First-principle investigation on catalytic hydrogenation of benzaldehyde over Pt-group metals

Yuk, Simuck F.; Lee, Mal-Soon; Akhade, Sneha A.; Nguyen, Manh-Thuong; Glezakou, Vassiliki-Alexandra; Rousseau, Roger

doi:10.1016/j.cattod.2020.07.039

Title: First-principle investigation on catalytic hydrogenation of benzaldehyde over Pt-group metals

Journal Article · 29 July 2020 · Catalysis Today

DOI: https://doi.org/10.1016/j.cattod.2020.07.039 · OSTI ID:1860250

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Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

We report that understanding the hydrogenation of organic compounds in the aqueous phase has always been fundamentally important for improving carbon neutral pathways to fuels and value-added chemicals. In this study, we investigated both thermodynamic and kinetic profiles of benzaldehyde hydrogenation over the Pd(111) and Pt(111) metal surfaces using density functional theory (DFT) and ab initio molecular dynamic (AIMD) simulations. The adsorption of H₂ shows the mixed preference of H adsorption sites on the Pt(111), while the fcc adsorption site is dominant for H on the Pd(111). When benzaldehyde is added to the systems, we observe a strong reduction of benzaldehyde on charged Pd (111) surface compared with that on neutral surface. In contrast, charged state of the Pt(111) surface does not change their interaction. Subsequent hydrogenation reaction of benzaldehyde over Pd(111), proceeding via Langmuir-Hinshelwood mechanism, is affected by two major factors: the presence of H₂O solvent and surface charge. The presence of H₂O solvent greatly reduces the activation energy of C-H and O-H bond formation during the hydrogenation process. Furthermore, the hydrogenation step via C-H bond formation is preferred thermodynamically and kinetically over O-H bond formation during thermocatalytic hydrogenation, while the opposite trend holds true during electrocatalytic hydrogenation.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE; USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC05-76RL01830; AC52-07NA27344

OSTI ID:: 1860250

Report Number(s):: LLNL-JRNL-807162; PNNL-SA-152016

Journal Information:: Catalysis Today, Journal Name: Catalysis Today Vol. 388-389; ISSN 0920-5861

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Title: First-principle investigation on catalytic hydrogenation of benzaldehyde over Pt-group metals

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