The conversion of different biogenic feedstocks to hydrocarbons is a major challenge when ensuring hydrocarbon and fuel supply in spite of the heterogeneity of this feed. Flexible adaptation to changing compositions is mandatory for the respective processes. In this study, different oxygenate model feeds, such as alcohols, aldehydes, carboxylic acids and esters, were converted at 500 °C and 5 barg H₂ using H-ZSM-5 zeolite catalysts with various Si/Al ratios to identify the relationship between the feed structure and the final product distribution. As the main outcome, the product distribution becomes increasingly independent of the feed structure for Al-rich H-ZSM-5 catalyst samples at low Time on Stream (ToS). Some minor exceptions are the increased formation of aromatics during ToS for carbonyl oxygenates compared to primary alcohols and the dominance of initial deoxygenation products for Si-rich H-ZSM-5 samples. This is interpreted by a multi-stage reaction sequence, which involves the initial deoxygenation of the feed and the subsequent integration of the olefin intermediates into a reaction network. The results pave the way towards the achievement of a desired product distribution in the conversion of different oxygenates simply by the adaption of the Al content of H-ZSM-5.

Organophosphinic acids, R ₂ P(O)(OH), and their derivatives are versatile compounds with applications in catalysis, material chemistry, biomolecular bridging, metal extraction, and flame retardancy. Current synthetic methods primarily rely on white phosphorus (P ₄ ) as a precursor, which is converted into nucleophilic or electrophilic P‐synthons through acid‐/base‐induced disproportionation (e.g., PH ₃ , [H ₂ PO ₂ ] ^– ) or chlorination (PCl ₃ ). However, P ₄ poses significant drawbacks due to its highly pyrophoric nature, environmental hazards, and the energy‐intensive production process from phosphate ores. Previously, we introduced a method to bypass P ₄ in the synthesis of P ^V compounds through the redox‐neutral activation of phosphates using trifluoromethanesulfonic anhydride (Tf ₂ O) and pyridine, yielding the electrophilic PO ₂ ⁺ phosphorylation reagent [(pyridine) ₂ PO ₂ ][OTf] ( 1a [OTf]). While this reagent exhibits high selectivity for alcohols, amides, and (pseudo)halides, it failed to react efficiently with organometallic compounds to form organophosphinates. Here, we present mechanistic studies that rationalize this limitation and report an optimized strategy, which successfully facilitates reactions with Grignard reagents. By replacing the pyridine leaving group in 1a [OTf] with 4‐dimethylaminopyridine (DMAP), the reagent [(DMAP) ₂ PO ₂ ][OTf] ( 1b [OTf]) is obtained, which enables the selective synthesis of a broad range of diaryl‐ and dialkynylphosphinates, thereby expanding the scope of redox‐neutral phosphate activation.