Substrate–Support Interactions Mediate Hydrogenation of Phenolic Compounds by Pd/CeO2 Nanorods

An, Yeongseo; Naik, Pranjali; Slowing, Igor I.; Venditti, Vincenzo

doi:10.1021/acsanm.0c02381

Substrate–Support Interactions Mediate Hydrogenation of Phenolic Compounds by Pd/CeO₂ Nanorods

Journal Article · Thu Nov 05 00:00:00 EST 2020 · ACS Applied Nano Materials

DOI:https://doi.org/10.1021/acsanm.0c02381· OSTI ID:1764847

An, Yeongseo ^[1]; Naik, Pranjali ^[2]; ^[2]; ^[1]

Iowa State Univ., Ames, IA (United States)
Iowa State Univ., Ames, IA (United States); Ames Lab., Ames, IA (United States)

Ceria-supported palladium (Pd/CeO₂) has spawned significant attention in recent years due to its ability to catalyze selective hydrogenation of phenolic compounds to cyclohexanones and cyclohexanols at a mild temperature and pressure. However, the mechanistic basis by which ceria enhances catalytic conversion is still unclear. Here, we use the increase in the ¹³C transverse relaxation rate upon the addition of nanoparticles (NPs) (¹³C ΔR₂) to investigate the adsorption of phenolic compounds on the surface of the Pd/CeO₂ catalyst by solution NMR. We show that hydroxyphenols adsorb on the support more efficiently than underivatized phenol and methoxyphenols and that phenol derivatives with an oxygen atom at position 2 (i.e., 2-hydroxyphenol and 2-methoxyphenol) form very stable interactions with the Pd site of Pd/CeO₂. An analysis of the kinetics of hydrogenation revealed that catalytic conversion is linearly correlated with the ability of the substrate to form interactions with the CeO₂ support and is inhibited by the formation of stable substrate–Pd adducts. Our data suggest that CeO₂–substrate interactions mediate phenol hydrogenation more efficiently than Pd–substrate interactions and explain the exceptional catalytic performance reported for Pd/CeO₂.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: AC02-07CH11358

OSTI ID:: 1764847

Report Number(s):: IS--J-10,403

Journal Information:: ACS Applied Nano Materials, Journal Name: ACS Applied Nano Materials Journal Issue: 11 Vol. 3; ISSN 2574-0970

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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