; Altstädt, Volker; Strohriegl, Peter; Senker, Jürgen; Ruckdäschel, Holger

doi:10.1016/j.scitotenv.2022.154035

Cited by 60 publications

(40 citation statements)

References 51 publications

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“…Additionally, solid-state 13 C magic-angle spinning (MAS) NMR spectroscopy was performed for identification and quantification of photooxidative defects accumulating with proceeding degradation. As previously reported [5,41] quantification is enabled by a multiple cross polarization (multiCP) pulse sequence [42,43]. Although solid-state NMR spectroscopy has rarely been considered for investigation of degradation products, it serves as a complementary method to other commonly used techniques, such as Fourier transform infrared (FTIR) or Raman spectroscopy, and pyrolysis-gas chromatography-mass spectrometry (Py-GC-MS) [23,24,28,29,[44][45][46].…”

Section: Introductionmentioning

confidence: 99%

Quantifying the fragmentation of polypropylene upon exposure to accelerated weathering

et al. 2022

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Polymers are omnipresent in our everyday lives. For specific applications, their properties can be extensively modified by various types of additives, e.g., processing stabilizers, antioxidants, UV-stabilizers, flame retardants, and plasticizers. While several additives are nowadays considered to be toxic or persistent in the environment, quantitative data characterizing plastic fragmentation and microplastic formation have not yet been discussed in detail. Here, we present a long-term, laboratory-controlled accelerated weathering study on polypropylene (PP) particles with and without processing stabilizers. We were able to identify the stabilizers as Irgafos® 168, and Irganox® 1010. For both PP sample sets, we monitored the degradation using a combination of various analytical methods, such as gel permeation chromatography, particle size distributions, scanning electron microscopy, solid-state 13C magic-angle spinning NMR and liquid-state 1H, 13C, 31P NMR spectroscopy, differential scanning calorimetry and matrix-assisted laser desorption ionization time of flight mass spectrometry. The stabilizers prevent degradation by simulated solar radiation for about 350 h. Then, degradation sets in rapidly, leading to an exponential decrease in molecular weight and particle size, accompanied by an increase in crystallinity and the formation of oxygen-containing functional groups. After 3200 h, representing approximately 2 years of outdoor weathering, both PP samples exhibit comparable characteristics and sizes, regardless if a stabilizer was initially present. During degradation, an extremely large number of 100,000 daughter particles (4 µm) are formed and released from one MP particle of 192 µm diameter. Their physical properties and chemical composition have largely changed, resulting in a very low molecular weight and a hydrophilic character. These particles no longer resemble pristine PP. We thus expect them to be more prone to biodegradation compared to the starting material.

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Section: Introductionmentioning

confidence: 99%

Quantifying the fragmentation of polypropylene upon exposure to accelerated weathering

et al. 2022

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“…Comparing the time constants of particle disintegration, we estimate that PP degrades ~ 6 times faster than PS (5) and ~ 4 times faster than LDPE (43). The average particle size of the reference (~ 190 µm) decreases down to 4 µm after 3200 h of irradiation with simulated solar radiation, which is comparable to ~ 2 years of outdoor weathering in Central Europe (Table S1).…”

Section: Discussionmentioning

confidence: 82%

“…Recently, we developed a three-stage degradation model for semi-crystalline, non-stabilized polymers, using unstabilized LDPE as exemplary material (43). Stage I represents surface abrasion, characterized by a roughly constant particle size, accompanied by a rounding of the particle surface.…”

Section: Particle Surface and Degradation Characteristicsmentioning

confidence: 99%

“…Additionally, solid-state 13 C Magic-Angle Spinning (MAS) NMR spectroscopy was performed for identi cation and quanti cation of photooxidative defects accumulating with proceeding degradation. As previously reported (5,43) quanti cation is enabled by multiple cross polarization (multiCP) pulse sequences (44,45). Although solid-state NMR spectroscopy has rarely been considered for investigation of degradation products, it serves as a complementary method to other commonly used techniques, such as Fourier Transform Infrared (FTIR) or Raman spectroscopy, and pyrolysis-gas chromatography-mass spectrometry (Py-GC-MS) (25,46,31,47,30,48,26).…”

Section: Introductionmentioning

confidence: 95%

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Quantifying the Fragmentation of Polypropylene upon Exposure to Accelerated Weathering

Meides

Mauel

Menzel

et al. 2022

Preprint

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Polymers are omnipresent in our everyday lives. For specific applications, their properties can be extensively modified by various types of additives, e.g., processing stabilizers, antioxidants, UV-stabilizers, flame retardants, and plasticizers. While several additives are nowadays considered to be toxic or persistent in the environment, quantitative data characterizing plastic fragmentation and microplastic formation have not yet been discussed in detail. Here, we present a long-term, laboratory-controlled accelerated weathering study on polypropylene (PP) particles with and without processing stabilizers. We were able to identify the stabilizers as Irgafos® 168, and Irganox® 1010. For both PP sample sets, we monitored the degradation using a combination of various analytical methods, such as Gel Permeation Chromatography, Particle Size Distributions, Scanning Electron Microscopy, solid-state 13C Magic-Angle Spinning NMR and liquid-state 1H, 13C, 31P NMR Spectroscopy, Differential Scanning Calorimetry and Matrix-Assisted Laser Desorption Ionization Time of Flight Mass Spectrometry. The stabilizers prevent degradation by simulated solar radiation for about 350 h. Then, degradation sets in rapidly, leading to an exponential decrease in molecular weight and particle size, accompanied by an increase in crystallinity and the formation of oxygen-containing functional groups. After 3200 h, representing approximately 2 years of outdoor weathering, both PP samples display comparable characteristics and sizes, regardless of the stabilizer initially present. During degradation, an extremely large number of 100000 daughter particles (4 µm) are formed and released from one MP particle of 192 µm diameter. Their physical properties and chemical composition have largely changed, resulting in a very low molecular weight and a hydrophilic character. These particles no longer resemble pristine PP. We thus expect them to be more prone to biodegradation compared to the starting material.

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“…, for weathered LDPE particles, significantly higher carboxyl proportions were detected with FTIR spectroscopy compared to 13 C MAS NMR spectroscopy, which was attributed to a preferential accumulation of carboxyl groups close to the surfaces. 45 NMR spectroscopy is an element sensitive bulk method and can be used in a quantitative fashion. 46 If the samples are soluble, 1 H liquid-state NMR spectroscopy provides sufficient sensitivity.…”

Section: Introductionmentioning

confidence: 99%

Quantification of photooxidative defects in weathered microplastics using¹³C multiCP NMR spectroscopy

et al. 2022

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Degradation of low-density polyethylene to nanoplastic particles by accelerated weathering

Cited by 60 publications

References 51 publications

Quantifying the fragmentation of polypropylene upon exposure to accelerated weathering

Quantifying the fragmentation of polypropylene upon exposure to accelerated weathering

Quantifying the Fragmentation of Polypropylene upon Exposure to Accelerated Weathering

Quantification of photooxidative defects in weathered microplastics using¹³C multiCP NMR spectroscopy

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Degradation of low-density polyethylene to nanoplastic particles by accelerated weathering

Cited by 60 publications

References 51 publications

Quantifying the fragmentation of polypropylene upon exposure to accelerated weathering

Quantifying the fragmentation of polypropylene upon exposure to accelerated weathering

Quantifying the Fragmentation of Polypropylene upon Exposure to Accelerated Weathering

Quantification of photooxidative defects in weathered microplastics using13C multiCP NMR spectroscopy

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Quantification of photooxidative defects in weathered microplastics using¹³C multiCP NMR spectroscopy