Automated spin-assisted layer-by-layer epitaxy produces highly oriented mixed-linker MOF thin filmsAfanasenko, Eleonora (Avtor) Marmiroli, Benedetta (Avtor) Asbaghi, Behnaz Abbasgholi Nejad (Avtor) Sartori, Barbara (Avtor) Birarda, Giovanni (Avtor) Stani, Chiaramaria (Avtor) Finšgar, Matjaž (Avtor) Hartmann, Peter E. (Avtor) Bieber, Mark (Avtor) Walitsch, Emma (Avtor) Breinbauer, Rolf (Avtor) Dal Zilio, Simone (Avtor) Klokic, Sumea (Avtor) Amentisch, Heinz (Avtor) crystal growthliquid phase epitaxymetal-organic frameworksorientation controlthin filmsControl over crystallographic orientation in metal-organic framework (MOF) thin films is crucial for exploiting their anisotropicproperties in sensing, catalysis, and separation. Achieving reproducible, highly oriented films remains challenging, especially formixed-linker, pillared-layered frameworks. Here we present an automated, spin-assisted layer-by-layer liquid-phase epitaxy (LbL-LPE) strategy that enables rapid, ambient-condition fabrication of highly oriented, mixed-linker MOF thin films, demonstratedfor Zn 2 BDC2 DABCO (BDC = terephthalate, DABCO = 1,4-diazabicyclo[2.2.2]octane). Correlative process monitoring bygrazing-incidence wide-angle x-ray scattering (GIWAXS), grazing-angle infrared (GI-IR) and UV-Vis spectroscopy, contact-angle measurements, scanning electron microscopy (SEM), and time-of-flight secondary ion mass spectrometry (ToF-SIMS)ensures formation of uniform films with exceptional out-of-plane (001) orientation (degree of orientation > 85%, Hermansorientation parameter ∼0.95) and excellent reproducibility. This strategy enables high-throughput fabrication of orientation-controlled MOF thin films, providing a generalizable alternative to conventional LbL approaches. The resulting highly orientedZn 2 (BDC) 2 (DABCO) thin films retain their crystallinity after prolonged exposure to 80% and short-term exposure up to 90% relativehumidity, whereas defect-rich films undergo rapid degradation. Thus, this reproducible, automated strategy establishes the roleof crystallographic orientation in humidity stability and advances the integration of oriented MOFs into optoelectronic, sensing,and membrane devices.Wiley20262026-09-16 10:14:19Članek v reviji100389UDK: 54COBISS_ID: 291038723DOI: 10.1002/anie.3901165ISSN pri članku: 1521-3773sl©2026TheAuthor(s)