Additive manufacturing (3D printing) is playing an increasingly
significant role in the processing and application of advanced materials by
enabling the fabrication of geometrically complex structures. However, to
expand the possibilities in materials design, it is essential to regulate the
alignment of building blocks from the macroscopic scale to the molecular
scale. 3D-printed Cellulose-Metal Organic Frameworks hybrids (CelloMOFs) have
become promising materials in many applications. Hybrid materials composed of
TEMPO-oxidized cellulose nanofibers (TCNFs) and nanocrystals (TCNCs),
combined with two MOFs ; ZIF-8 and SU-101 which were synthesized in situ
within the cellulose matrices were investigated during 3D printing using
synchrotron small angle X ray scattering (SAXS) at ForMAX beamline. The
results indicated that all the systems are anisotropic and had preferred
orientation along the printing direction irrespective of the printing speed
(30 mm/s and 60 mm/s). The TCNF and TCNCs without MOFs have higher degree of
orientation when compared to their MOFs incorporated counterparts at all
speeds. Surprisingly, despite the rod shape of SU-101, ZIF-8-containing inks
exhibited higher extent of anisotropy, which will need further analyzis.
These results demonstrate the intricate relationship between MOF structure
and nanocellulose alignment in printed composites and provide valuable
details for creating anisotropic functional material architectures.

Acknowledgement : The authors acknowledge funding from the PRISMAS
programme and the European Union. We also extend our thanks to all
collaborators, including Mika Sipponen and his team, Lennart Bergström and
his team, and Houssine Khalili.