Mechanical Stability and Binder Interaction in MOF Composites: An Integrated Experimental and DFT Study

An integrated study combining experimental methods and DFT simulations was undertaken to investigate the binder/MOF composites. The findings demonstrate a strong correlation between the crush strength and surface adsorption energy of methylcellulose (MC) on HKUST, ZIF-8, UiO-66-(Zr), and MIL-53-(Al)-TDC surfaces. Experimental thermogravimetric data and compressive strength measurements, combined with simulated adsorption energies, bond distances, and charge distributions, supported this relationship. DFT calculations of adsorption energy and structural analysis showed that MC/HKUST and MC/ZIF-8 composites exhibit stronger interactions with MC, consistent with their higher mechanical strength at higher temperatures. In contrast, MC/UiO-66-(Zr) and MC/MIL-53-(Al)-TDC presented weaker interactions and lower resistance under thermal stress. This study demonstrates that computational methods, when integrated with experimental techniques, can offer valuable insights into the design of mechanically stable binder/MOF composites.