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 National 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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