LAUSR

As a result of the increasing gap between the supply and demand of butadiene, the catalytic coupling of ethanol has regained the attention of the scientific and industrial community as an “on‐purpose” production route to butadiene. The most promising systems are based on bifunctional catalysts that comprise metal sites that can dehydrogenate ethanol to acetaldehyde and Lewis acid sites that catalyze the aldol condensation between two aldehyde molecules and the Meerwein–Ponndorf–Verley reduction of the intermediate crotonaldehyde. Here, we investigate the role of Ag in an established Ag‐Zr‐BEA catalyst using modulated operando diffuse reflectance infrared Fourier transform spectroscopy and mass spectrometry experiments. We obtain insights into the complex reaction network that involves several consecutive and parallel reactions. Based on our investigations, we formulate suggestions for catalyst optimization.