Upscaling cellulose oxidation: Integrating TEMPO-mediated oxidation in a pilot-plant twin-screw extruder for cellulose nanofibril production

(TEMPO)-mediated oxidation (TMO) is a widely recognized pretreatment for producing highly fibrillated cellulose nanofibrils (CNFs) because of its efficiency and selectivity. However, the challenges of scaling up this process is limiting its implementation. This study explores enhancing the production of oxidized pulps (OPs) by performing the TMO reaction within a pilot-plant twin-screw extruder (TSE). This approach aims to oxidize large volumes of cellulose at high concentrations while simultaneously applying a soft mechanical fibrillation, making the upscaling process more sustainable and feasible. OPs and CNFs were characterized and compared to those obtained from the traditional TMO pretreatment in a stirred reactor as well as those pretreated by mechanical TSE. Results demonstrate that TMO within the TSE is more efficient and increase the yield fibrillation using 0.8, 0.08 and 2 mmol/g pulp of NaBr, TEMPO and NaClO, respectively. Multiple TSE steps decrease polymerization degree, enhance the process yield, and reduce the number of large fibers. Gradual addition of oxidants in multiple TSE steps prevents harsh reaction conditions and avoids yellowing of the final products.