Conversion of ethanol to 1,3–butadiene over Ag–ZrO2/SiO2 catalysts: The role of surface interfaces

Li, Houqian; Pang, Jifeng; Jaegers, Nicholas R.; Engelhard, Mark; Kovarik, Libor; Savoy, Anthony W.; Hu, Jianzhi; Sun, Junming; Wang, Yong

doi:10.1016/j.jechem.2020.05.038

Conversion of ethanol to 1,3–butadiene over Ag–ZrO₂/SiO₂ catalysts: The role of surface interfaces

Journal Article · Sun May 23 00:00:00 EDT 2021 · Journal of Energy Chemistry

DOI:https://doi.org/10.1016/j.jechem.2020.05.038· OSTI ID:1634818

^[1]; Pang, Jifeng ^[2]; Jaegers, Nicholas R. ^[3]; ^[4]; Kovarik, Libor ^[4]; ^[1]; Hu, Jianzhi ^[4]; ^[1]; Wang, Yong ^[3]

Washington State Univ., Pullman, WA (United States)
Chinese Academy of Sciences (CAS), Dalian (China)
Washington State Univ., Pullman, WA (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

A series of Ag–ZrO₂/SiO₂ catalysts with different metal–support interfaces were synthesized in an effort to elucidate the roles of specific interfaces in controlling the ethanol to 1,3–butadiene conversion and selectivity. According to the results of detailed characterizations (e.g. CO/pyridine–DRIFTS, XPS, TEM, NH₃–TPD, and ¹H MAS NMR), it was found that the Ag–O–Si interfaces significantly enhanced the dehydrogenation of ethanol while the presence of ZrO₂ improved the interaction between Ag and ZrO₂/SiO₂, creating more Ag^δ+ active sites. In this research, the high dispersion of ZrO₂ on SiO₂ generated abundant Zr–O–Si interfaces with medium and weak Lewis acidity, promoting the condensation of acetaldehyde to crotonaldehyde. These Zr–O–Si interfaces in close interaction with Ag^δ+ species played a critical role in the enhanced H transfer during the MPV reduction of crotonaldehyde to crotyl alcohol. The synergies among the interfaces resulted in retarded ethanol dehydration reactivity, balanced ethanol dehydrogenation and condensation reactions, and a subsequent high 1,3–butadiene yield.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: National Natural Science Foundation of China (NNSFC); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1634818

Alternate ID(s):: OSTI ID: 1632742

Report Number(s):: PNNL-SA--153728

Journal Information:: Journal of Energy Chemistry, Journal Name: Journal of Energy Chemistry Journal Issue: C Vol. 54; ISSN 2095-4956

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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