%0 Journal Article 
%A Ballesteros Soberanas, Jordi
%A Martín, Nuria
%A Bacic, Matea
%A Tiburcio, Estefanía
%A Mon, Marta
%A Hernández Garrido, Juan Carlos
%A Marini, Carlo
%A Boronat, Mercedes
%A Ferrando Soria, Jesús
%A Armentano, Donatella
%A Pardo, Emilio
%A Leyva Pérez, Antonio
%T A MOF-supported Pd1–Au1 dimer catalyses the semihydrogenation reaction of acetylene in ethylene with a nearly barrierless activation energy
%D 2024
%@ 2520-1158
%U http://hdl.handle.net/10498/33694
%X The removal of acetylene from ethylene streams is key in industry for
manufacturing polyethylene. Here we show that a well-defned Pd1–Au1
dimer, anchored to the walls of a metal–organic framework (MOF), catalyses
the selective semihydrogenation of acetylene to ethylene with ≥99.99%
conversion (≤1 ppm of acetylene) and >90% selectivity in extremely rich
ethylene streams (1% acetylene, 89% ethylene, 10% H2, simulated industrial
front-end reaction conditions). The reaction proceeds with an apparent
activation energy of ∼1 kcal mol–1, working even at 35 °C, and with
operational windows (>100 °C) and weight hourly space velocities
(66,000 ml g−1
cat h−1
) within industrial specifcations. A combined
experimental and computational mechanistic study shows the cooperativity
between both atoms, and between atoms and support, to enable the
barrierless semihydrogenation of acetylene.
%~ Universidad de Cádiz