M 110eh

TEMPO-oxidized cellulose nanofibrils were prepared using TEMPO-mediated oxidation of dissolving grade pulp at neutral conditions based on a previously published procedure [50 (link)], which is an adaptation from the procedure first reported by Saito et al. [51 (link)]. A full description of the procedure can be found in the supporting information. The fibrils were subsequently liberated from the fibers by high pressure homogenization using a microfluidizer (M-110EH, Microfluidics Corp, Red Bank, NJ, USA). The colloidally stable CNFs dispersions were then prepared according to previously described procedure [52 (link)].

Never-dried tunicate cellulose was firstly subjected to disintegration (Frank-PTI GmbH, Germany) for 10 min (30,000 revolutions). Then the pretreated cellulose was mechanically disintegrated through high pressure homogenization by using a Microfluidizer (M-110EH, Microfluidics Corp., Westwood, MA, USA) at 10 g/L using two large chambers in series (400 and 200 µm, respectively) at 925 bar for the first pass and smaller chambers (200 and 100 µm, respectively) at 1600 bar for five passes. The obtained CNF dispersed in water were diluted to 0.5% in weight for further use.

Pulps were dried overnight
at 50 °C and milled through a 2 mm sieve using a Thomas model
4 Wiley Mill. Hydrolyses were conducted for 30 min at 55 °C using
either 58 or 64 wt % sulfuric acid. An additional 64 wt % sulfuric
acid hydrolysis for 45 min at 45 °C was performed on cotton (Whatman
Filter Aids, referred to as COT). All hydrolyses used a ratio of 40
g of o.d. cellulose to 17.5 mL of acid. Reactions were quenched by
their addition to chilled water at 10-fold volume and then allowed
to settle, with the upper clear phase discarded and the lower phase
collected and rinsed by centrifugation (10 min cycles, 3600g). Next, the collected material was dialyzed extensively
until a constant suspension pH was reached and homogenized by 1 pass
through a microfluidizer at 1700 bar (M110-EH, Microfluidics). After
microfluidization, the yield of the material was determined from the
solid content (gravimetric concentration in wt %) and the total amount
of material that was collected.

E(AH) compounds were generated using the thin-film hydration method. L-α-Phosphatidylcholine (Sigma-Aldrich), TEGO Care CG 90 surfactant (Evonik Industries AG, Germany), and AH compounds were added to 20 ml ethanol (Duksan Co.). We used a rotary evaporator (RE100-Pro, DLAB, China) to completely remove ethanol and form a lipid membrane on the flask wall. The lipid membrane was hydrated in 20 mL 5% ethanol and used as an elastic ethosome. After homogenization to produce a particle with a consistent size using a microfluidizer (M110EH, Microfluidics, USA), the unloaded components were removed using a 0.45 μM syringe filter (Advantec, Japan) and ethosomes were stirred overnight at 4°C for stabilization.

Thaumatin was purchased from Penta Manufacturing (New Jersey, USA). The printable ink was prepared by reconstituting thaumatin in Evian water (Evian, Cachat, France) at different concentrations, corresponding to ink formulations with variable sweetness potencies, detailed in Table 1. The solution was stirred with a magnetic stirrer at 600 rpm for one hour (Ika Yellowline MST basic c, Staufen im Breisgau, Germany). Caprylic capric triglycerides (CCT) (Mibelle Group, Buchs, Switzerland, Lot 10339) and polyglycerol poly-crinoleate (PGPR) (Danisco, Rotterdam, Netherlands) were added to the aqueous solution and were mixed with a Polytron mixer at 3000 rpm for two minutes (Kinematica GmbH, Kriens Luzern, Switzerland). The premix was transferred to a Microfluidizer processor (M-110EH Microfluidics, Newton MA, USA), where the mix was emulsified for six cycles at 1000 bar to form a W/O emulsion. Seeded cocoa butter was manufactured in a SeedMaster (SeedMas- ter cryst, Bu¨hler AG, Switzerland) for 150 min (see details in^{41 (link)}) and was added to the emulsion at a weight ratio of 9:1. The ink (short for print- able ink mass) was carefully stirred for three minutes and either transferred to a preheated cartridge at 33.0 ± 0.1 °C or stored for rheology and calorimetric analysis, as detailed in the following subchapters.