Thermal Unequilibrium of PdSn Intermetallic Nanocatalysts: From In Situ Tailored Synthesis to Unexpected Hydrogenation Selectivity

dc.contributor.author Chen, Minda
dc.contributor.author Yan, Yu
dc.contributor.author Gebre, Mebatsion
dc.contributor.author Huang, Wenyu
dc.contributor.author Ordonez, Claudio
dc.contributor.author Liu, Fudong
dc.contributor.author Qi, Long
dc.contributor.author Lamkins, Andrew
dc.contributor.author Jing, Dapeng
dc.contributor.author Dolge, Kevin
dc.contributor.author Zhang, Biying
dc.contributor.author Heintz, Patrick
dc.contributor.author Shoemaker, Daniel
dc.contributor.author Wang, Bin
dc.contributor.author Huang, Wenyu
dc.contributor.department Ames Laboratory
dc.contributor.department Chemistry
dc.date 2021-08-04T22:56:06.000
dc.date.accessioned 2021-08-14T01:37:53Z
dc.date.available 2021-08-14T01:37:53Z
dc.date.embargo 2022-06-10
dc.date.issued 2021-06-10
dc.description.abstract <p>Effective control on chemoselectivity in the catalytic hydrogenation of C=O over C=C bonds is uncommon with Pd-based catalysts because of the favored adsorption of C=C bonds on Pd surface. Here we report a unique orthorhombic PdSn intermetallic phase with unprecedented chemoselectivity toward C=O hydrogenation. We observed the formation and metastability of this PdSn phase in situ. During a natural cooling process, the PdSn nanoparticles readily revert to the favored Pd3Sn2 phase. Instead, using a thermal quenching method, we prepared a pure-phase PdSn nanocatalyst. PdSn shows an >96 % selectivity toward hydrogenating C=O bonds of various α,β-unsaturated aldehydes, highest in reported Pd-based catalysts. Further study suggests that efficient quenching prevents the reversion from PdSn- to Pd3Sn2-structured surface, the key to the desired catalytic performance. Density functional theory calculations and analysis of reaction kinetics provide an explanation for the observed high selectivity.</p>
dc.identifier archive/lib.dr.iastate.edu/ameslab_manuscripts/963/
dc.identifier.articleid 1964
dc.identifier.contextkey 24184303
dc.identifier.s3bucket isulib-bepress-aws-west
dc.identifier.submissionpath ameslab_manuscripts/963
dc.identifier.uri https://dr.lib.iastate.edu/handle/20.500.12876/aw4N48yr
dc.language.iso en
dc.relation.ispartofseries IS-J 10555
dc.source.bitstream archive/lib.dr.iastate.edu/ameslab_manuscripts/963/IS_J_10555.pdf|||Sat Jan 15 02:35:47 UTC 2022
dc.source.uri 10.1002/anie.202106515
dc.subject.disciplines Materials Science and Engineering
dc.title Thermal Unequilibrium of PdSn Intermetallic Nanocatalysts: From In Situ Tailored Synthesis to Unexpected Hydrogenation Selectivity
dc.type article
dc.type.genre article
dspace.entity.type Publication
relation.isAuthorOfPublication 6acd59cc-28ec-46dd-8bf0-51bcc56d79f9
relation.isOrgUnitOfPublication 25913818-6714-4be5-89a6-f70c8facdf7e
relation.isOrgUnitOfPublication 42864f6e-7a3d-4be3-8b5a-0ae3c3830a11
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