Demand for biodiesel has increased due to being a more environmentally‐friendly fuel. Cold weather operation of biodiesel is challenging due to fatty acid methyl ester (FAME) content in biodiesel. Saturated FAMEs crystallize at relatively high temperatures, increase the viscosity of biodiesel, and can clog fuel lines. Here, several factors altered crystallization temperature (CT) of FAMEs, including composition, shear rate, and cooling rate. The crystallization of pure and binary mixtures of methyl palmitate, methyl myristate, and methyl stearate were studied under shear flow and static conditions. Static phase CTs of pure methyl palmitate, methyl myristate, and methyl stearate were 26, 14, and 35°C, respectively. In binary mixtures, CTs were depressed up to 7°C, which agreed with freezing point depression theory. Increasing shear rate up to 100 s−1 decreased CT by 2°C compared to static conditions. Decreasing cooling rate from 1 to 0.1°C/min increased CT less than 2°C. Overall, FAME composition altered CT more than shear flow or cooling rate for pure and binary mixtures of three FAMEs.
Complex coacervates formed through the association of charged polymers with oppositely charged species are often investigated for controlled release applications and can provide highly sustained (multi-day, -week or -month) release of both small-molecule and macromolecular actives. This release, however, can sometimes be too slow to deliver the active molecules in the doses needed to achieve the desired effect. Here, we explore how the slow release of small molecules from coacervate matrices can be accelerated through mechanical stimulation. Using coacervates formed through the association of poly(allylamine hydrochloride) (PAH) with pentavalent tripolyphosphate (TPP) ions and Rhodamine B dye as the model coacervate and payload, we demonstrate that slow payload release from complex coacervates can be accelerated severalfold through mechanical stimulation (akin to flavor release from a chewed piece of gum). The stimulation leading to this effect can be readily achieved through either perforation (with needles) or compression of the coacervates and, besides accelerating the release, can result in a deswelling of the coacervate phases. The mechanical activation effect evidently reflects the rupture and collapse of solvent-filled pores, which form due to osmotic swelling of the solute-charged coacervate pellets and is most pronounced in release media that favor swelling. This stimulation effect is therefore strong in deionized water (where the swelling is substantial) and only subtle and shorter-lived in phosphate buffered saline (where the PAH/TPP coacervate swelling is inhibited). Taken together, these findings suggest that mechanical activation could be useful in extending the complex coacervate matrix efficacy in highly sustained release applications where the slowly releasing coacervate-based sustained release vehicles undergo significant osmotic swelling.
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