The starting material was Arabica coffee grounds collected from a local coffee shop, dried to about five percent moisture and defatted with n-hexane. Coffee grounds are carbohydrate-rich, with carbohydrates representing 57 to 82 percent of the dry matter depending on the coffee source and processing conditions. These carbohydrates exist mainly as polysaccharides such as cellulose, hemicellulose, pectin, and galactomannans. The researchers used an alkaline extraction method, mixing the dried grounds with sodium hydroxide solution at a solid-to-liquid ratio of 1:20 and heating to 95 °C for three hours at four different pH values: 8, 9, 10, and 11. After centrifugation, concentration, ethanol precipitation, dialysis, and lyophilization, the team obtained polysaccharide–protein composite powders that spontaneously form nanoparticles in water.

Extraction pH proved decisive. The product yield increased significantly with increasing alkalinity, reaching 7.00 ± 0.64 percent at pH 11, as alkali more effectively disrupted the cell wall structure and released more polysaccharide molecules. Total sugar content peaked at pH 9 with 53.26 ± 2.64 percent, but protein content climbed steadily to 19.56 ± 1.34 percent at pH 11. Galactose was the predominant monosaccharide in all samples, reaching 62.52 percent at pH 11, confirming that the extracted polysaccharides originate primarily from cell-wall hemicellulose. The weight-average molecular weight also increased with pH, from 8.95 kDa at pH 8 to 15.28 kDa at pH 11, because hydroxide ions hydrolyze acetyl and glycosidic bonds in hemicellulose, liberating higher-molecular-weight components.

Structural analysis revealed that all samples were amorphous, with no obvious crystalline diffraction peaks in X-ray diffraction patterns. Fourier-transform infrared spectroscopy showed characteristic carbohydrate bands near 3469 and 2926 cm⁻¹, assigned to OH and CH stretching vibrations, with more intense carboxylate bands in the pH 10 and 11 samples, consistent with higher glucuronic acid content. Thermogravimetric analysis showed that the weight-loss rate decreased as extraction pH increased, attributed to removal of low-molecular-weight compounds and formation of carboxylate salts, which enhanced thermal stability.

In water, the composites existed mainly as nanoparticles ranging from 200 to 250 nanometers, with all particles exhibiting negative zeta potentials. The pH 11 sample, labeled CPP-11, showed a significantly more negative charge than the others, attributed to its higher protein content. Contact angle measurements revealed that all particles were hydrophobic, with contact angles greater than 90°, and hydrophobicity increased with extraction pH, reflecting greater exposure of hydrophobic protein groups under strongly alkaline conditions. Dynamic interfacial tension measurements at air/water, fish oil/water, and soybean oil/water interfaces showed that the composites gradually adsorbed and rearranged to form stable interfacial layers, with the pH 11 sample forming interfaces more resistant to deformation.

Emulsifying performance was evaluated with soybean oil and fish oil emulsions. All composites stabilized emulsions with good physical stability, showing no significant changes in droplet size within seven days of storage. Increasing composite concentration gradually decreased emulsion droplet size, attributed to better interfacial tension reduction and formation of a thicker layer on droplet surfaces. Considering yield, surface charge, and storage stability collectively, the researchers selected CPP-11 for flavor-loading experiments with six commercial flavor products: menthol, vanilla bean flavor, vanillin, geraniol, cocoa flavor extract, and vanilla extract.

The six flavor emulsions, labeled D1 through D6, had particle sizes ranging from 560 to 645 nanometers. The cocoa flavor extract formulation, D5, showed excellent physical stability over the seven-day storage period, with particle size changing from 572.41 ± 98.45 to 477.62 ± 25.64 nanometers without statistical significance, and absolute zeta potential increasing from 30.05 ± 0.68 to 31.67 ± 0.25 mV. Scanning electron microscopy of the lyophilized powders revealed that the composite alone exhibited a sheet-like morphology with rough, heterogeneous surfaces, while the flavor-loaded powder showed a more compact, quasi-spherical morphology with smoother edges, indicating enhanced intermolecular interactions within the system.

Antioxidant activity after heating was striking. After thermal treatment at 80 °C, the composite-stabilized cocoa flavor formulation exhibited a DPPH radical-scavenging activity of 30.21 ± 0.55 percent, compared with 9.20 ± 0.57 percent for free cocoa flavor and 13.65 ± 0.19 percent for the composite alone. This substantially higher activity was not simply additive, suggesting the carrier system helps preserve functional properties during thermal processing.

Headspace solid-phase microextraction gas chromatography–mass spectrometry revealed that the nanoparticles themselves contained multiple volatile compounds, including 2-methoxy-4-vinylphenol, phenylethyl phenylacetate, cinnamaldehyde, 2,4-di-tert-butylphenol, and vanillin. The high abundance of vanillin may result from degradation of lignin in the coffee grounds. These compounds contribute smoky, spicy, warm cinnamon-like, floral, and honey-like aroma notes. The flavor-loaded formulation exhibited a more diverse volatile profile, combining intrinsic coffee-derived volatiles with compounds introduced by the cocoa extract. Storage temperature shifted the aroma profile: at 4 °C, 2-methoxy-4-vinylphenol dominated the composite, whereas vanillin increased at 45 °C, shifting from phenolic and smoky notes toward a sweeter, vanilla-like character.

Pyrolysis–gas chromatography–mass spectrometry at 200, 275, and 350 °C demonstrated the thermal resilience of the encapsulated flavors. At 200 °C, the flavor-loaded powder was dominated by vanillin at 68.67 percent and propylene glycol at 23.99 percent, indicating the encapsulated cocoa flavor compounds remained largely intact and were gradually released rather than degraded. The bare nanoparticles, by contrast, generated substantial carbon dioxide, methyl stearate, and methyl hexadecanoate, marking initial decomposition of polysaccharide and lipid components. At 275 °C, the bare composites showed characteristic carbohydrate pyrolysis products including levoglucosan at 52.57 percent, while the flavor-loaded powder still retained detectable vanillin at 47.77 percent and 2-phenylethyl phenylacetate, suggesting interactions between flavor molecules and the polysaccharide–protein matrix delayed thermal degradation. At 350 °C, vanillin decreased to 24.29 percent as extensive fragmentation and secondary reactions took over.

The findings highlight the potential of naturally occurring polysaccharide–protein composites as multifunctional delivery systems integrating structural support, flavor protection, and thermally triggered aroma release. Beyond cocoa flavor, the nanoparticles could serve as carriers for lipophilic flavor and aroma compounds in tobacco products, bakery and confectionery items, instant beverage powders, and other emulsion-based or thermally processed foods. The authors note that product-specific sensory properties, processing stability, safety, and regulatory compliance should be evaluated before practical application. More importantly, the work demonstrates how waste-derived materials can be transformed into functional ingredients, turning the residue of the world’s favorite beverage into a vehicle for the flavors of tomorrow.

Subject of Research: Food Chemistry

Article Title: Endogenous polysaccharide–protein composite nanoparticles prepared from spent coffee grounds as multi-flavor carriers

Article References: Endogenous polysaccharide–protein composite nanoparticles prepared from spent coffee grounds as multi-flavor carriers. (n.d.). https://doi.org/10.1016/j.fochx.2026.104636

Image Credits: AI Generated

DOI: 10.1016/j.fochx.2026.104636

Keywords: spent coffee grounds, nanoparticles, flavor encapsulation, Pickering emulsions, food waste valorization, pyrolysis, aroma release, Endogenous, polysaccharide, protein, composite, prepared