Modulation of surface properties of cellulose nanocrystals through adsorption of tannic acid and alkyl cellulose derivatives

Cellulose nanocrystals (CNCs) are hydrophilic nanoparticles that cannot be dispersed in non-polar solvents or hydrophobic polymer matrices. Here, we demonstrate the tunable modification of CNC surfaces by physical adsorption of tannic acid (TA) and two alkyl cellulose derivatives (ACDs), methyl cellulose (MC) and ethyl cellulose (EC), while maintaining their sustainable nature. We compare the impact of ACD adsorption when mixed with CNCs to CNCs precoated with tannic acid (CNC@TA), varying ACD weight fractions in CNC suspensions. Our results show that CNC@ACD and CNC@TA@ACD aqueous suspensions display good colloidal stability in water, while their surface properties are altered. We use a wide range of analytical techniques to characterize these suspensions, with a focus on their interaction with water. The two selected ACDs adsorb on both CNCs and CNC@TA at low fractions (ACD ≤ 10 % w/w), followed by an intermediate region of saturation between 10 % and 30 % w/w. At fractions above 30 % w/w, we observe the formation of CNC- or CNC@TA-reinforced ACD composites. Most samples can be redispersed in water upon freeze-drying, except for EC-rich samples redispersible in toluene. Our facile method for preparing ACD-coated CNCs allows for the creation of a range of nanomaterials with modulable wetting and emulsification properties.