In
recent years, stable hydrogen-bonded stimuli-responsive polymer
capsules have been receiving great interest for the encapsulation
and release of sensitive molecules such as lipase enzymes. Compartmental
capsules having a liquid gel core stabilized with temperature-responsive
hydrogen-bonded multilayers are advantageous over other conventional
systems because of their ability to maintain hydrophilic lipase and
other hydrophobic compounds in compatible protected molecular vehicle
environments and prolong their native properties, e.g., in the body.
In this work, we report a methodology to stabilize an aqueous liquid
gellan gum (GG) core in a capsule using neutral and nontoxic building
blocks, namely, poly(2-n-propyl-2-oxazoline) (PnPrOx) and tannic acid (TA), to fabricate temperature-responsive
capsules, comprising both lipase and hydrophobic oil droplets. The
capsules were fabricated by adding GG droplets to a PnPrOx suspension at a temperature (T) higher than
its cloud point temperature (T
CP). Notably,
the formed capsules were not stable in water without TA stabilization
via hydrogen bonding. Scanning electron microscopy (SEM) investigations
of the GG/building block interphase revealed that the collapsed PnPrOx globules that are present above the T
CP stabilized the GG interphase as a Pickering emulsion,
while undergoing a configurational transformation into its linear
form by interacting with TA in the next step of capsule formation
resulting in a smooth PnPrOx/TA capsule wall. The
encapsulation efficiencies of the capsules for model fluorescent molecules
were found to be 52, 54, and 24% for FITC-dextran, rhodamine, and
Nile red, respectively. The stability experiments exhibited swelling
and shell thinning at certain locations followed by complete rupture
of the capsules at 37 °C, while the capsules were stable for
several weeks at temperatures below the T
CP of PnPrOx. The capsules were found to be stable
in stimulated gastric fluid (SGF) for several hours at 37 °C
while successfully releasing the encapsulated lipase and Nile red
(model hydrophobic compound) in stimulated intestinal fluid (SIF).
The released lipase was found to retain almost 100% of its activity.
The reported capsules have high potential for use as carriers for
encapsulation and release of a variety of payloads ranging from proteins
and vitamin supplements to enzymes and probiotics through the oral
route of administration.