The role of adsorbed species in 1-butene isomerization: Parahydrogen-induced polarization NMR of Pd-Au catalyzed butadiene hydrogenation

Wang, Weiyu, Lewis, Richard J., Lu, Bintian, Wang, Qiang, Hutchings, Graham J. ORCID: https://orcid.org/0000-0001-8885-1560, Xu, Jun and Deng, Feng 2024. The role of adsorbed species in 1-butene isomerization: Parahydrogen-induced polarization NMR of Pd-Au catalyzed butadiene hydrogenation. ACS Catalysis 14 (4) , 2522–2531. 10.1021/acscatal.3c05968

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Abstract

Isomerization of 1-butene critically influences product distributions in 1,3-butadiene hydrogenation. However, distinguishing between the isomerization and hydrogenation pathways is challenging. Here, we employ parahydrogen-induced polarization (PHIP) NMR spectroscopy to determine the extent of the isomerization pathway when using Pd–Au bimetallic nanoparticles synthesized via a colloidal protocol in the presence or absence of a polyvinylpyrrolidone (PVP) stabilizing ligand and immobilized on TiO2. Residual additives, in particular, sulfur, are observed to considerably influence the pairwise hydrogenation and 1-butene isomerization pathways. PHIP NMR analysis reveals that the PVP ligand can induce strong polarized signals, likely due to restricted proton migration, but minimally impact 1-butene isomerization. In contrast, removing surface sulfur species introduced during catalyst synthesis profoundly enhances 1-butene isomerization by reducing the hydrogen concentration at the nanoparticle surface. This work elucidates how residual species can modulate key reaction pathways such as isomerization during 1,3-butadiene hydrogenation, with implications for rational catalyst design.

Item Type:	Article
Date Type:	Publication
Status:	Published
Schools:	Schools > Chemistry Research Institutes & Centres > Cardiff Catalysis Institute (CCI)
Publisher:	American Chemical Society
ISSN:	2155-5435
Funders:	Cardi� University and the Max Planck Centre for Fundamental Heterogeneous Catalysis (FUNCAT)
Date of First Compliant Deposit:	21 February 2024
Date of Acceptance:	17 January 2024
Last Modified:	02 Feb 2025 02:45
URI:	https://orca.cardiff.ac.uk/id/eprint/166432

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