A mixture of the Ch-CNC suspension and latex NPs was emulsified in the flow-focusing microfluidic droplet generator (fig.S2) (40) using a syringe pump (Harvard Apparatus PHD 2000 Syringe Pump, USA). A mixture of 50 μl of NP dispersion with NP concentration from 1.1 × 10−3 to 1.19 × 10−1 and 450 μl of the Ch-CNC phase was prepared by shaking at 50 Hz for 2 min at 25°C in a vortex mixer and immediately supplied to the microfluidic droplet generator as a droplet phase. Fluorinated oil HFE-7500 mixed with 0.5 wt % of the copolymer surfactant (denoted as F-oil) was supplied to the microfluidic device as a continuous phase by using the second syringe pump (PHD 2000 Harvard Apparatus, USA). The flow rate of F-oil and the Ch-CNC/NP mixture were 0.2 and 0.02 ml/hour, respectively. The droplets were collected in a 2-ml vial and transferred into a cell consisting of two parallel glass slides separated with a 400-μm-thick spacer. The cell was sealed with epoxy glue, and the droplets were equilibrated for 3 days.

The procedure of the generation of the NP-free Ch-CNC droplets was similar to the protocol of the preparation of the Ch-CNC/NP droplets. Deionized water (50 μl) was added to 450 μl of the Ch-CNC phase to achieve the same concentration of CNCs in both cases. The suspension was mixed at 50 Hz for 2 min at 25°C in a vortex mixer and, subsequently, emulsified in the microfluidic device.

The method of preparation of Ch-CNC droplets loaded with magnetic NPs is similar to the procedure of generation of the Ch-CNC droplets loaded with latex NPs. Instead of using latex NPs, a mixture of 50 μl of magnetic NP dispersion with NP volume fraction from 9.7 × 10−3 to 1.9 × 10−2 and 450 μl of the Ch-CNC phase was prepared by shaking at 50 Hz for 2 min at 25°C in a vortex mixer and immediately supplied to the microfluidic droplet generator as a droplet phase.

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