Wear and Friction Behavior of Cellulose Nanofibers-Based Biogreases

(1) Background: Developing fully bio-based lubricating greases requires eco-friendly alternatives to conventional harmful components. This study highlights unmodified nanocellulose as an effective structuring agent in vegetable oils, enabling 100% bio-based formulations. (2) Methods: Three bio-based greases were formulated using 1.4 wt.% cellulose nanofibers (CNFs), derived from elm wood pulp through mechanical and chemical pretreatment, as thickening agents in castor oil. Their tribological performance was evaluated under varying temperatures and contact loads and compared to a reference lithium-based grease (LBG) containing 14 wt.% thickener, also formulated with castor oil. (3) Results: Among the CNFs, the unbleached variant (CNF-U) which retained the highest lignin content exhibited the highest coefficient of friction (COF), ranging from 0.09 to 0.14 across test conditions, along with a wear scar diameter of approximately 615 µm at 60 °C. Notable differences in shear stress sensitivity were observed between mechanically and chemically treated nanofibers. The TEMPO-oxidized nanofiber (CNF-TO) grease demonstrated outstanding lubrication stability across contact loads of 10–40 N and temperatures from 25 to 100 °C, maintaining COF values below 0.1—comparable to the reference LBG at 40 N load. Wear scar analysis confirmed that CNF-based greases significantly reduced wear relative to the lithium reference: CNF-B produced the smallest scar diameter (188 µm at 25 °C) while CNF-TO yielded the lowest at 60 °C (457 µm). (4) Conclusions: Nanofiber type and pretreatment significantly impact the tribological performance of CNF-based biogreases. TEMPO-oxidized CNFs provided stable lubrication under varied loads and temperatures, while all CNFs showed strong thermal adaptability, supporting their use in sustainable lubrication.