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Lee, et al.
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           Figure 1. An overview of the formulation of coconut cream inks added with coconut oil, and results from oil separation test. (A) Coconut
           cream base was initially formulated by mixing coconut cream powder with different water concentrations (20, 25, and 33%) and fixed
           concentration of pandan extract at 0.2%. Next, different weight concentrations of coconut oil (% w/w, with respect to the weight of the
           coconut cream base) were added to the coconut cream base to observe the occurrence of the oil separation. (B) A plot showing oil separation
           ratio as a function of oil concentration. (C) A diagram showing inks that exhibited or did not exhibit oil separation at different oil and water
           content.

           expected, the oil separation ratio increased as the amount   4.2. Rheological characterization of coconut
           of oil separated increased (Figure  1B). Oil separation   cream ink
           occurred in inks containing 20% (w/w) water content with
           additional oil content >5% (w/w), inks containing 25%   Next, we studied the rheological properties of the inks.
           (w/w) water content with the additional oil content >10%   Rheological properties such as yield stress and storage
           (w/w), and inks containing 33% (w/w) water content with   modulus (G’) are important to determine the printability
                                                                    [42]
           the additional oil content >15% (w/w) (Figure 1B). As   of ink .  The yield  stress of the ink is the minimum
           the water content increased from 20% to 33% (w/w), the   shear stress needed to initiate flow in DIW 3D printing.
           tendency for oil separation to occur decreased. The oil   G’ is a measure of mechanical strength at rest condition
           separation ratio increased from 0.10 (10% w/w oil) to   which determines the structural integrity of the printed
           0.80 (30% w/w oil) for inks containing 20% water, 0.01   material after deposition. The rheological properties were
           (12.5% w/w oil) to 0.50 (30% w/w oil) for inks containing   determined using the same method described in previous
                                                                   [23]
           25% water, and 0.01 (20% w/w oil) to 0.35 (30% w/w   work .  All  inks  displayed  shear  thinning  property,
                                                                                                              0
                                                                                                        3
           oil) for inks containing 33% water. As expected, the oil   where the viscosity decreased from an order of 10  to 10
                                                                                                             −1
           separation became prominent at high concentrations of   Pa·s with increasing shear rates between 0.01 and 100 s
           the oil. With the increase in water content, the amount   (Figure 2A). Shear-thinning properties are desirable for
           of dispersed water also increased  which allowed the   the extrusion of ink from the nozzle on applied pressure.
                                        [41]
           emulsifier to achieve continuous interface between water   The increase  in water content  from 25 to 33% (w/w)
           and oil without phase separation. However, the increased   resulted  in a reduced  viscosity due to the weakened
           water content decreased the viscosity of the overall ink,   colloidal network caused by lower ratios of emulsifier.
           which would affect the 3D printability of inks. Overall,   Similarly, the increase in the oil content from 10 to 12.5%
           we  selected  three  samples  (Ink A  contains  25%  water   (w/w) led to a decreased viscosity. We also observed mild
           with  10%  (w/w) oil,  Ink  B  contains  25%  water  with   oil separation in Ink B presumably due to the weakened
           12.5% (w/w) oil, and Ink C contains 33% water with   colloidal network within the ink.
           10% oil (w/w)) for the characterization of the rheological   The previous studies have suggested that the inks
           properties to ensure the 3D printability by cold extrusion.   with  the  yield  stress of 106–330 Pa and  the  storage

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