Photocatalytic alkane production from fatty acid decarboxylation over hydrogenated catalyst
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摘要:
Conversion of renewable biomass into alkanes has gained significant attention as an alternative to replace fossil-based alkanes for sustainable fuel production [1,2].In this context, bio-derived fatty acids are promising feedstock, owing to their inherent structural similarities to diesel-type hydrocarbons and availability from biomass processing in large quantities [3].Numerous systems have been developed for fatty acid deoxygenation into alkane [4].Generally, harsh conditions (temperatures ≥250 ℃, H2 pressures ≥2 MPa) and excess H2 consumption are required, indicating intensive energy input and potential safety hazards.Therefore, efficient transformation under milder conditions is always appealing and desirable, which requires the development of more efficient catalysts and subtle methods.Through an oxidative decarboxylation process, fatty acid can be transformed into alkyl radical intermediates under much milder conditions [5].However, the subsequent production of desired diesel-range alkane which derive from the combination of alkyl radical and hydrogen are impeded by the uncontrollable reactivity of radical intermediates.These active species not only tend to dimerize, but also can further oxidize to corresponding cations, and subsequently form ethers, esters and oligomeric hydrocarbons [6,7].Consequently, controlling the conversion of radical intermediates for preferential hydrogen termination remained challenging, and desired alkanes were always attained in low yield (<50%) via oxidative decarboxylation, despite the avoidance of harsh operation conditions [8].