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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