4.7 Article

Carbon Dot-Triggered Photocatalytic Degradation of Cellulose Acetate

Journal

BIOMACROMOLECULES
Volume 22, Issue 5, Pages 2211-2223

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.biomac.1c00273

Keywords

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Funding

  1. Wallenberg Wood Science Center - Knut and Alice Wallenberg Foundation
  2. Swedish Research Foundation, VR [2018-03451]
  3. Swedish Research Council [2018-03451] Funding Source: Swedish Research Council
  4. Vinnova [2018-03451] Funding Source: Vinnova

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Chemical modification of biopolymers can reduce their degradation susceptibility, with carbon dots acting as green photocatalytic triggers for degrading cellulose acetate in open environments. The addition of carbon dots catalyzes the deacetylation reaction, leading to significant weight loss, release of small molecules, and regeneration of cellulose fibers. These results show promise for developing products with environmentally degradable processes triggered by photocatalysis, such as mulching films.
Chemical modification of biopolymers, before use in thermo-plastic applications, can reduce the susceptibility to open environment degradation. We demonstrate carbon dots (CDs) as green photocatalytic triggers that can render the common cellulose derivative, cellulose acetate (CA), degradable under open environment relevant conditions. CD-modified cellulose acetate (CA + CD) films were subjected to UV-A irradiation in air and simulated sea water, and the degradation process was mapped by multiple spectroscopic, chromatographic, and microscopy techniques. The addition of CDs effectively catalyzed the deacetylation reaction, the bottleneck preventing biodegradation of CA. The photocatalytically activated degradation process led to significant weight loss, release of small molecules, and regeneration of cellulose fibers. The weight loss of CA + CD after 30 days of UV-A irradiation in air or simulated sea water was 53 and 43%, respectively, while the corresponding values for plain CA films were 12 and 4%. At the same time the weight average molar mass of CA + CD decreased from 62,000 to 11,000 g/mol and 15,000 g/mol during UV-A irradiation in air and simulated sea water, respectively, and the degree of substitution (DS) decreased from 2.2 to 1.6 both in air and in water. The aging in water alone did not affect the weight average molar mass, but the DS was decreased to 1.9. Control experiments confirmed the generation of hydrogen peroxide when aqueous CD dispersion was subjected to UV-A irradiation, indicating a free radical mechanism. These results are promising for the development of products, such as mulching films, with photocatalytically triggered environmental degradation processes.

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