Uncovering the active sites and demonstrating stable catalyst for the cost-effective conversion of ethanol to 1-butanol

Guo, Mond F.; Gray, Michel J.; Job, Heather M.; Alvarez-Vasco, Carlos A.; Subramaniam, Senthil; Zhang, Xiao; Kovarik, Libor; Murugesan, Vijayakumar; Phillips, Steven D.; Kallupalayam Ramasamy, Karthikeyan

doi:10.1039/d1gc01979a

Title: Uncovering the active sites and demonstrating stable catalyst for the cost-effective conversion of ethanol to 1-butanol

Journal Article · Tue Aug 24 00:00:00 EDT 2021 · Green Chemistry

DOI:https://doi.org/10.1039/d1gc01979a· OSTI ID:1846186

^[1]; Gray, Michel J. ^[2]; Job, Heather M. ^[2]; Alvarez-Vasco, Carlos A. ^[1]; Subramaniam, Senthil ^[1];

^[1];

^[2];

^[2]; Phillips, Steven D. ^[2]; Kallupalayam Ramasamy, Karthikeyan ^[2]

Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Washington State Univ., Richland, WA (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

We report the recent emergence of a robust renewable ethanol industry has provided a sustainable platform molecule toward the production of value-added chemicals and fuels; what is lacking now are viable conversion processes from ethanol that can displace the current production pathways from non-renewable pathways. Here in the work, we demonstrate the highly selective conversion of ethanol to higher alcohols over low copper loaded MgAl mixed oxide catalysts, with 50% improvement in higher alcohol yields over the current state of the art. At these copper concentrations, atomically dispersed Cu⁺¹ were found to be stable even at highly reductive conditions and highly active towards higher alcohol products (e.g. butanol, hexanol) while suppressing side reaction pathways and leading to extended lifetimes of over 150 hours time on stream. Technoeconomic analysis conducted based on these experimental results demonstrate that this catalytic system is cost-competitive with the conventional process. This marks significant progress in the development of Guerbet coupling of ethanol as a viable renewable process and offers a pathway toward sustainable chemical and fuel production.

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

Sponsoring Organization:: USDOE Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: AC05-76RL01830; AC02-06CH11357

OSTI ID:: 1846186

Alternate ID(s):: OSTI ID: 1819004

Report Number(s):: PNNL-SA-164007

Journal Information:: Green Chemistry, Vol. 23, Issue 20; ISSN 1463-9262

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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