Towards a Synergy‐Driven Design Paradigm for Metal‐Organic Framework/Polymer Nanocomposites via Predictive Multiscale Simulations

Experimental reports indicate that embedding metal-organic frameworks (MOFs) in polymer matrices both facilitates practical engineering applications and may yield properties surpassing the rule-of-mixtures expectations owing to interfacial synergy. Herein, computational methods are used to predict this amplification a priori, opening the door to in-silico synergy-driven design paradigm. Thermal conductivity is chosen as the model property, important because heat management governs adsorption-driven separations employing MOFs. Non-equilibrium molecular dynamics provides conductivities for the MOF, the polymer, and the interphase; a multiscale scheme then delivers the composite value. The workflow is applied to HKUST-1/polyethylene glycol(PEG) and UiO-66/PEG and benchmarked against ZIF-8/stearic acid(SA). For HKUST-1/PEG a conductivity of 0.39 W/mK is predicted, representing a 0.09 W/mK synergy above the rule-of-mixtures baseline; experimental measurements report, respectively, 0.428 and 0.14 W/mK, confirming the model predictions. UiO-66/PEG model and its experimental analogue UiO-66(CH3)/PEG display comparable agreement and, notably, outperform both bulk constituents. In contrast, ZIF-8/SA exhibits no significant enhancement. The demonstrated predictive route identifies MOF/polymer pairs with favorable thermal transport and guides rational design of advanced adsorbent composites.