Cellulose foams are in high demand in an era of prioritizing environmental consciousness. Yet, transferring the exceptional mechanical properties of cellulose fibers into a cellulose network remains a significant challenge. To address this challenge, an innovative multiscale design is developed for producing cellulose foam with exceptional network integrity. Specifically, this design relies on a combination of physical cross-linking of the microfibrillated cellulose (MFC) networks by cellulose nanofibril (CNF) and aluminum ion (Al3+), as well as self-densification of the cellulose induced by ice-crystal templating, physical cross-linking, solvent exchange, and evaporation. The resultant cellulose foam demonstrates a low density of 40.7 mg cm-3, a high porosity of 97.3%, and a robust network with high compressive modulus of 1211.5 ± 60.6 kPa and energy absorption of 77.8 ± 1.9 kJ m-3. The introduction of CNF network and Al3+ cross-linking into foam also confers excellent wet stability and flame self-extinguish ability. Furthermore, the foam can be easily biodegraded in natural environments , re-entering the ecosystem's carbon cycle. This strategy yields a cellulose foam with a robust network and outstanding environmental durability, opening new possibilities for the advancement of high-performance foam materials.
Keywords: air drying, cellulose, cross–linkings, fibrillation, foams.
© 2023 The Authors. Small published by Wiley‐VCH GmbH.