Measuring and Modulating Substrate Confinement during Nitrogen-Atom Transfer in a Ru2-Based Metal-Organic Framework

We demonstrate that significant substrate confinement within a microporous Ru₂-based MOF can be rationally tuned by modulating network mesoporosity. The reported data provide the first demonstration of tunneling during interstitial MOF chemistry and illustrate an experimental strategy to evaluate the impact of material structure on substrate mobility in porous catalysts.