Department of Chemistry and Chemical Biology, Harvard University, Cambridge, MA 02138,
Department of Chemical and Biomolecular Engineering, University of California, Los Angeles, CA 90095,, Department of Chemistry and Biochemistry, University of California, Los Angeles, CA 90095,
Department of Chemistry, Tufts University, Medford, MA 02155,
John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138,
Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, NY 11973-5000
Department of Chemistry and Chemical Biology, Harvard University, Cambridge, MA 02138,, John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138,
The energy efficiency of catalytic processes hinges on achieving high selectivity and activity; bimetallic catalysts have potential to increase both by exploiting different chemical properties of the components. Transport of intermediates between the two metals, for example, transport of hydrogen atoms for selective hydrogenation, is required to capitalize on this bifunctionality. A mechanism for the migration of hydrogen atoms to silver from palladium is demonstrated here. Dihydrogen first dissociates on palladium, then forms a dense hydrogen phase on the palladium island. The dense phase includes weakly bound hydrogen atoms that are nearly isoenergetic with hydrogen on silver, rendering migration nearly energy neutral. The efficiency for hydrogen migration across the palladium−silver is maximized for small ensembles of palladium atoms.
O’Connor, Christopher R., et al. "Facilitating hydrogen atom migration via a dense phase on palladium islands to a surrounding silver surface." Proceedings of the National Academy of Sciences of the United States of America, vol. 117, no. 37, Sep. 2020. https://doi.org/10.1073/pnas.2010413117
O’Connor, Christopher R., Duanmu, Kaining, Patel, Dipna A., Muramoto, Eri, van Spronsen, Matthijs A., Stacchiola, Dario, Sykes, E. Charles H., Sautet, Philippe, Madix, Robert J., & Friend, Cynthia M. (2020). Facilitating hydrogen atom migration via a dense phase on palladium islands to a surrounding silver surface. Proceedings of the National Academy of Sciences of the United States of America, 117(37). https://doi.org/10.1073/pnas.2010413117
O’Connor, Christopher R., Duanmu, Kaining, Patel, Dipna A., et al., "Facilitating hydrogen atom migration via a dense phase on palladium islands to a surrounding silver surface," Proceedings of the National Academy of Sciences of the United States of America 117, no. 37 (2020), https://doi.org/10.1073/pnas.2010413117
@article{osti_1657616,
author = {O’Connor, Christopher R. and Duanmu, Kaining and Patel, Dipna A. and Muramoto, Eri and van Spronsen, Matthijs A. and Stacchiola, Dario and Sykes, E. Charles H. and Sautet, Philippe and Madix, Robert J. and Friend, Cynthia M.},
title = {Facilitating hydrogen atom migration via a dense phase on palladium islands to a surrounding silver surface},
annote = {Significance The energy efficiency of catalytic processes hinges on achieving high selectivity and activity; bimetallic catalysts have potential to increase both by exploiting different chemical properties of the components. Transport of intermediates between the two metals, for example, transport of hydrogen atoms for selective hydrogenation, is required to capitalize on this bifunctionality. A mechanism for the migration of hydrogen atoms to silver from palladium is demonstrated here. Dihydrogen first dissociates on palladium, then forms a dense hydrogen phase on the palladium island. The dense phase includes weakly bound hydrogen atoms that are nearly isoenergetic with hydrogen on silver, rendering migration nearly energy neutral. The efficiency for hydrogen migration across the palladium−silver is maximized for small ensembles of palladium atoms.},
doi = {10.1073/pnas.2010413117},
url = {https://www.osti.gov/biblio/1657616},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
issn = {ISSN 0027-8424},
number = {37},
volume = {117},
place = {United States},
publisher = {Proceedings of the National Academy of Sciences},
year = {2020},
month = {09}}
Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Issue: 37 Vol. 117; ISSN 0027-8424