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PdCu Single Atom Alloys for the Selective Oxidation of Methanol to Methyl Formate at Low Temperatures

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Abstract

The selective catalytic oxidation of methanol to methyl formate (MF) has been considered as an attractive route to produce MF, an important precursor in the chemical industry. Although supported Pd nanoparticles are active for the selective oxidation of methanol to MF, the relatively low MF selectivity and yield remains an unsolved issue. Herein, we show that adding a small amount of Pd into Cu forming PdCu single atom alloy (SAA) catalysts can catalyze the oxidation of methanol to MF selectively at low temperatures, with a high catalyst stability. The atomic dispersion of Pd atoms in the Cu matrix was confirmed by various in-situ characterization techniques. The activity and selectivity of PdCu SAA catalysts were compared to monometallic Cu and Pd catalysts, in a flow reactor at similar conditions. This work may guide the design of new SAA based catalysts for selective oxidation reactions.

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Acknowledgements

This work was supported as part of the Integrated Mesoscale Architectures for Sustainable Catalysis, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under award #DESC0012573. The XAS research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science, User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357.

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Authors and Affiliations

  1. Department of Chemical and Biological Engineering, Tufts University, Medford, MA, 02155, USA

    Junjun Shan, Georgios Giannakakis, Jilei Liu, Sufeng Cao, Mengyao Ouyang, Mengwei Li & Maria Flytzani-Stephanopoulos

  2. NICE America Research, Inc., Mountain View, CA, 94043, USA

    Junjun Shan

  3. X-ray Science Division, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, IL, 60439, USA

    Sungsik Lee

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  1. Junjun Shan
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Correspondence to Junjun Shan.

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Shan, J., Giannakakis, G., Liu, J. et al. PdCu Single Atom Alloys for the Selective Oxidation of Methanol to Methyl Formate at Low Temperatures. Top Catal 63, 618–627 (2020). https://doi.org/10.1007/s11244-020-01288-x

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