![]() The differences between these solvent structure motifs provide opportunities to manipulate enthalpy–entropy compensation relationships and greatly increase the rates of catalysis. Here, we show by spectroscopic measurements and molecular dynamics simulations that H2O molecules form bulk-like three-dimensional structures within 1.3 nm cages, whereas H2O molecules coalesce into oligomeric one-dimensional chains when the pore diameter falls below 0.65 nm. Within zeolite pores, H2O molecules form hydrogen-bonded structures that differ substantially from bulk H2O. ![]() Solvent structures that surround active sites reorganize during catalysis and influence the stability of surface intermediates.
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