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/ange.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

DOI:https://doi.org/10.1002/ange.202106515· OSTI ID:1808607

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]

Department of Chemistry Iowa State University Ames IA 50011 USA
School of Chemical, Biological, and Materials Engineering The University of Oklahoma Norman OK 73019 USA
Department of Materials Science and Engineering University of Illinois Urbana-Champaign Urbana IL 61801 USA
Department of Civil, Environmental, and Construction Engineering Catalysis Cluster for Renewable Energy and Chemical Transformations (REACT) NanoScience Technology Center (NSTC) University of Central Florida Orlando FL 32816 USA
Ames Laboratory U.S. Department of Energy Ames IA 50011 USA
Ames Laboratory U.S. Department of Energy Ames IA 50011 USA, Materials Analysis and Research Laboratory Iowa State University Ames IA 50011 USA
Department of Chemistry Iowa State University Ames IA 50011 USA, Ames Laboratory U.S. Department of Energy Ames IA 50011 USA

Abstract

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 Pd ₃ Sn ₂ 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 Pd ₃ Sn ₂ ‐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 (Publisher)

Sponsoring Organization:: USDOE

Grant/Contract Number:: SC0018284; SC0013897; AC02-06CH11357

OSTI ID:: 1808607

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie Journal Issue: 33 Vol. 133; ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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