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Ultrasound-Assisted Extraction of Methylxanthines from Cocoa Bean Shells Using Glycerol-Urea Natural Deep Eutectic
Luciana L Nascimento1, Paulo N A Dos Santos2, Luciano Albuquerque1
1Programa de Pós-Graduação em Ciência de Alimentos, Universidade Federal da Bahia, Salvador, BA 40170-115, Brazil.
ACS Omega
|October 6, 2025
Summary
This study optimized ultrasound-assisted extraction of theobromine and caffeine from cocoa shells using eco-friendly glycerol-urea solvents. The green method efficiently recovers bioactive compounds for food and nutraceutical applications.
Area of Science:
- Green Chemistry
- Extraction Technologies
- Food Science
Background:
- Cocoa bean shells are a rich source of bioactive compounds.
- Efficient and sustainable extraction methods are needed for valorizing cocoa processing residues.
Purpose of the Study:
- To optimize ultrasound-assisted extraction of theobromine and caffeine from cocoa bean shells.
- To utilize glycerol-urea natural deep eutectic solvents for enhanced extraction efficiency and sustainability.
Main Methods:
- Ultrasound-assisted extraction (UAE) optimized using a Doehlert design.
- Glycerol-urea natural deep eutectic solvents (DES) characterized by rheological analysis and infrared spectroscopy.
- Quantification of theobromine and caffeine using high-performance liquid chromatography (HPLC).
Main Results:
- Optimized conditions (45.5% water, 4 min sonication) yielded high concentrations of theobromine (29.18 mg g⁻¹ DM) and caffeine (2.46 mg g⁻¹ DM).
- Extracts exhibited significant antioxidant capacity (ABTS: 230.65 mg TE g⁻¹ DM, DPPH: 74.34 mg TE g⁻¹ DM).
- Greenness assessment confirmed low environmental impact, aligning with green chemistry principles.
Conclusions:
- The proposed UAE method using glycerol-urea DES is a sustainable and efficient alternative for recovering bioactive compounds from cocoa waste.
- The process is cost-effective, uses food-relevant components, and supports circular economy strategies.
- The resulting extract is suitable for food, beverage, and nutraceutical ingredient formulation.

