Sustainable valorization of paper mill sludge into cellulose nanofibrils and cellulose nanopaper

As a kind of agro-industrial wastes, paper mill sludge (PMS) has posed serious environmental and economic challenges for disposal due to the more stringent regulations and diminishing land availability in recent years. The present study is aimed at providing a sustainable approach to efficiently convert PMS to cellulose nanofibrils (CNFs) and cellulose nanopaper (CNP) by formic acid (FA) hydrolysis pretreatment and the followed microfluidization. It is found that FA hydrolysis (4–6 h) could swell and shorten PMS fibers, and only two-pass microfluidization is sufficient to get uniform CNFs from the collected cellulose residual. Results indicate that the obtained CNFs show high thermal stability and crystallinity index, surface functionality (ester groups), as well as a high yield of over 75 wt.%. Notably, more than 90 % FA can be recovered and the hydrolyzed sugars could be potentially used to produce platform chemicals (e.g. lactic acid, furfural). Finally, transparent CNP is prepared from the CNFs suspension via a simple vacuum filtration technique. The resultant CNP shows good mechanical properties with the maximum tensile strength and toughness of 106.4 MPa and 6.62 MJ/m3, respectively. Therefore, the current work provides a green and sustainable method to valorize PMS for the production of valuable CNFs and CNP.