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Influence of Preparation Methods on the Catalytic Activity of Pd–Cu/Mn<sub>2</sub>O<sub>3</sub> Catalyst in the Hydrogenation of 1,3-Butadiene

By Tareque Odoom-Wubah (1760719), Qun Li (222962), Min Chen (147733), Huihuang Fang (5806601), Bernard Baffour Asare Bediako (6208865), Isroil Adilov (6208868), Jiale Huang (1595080) and Qingbiao Li (399550)

Abstract

Mn<sub>2</sub>O<sub>3</sub>-supported Pd–Cu catalysts synthesized by two biogenic methods, sol-immobilization (SI) and adsorption–reduction, are compared to catalysts prepared via three conventional methods, impregnation (IP), deposition–precipitation with urea (DPU), and deposition of colloids stabilized with poly­(vinylpyrrolidone) (DCPVP). The as-synthesized supported alloy catalysts of sizes between 2 and 8 nm were employed in the gas-phase selective hydrogenation of 1,3-butadiene. Their alloy nature was proved from characterizations including diffuse reflectance infrared Fourier transform spectroscopy and CO adsorption tests, temperature-programmed reduction, X-ray photoelectron spectroscopy, and X-ray diffraction. It was observed that the synthesis method greatly affects the final surface constituent of catalyst Pd/Cu ratio and partial particle reconstruction occurs under CO exposure. The optimum catalyst constituent of Pd–Cu<sub>0.06</sub>–Mn<sub>2</sub>O<sub>3</sub> was selected since it provided excellent conversion with poor selectivity to unwanted butane. Selectivity of all of the catalysts directly correlated with increasing Cu content and Pd-to-butadiene conversion. The bioreduction-supported catalysts using SI with a Pd/Cu atomic ratio of 0.9:1.4 showed excellent balances between butadiene conversion of 99.1% and selectivity to total butene above 92%, which we attribute to repulsion to H and its neighboring adsorbed inherent C and N atoms with adjacent Pd atoms and alloy synergy. The IPC catalyst showed the worst performance but was highly selective to butenes. And the DCPVP and DPU catalysts with 100% conversion produced worse 1-butene selectivity

Topics: Cell Biology, Physiology, Biotechnology, Evolutionary Biology, Science Policy, Environmental Sciences not elsewhere classified, Biological Sciences not elsewhere classified, Chemical Sciences not elsewhere classified, Information Systems not elsewhere classified, synthesis method, bioreduction-supported catalysts, alloy synergy, alloy nature, N atoms, Pd atoms, butadiene conversion, X-ray diffraction, CO exposure, alloy catalysts, catalyst constituent, DCPVP, Cu content, DPU catalysts, 8 nm, biogenic methods, Pd-to-butadiene conversion, SI, IPC catalyst, particle reconstruction, CO adsorption tests, Catalytic Activity, X-ray photoelectron spectroscopy, 1- butene selectivity, temperature-programmed reduction, Preparation Methods, surface constituent
Year: 2019
DOI identifier: 10.1021/acsomega.8b03216.s001
OAI identifier: oai:figshare.com:article/7590797
Provided by: FigShare
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