The production of chemicals and fuels by renewable-sourced carbon is a tremendous challenge facing researchers today. When produced by the dehydration of bio-derived alcohols, light olefins serve as a source of renewable comonomers, fine chemicals, and fuels through a catalytic oligomerization upgrading step. While propylene and higher olefins are readily oligomerized over solid acid catalysts such as ZSM-5, ethylene is difficult to activate and requires high temperatures that contribute to undesirable side reactions. Conversely, metal-based catalysts enable ethylene activation at moderate temperatures (100-150 °C) with high selectivity to oligomeric products (&gt;90%). Notably, nickel cations supported on mesoporous aluminosilicates have been demonstrated to be the most active and stable heterogeneous catalysts for the oligomerization of ethylene. Governing the rate of oligomerization are the subsequent steps of initiation, propagation, and termination, of which the electronic environment of nickel plays an important role. As a result, moderate changes in the identity of nearby neighbors to nickel have been shown to play a large role in the activity and selectivity of these catalysts towards desired chemicals and fuels. The goal of this study is to demonstrate the present state of the art in heterogeneous nickel-containing catalysts for ethylene oligomerization alongside new materials that possess modified electronic environments. The role of support and electronic promoters is explored. The catalytic performance of these materials is then characterized by fixed bed reactor experiments, while X-ray photoelectron spectroscopy (XPS) studies guide insights into the catalytically-governing electronic environment of nickel.

Modified heterogeneous nickel catalysts for the production of chemicals and fuels from bioderived light olefins

249th National Meeting (2015)

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