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Gray, Michel J.

Publications and source records attributed to Gray, Michel J..

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

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.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Production of Gaseous Olefins from Syngas over a Cobalt-HZSM-5 Catalyst

Light olefins (C2–C5) are high-value platform chemicals used to produce plastics, lubricants, coating material, and surfactants, and can be intermediates to produce transportation fuels. In this study we report on the development of a Co-based catalyst for direct conversion of fossil as well as biomass derived syngas into light olefins that enables high conversion and olefin/paraffin (O/P) product ratio, minimal selectivity to CO2 (<?1%) and wax formation (C14+ selectivity?<?1%). Over a Co/HZSM-5 bi-functional catalyst 38% CO conversion with C2–C5 olefin selectivity of 48%, and O/P ratio of 4.0 was achieved at 240 °C, 17 bar, and 1.5 L/(g–h). In addition to a gaseous olefin-rich stream a C6–C13 mixed olefin/paraffin liquid byproduct was also produced with 25% selectivity. Both Co loading and the HZSM-5 acidity levels were optimized to maintain the balance between the hydrogenation and the cracking activity to generate high levels of C2–C4 olefins. A suite of catalyst characterization tools were used to correlate the physical and chemical property of the catalyst to the performance of the catalyst towards syngas conversion and C2–C4 olefin selectivity.

Maddi, Balakrishna↗

Method of converting ethanol to higher alcohols

A method and catalyst for forming higher alcohols from lower alcohol feedstocks. In one application a highly selective and stable copper pseudo-single-atom supported on MgO—Al2O3 catalyst is provided which provides ethanol condensation to higher alcohols at ˜50% yields and ˜85% selectivity is demonstrated with stable catalyst lifetime over 500 hours in a continuous flow system. In some applications a Guerbet condensation process is further utilized to yield a higher alcohol at a selectivity of near ˜90%.

09 BIOMASS FUELS↗