Abstract
The removal of acetylene from ethylene streams is key in industry for manufacturing polyethylene. Here we show that a well-defined 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 (66,000mlgcat−1h−1\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$66{,}000\\,{\\mathrm{ml}}\\,{\\mathrm{g}}^{-1}_{\\mathrm{cat}}\\,{\\mathrm{h}}^{-1}$$\\end{document}) within industrial specifications. 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.
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