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

Chen, Minda; Yan, Yu; Gebre, Mebatsion; Ordonez, Claudio; Liu, Fudong; Qi, Long; Lamkins, Andrew; Jing, Dapeng; Dolge, Kevin; Zhang, Biying; Heintz, Patrick; Shoemaker, Daniel P.; Wang, Bin; Huang, Wenyu

doi:10.1002/anie.202106515

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

Journal Article · Fri Jul 16 00:00:00 EDT 2021 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.202106515· OSTI ID:1817653

Chen, Minda ^[1]; Yan, Yu ^[2]; Gebre, Mebatsion ^[3]; Ordonez, Claudio ^[1]; Liu, Fudong ^[4]; Qi, Long ^[5]; Lamkins, Andrew ^[1]; Jing, Dapeng ^[6]; Dolge, Kevin ^[1]; Zhang, Biying ^[1]; Heintz, Patrick ^[1]; Shoemaker, Daniel P. ^[3]; ^[2]; ^[7]

Iowa State Univ., Ames, IA (United States)
Univ. of Oklahoma, Norman, OK (United States)
Univ. of Illinois at Urbana-Champaign, IL (United States)
Univ. of Central Florida, Orlando, FL (United States). Catalysis Cluster for Renewable Energy and Chemical Transformations (REACT), NanoScience Technology Center (NSTC)
Ames Lab., Ames, IA (United States)
Ames Lab., Ames, IA (United States); Iowa State Univ., Ames, IA (United States). Materials Analysis and Research Lab.
Ames Lab., and Iowa State Univ., Ames, IA (United States)

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. Furthermore, 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.

View Accepted Manuscript (DOE)

Research Organization:: Ames Laboratory (AMES), Ames, IA (United States)

Sponsoring Organization:: USDOE; National Science Foundation (NSF)

Grant/Contract Number:: AC02-07CH11358; AC02-07CH11358; AC02-07CH11358; AC02-07CH11358; AC02-07CH11358; AC02-07CH11358; AC02-07CH11358

OSTI ID:: 1817653

Alternate ID(s):: OSTI ID: 1808608
OSTI ID: 1814768
OSTI ID: 1814797
OSTI ID: 1818354

Report Number(s):: IS--J 10,555

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 33 Vol. 60; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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