Garbage to Nanocellulose: Quantitative Isolation and Characterization of Steam-Treated Carboxymethyl Holocellulose Nanofibrils from Municipal Solid Waste

Municipal solid waste (MSW) is a major source of greenhouse gas emissions unless its carbons are sequestered into highervalue products. This study focuses on isolating organic solids and cellulose-rich fibers from MSW via high-pressure steam treatment and converting the fibrous, prepulped materials from wastepaper, packaging materials, cardboard, etc., into value-added cellulose nanofibrils. Chemical-mechanical defibrillation of steam-treated municipal solid waste was optimized using heterogeneous and nonregioselective carboxymethyl etherification coupled with shearing by blender, thus transforming a heterogeneous mix of MSW into homogeneous carboxymethyl holocellulose nanofibrils without the use of conventional pretreatments of crude cellulosic feedstock. These carboxymethylated, hemicellulose-coated, cellulose nanofibrils were isolated quantitatively at >95% yield with widths 3-8 nm, thicknesses 1-3 nm, and lengths up to 1000 nm. We posit that this advancement of combining an inexhaustible, global supply of waste cellulose, large-scale steam autoclaving pretreatment, and an industrially relevant carboxymethylation process could unlock the higher potential of sustainable cellulosic nanomaterials for a circular economy.