Carbene-Mediated Photoconversion of Cellulose Diacetate.
basic_science · Level V
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- Record sourced from PubMed, PMID 42206526.
- Also identified by DOI 10.1021/acsnano.6c02702.
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Abstract
Amid rising global demand for renewable energy and effective plastic waste management, adopting green methods to utilize plastic waste for chemicals is a win-win strategy. Constituting the largest amount of single-use plastic litter worldwide, cellulose diacetate (CDA) based waste cigarette filters urgently require sustainable valorization pathways. However, CDA photoconversion remains highly challenging due to substantial energy barriers for selective bond cleavage, inadequate radical generation capability, and inefficient charge-carrier separation. Herein we propose a strategy to efficiently obtain C<sub>2</sub>H<sub>4</sub> through carbene-mediated CDA photoconversion by using a sulfur vacancy-regulated copper-gallium-zinc-sulfide (V<sub>S</sub>-CGZS) catalyst. V<sub>S</sub>-CGZS enhances the thermal effect of light and lowers the energy barrier for acetyl group (*CH<sub>3</sub>CO) desorption from CDA. V<sub>S</sub> reduces the adsorption energy of *CH<sub>3</sub>CO on V<sub>S</sub>-CGZS and facilitated :CH<sub>2</sub> formation. Consumption of photogenerated holes via *CH<sub>3</sub>CO desorption and V<sub>S</sub>-enhanced carrier separation synergistically elevate the photogenerated electrons concentration for :CH<sub>2</sub> coupling, thereby selectively triggering and boosting C<sub>2</sub>H<sub>4</sub> yield. Therefore, we achieve a record-breaking 14.43 mmol·g<sub>cat</sub><sup>-1</sup> C<sub>2</sub>H<sub>4</sub> for CDA photoconversion within 4 h, over 6 times exceeding previous reports on photoconverting plastic into C<sub>2</sub>H<sub>4</sub>. This work establishes a strategy for efficient ethylene production from photoconversion of cellulose diacetate and carves out a paradigm in solar-driven plastic valorization.