The potential of TEMPO (2,2,6,6-tetramethyl-1-piperidinyloxy)-mediated oxidation (TMO) to produce cellulose nanofibrils (CNFs) is hindered using costly and environmentally harmful catalysts, limiting its large-scale implementation. To promote sustainability, the TMO medium should be reused but there is a lack of knowledge on this process. The novelty of this research is the identification of the key parameters that affect the recirculation of the TMO medium, and their impact on the quality of the oxidized pulps and CNF products. Contrary to previous hypothesis, results show that the accumulation of salts is not a key parameter; instead, the pulp consistency during oxidation plays a vital role since concentrations higher than 10 g/L led to better CNF quality. Thus, reusing 75 % of the reaction medium, when high pulp consistency is used, does not alter the CNF properties. By reusing the reaction medium up to six times, the catalyst dose is dramatically reduced by >90 % for TEMPO and 80 % for NaBr, compared to the conventional process (0.1 mmol of TEMPO/g and 1 mmol of NaBr/g without medium reuse). Additionally, the high consistency oxidation enables a reduction of >80 % in the reaction time and effluent, and thus a threefold increase in CNF production.
Keywords: Catalyst reusing; Cellulose nanofibers; Circular economy; Nanocellulose; TEMPO; TEMPO-mediated oxidation.
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