Effect of the SiO2 Support on the Catalytic Performance of Ag/ZrO2/SiO2 Catalysts for the Single-Bed Production of Butadiene from Ethanol

Dagle, Vanessa; Flake, Matthew D.; Lemmon, Teresa L.; Saavedra Lopez, Johnny; Kovarik, Libor; Dagle, Robert A.

doi:10.1016/j.apcatb.2018.05.055

Title: Effect of the SiO2 Support on the Catalytic Performance of Ag/ZrO2/SiO2 Catalysts for the Single-Bed Production of Butadiene from Ethanol

Journal Article · Thu Nov 15 00:00:00 EST 2018 · Applied Catalysis. B, Environmental

DOI:https://doi.org/10.1016/j.apcatb.2018.05.055· OSTI ID:1514854

Dagle, Vanessa ^[1]; Flake, Matthew D. ^[1]; Lemmon, Teresa L. ^[1];

^[1]; Kovarik, Libor ^[1];

^[1]

BATTELLE (PACIFIC NW LAB)

A ternary Ag/ZrO2/SiO2 catalyst system was studied for the single-step conversion of ethanol to butadiene by varying the catalyst composition (Ag, Ir, or Pt metal component, Ag/ZrO2 loading, and choice of SiO2 support) and operating conditions (space velocity and feed gas composition). Exceptional catalytic performance was achieved over a 1%Ag/4%ZrO2/SiO2-SBA-16 catalyst leading to 99% conversion and 71% butadiene selectivity while operating under mild conditions (325ºC, 1 atm, 0.23 hr-1). Several classes of silica (i.e., silica gels, fumed silicas, meoporous silicas) were evaluated as support, and SBA-16 was found to be the most promising. The nature of the SiO2 support was found to have a strong influence on both conversion and selectivity. Higher SiO2 catalyst surface areas lead to greater conversion due to increased Ag dispersion thus accelerating the initial ethanol dehydrogenation reaction. By independently varying Ag and ZrO2 loading, Ag was found to be the main component affecting ethanol conversion. Butadiene selectivity varied depending on the concentration of ZrO2 and acidic characteristics of the SiO2 support. A direct relationship between butadiene selectivity and concentration of Lewis acid sites was evidenced. Also, adding H2 to the feed had little effect on conversion while improving catalytic stability, however, selectivity to butadiene was decreased. Finally, catalyst regenerability was successfully demonstrated for several cycles.

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

Sponsoring Organization:: USDOE

DOE Contract Number:: AC05-76RL01830

OSTI ID:: 1514854

Report Number(s):: PNNL-SA-128543

Journal Information:: Applied Catalysis. B, Environmental, Vol. 236

Country of Publication:: United States

Language:: English

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Catalytic conversion of ethanol into butadiene over high performance LiZnHf-MFI zeolite nanosheets Wang, Chan; Zheng, Mingyuan; Li, Xinsheng Green Chemistry, Vol. 21, Issue 5 https://doi.org/10.1039/c8gc03983f	journal	January 2019
Catalytic activation of ethylene C–H bonds on uniform d ⁸ Ir( i ) and Ni( ii ) cations in zeolites: toward molecular level understanding of ethylene polymerization on heterogeneous catalysts Jaegers, Nicholas R.; Khivantsev, Konstantin; Kovarik, Libor Catalysis Science & Technology, Vol. 9, Issue 23 https://doi.org/10.1039/c9cy01442j	journal	January 2019
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Effect of ZnO on acid–base properties and catalytic performances of ZnO/ZrO ₂ –SiO ₂ catalysts in 1,3-butadiene production from ethanol–water mixture Larina, Olga V.; Kyriienko, Pavlo I.; Balakin, Dmytro Yu. Catalysis Science & Technology, Vol. 9, Issue 15 https://doi.org/10.1039/c9cy00991d	journal	January 2019

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Title: Effect of the SiO2 Support on the Catalytic Performance of Ag/ZrO2/SiO2 Catalysts for the Single-Bed Production of Butadiene from Ethanol

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