Increasing demand for renewable chemicals and fuels has stimulated the search for alternative feedstocks and is driving the ongoing transition to a more renewables-based society. Considerable academic efforts have been directed at the valorisation of biomass sources and derived intermediates, so called platform molecules, to produce value-added chemicals and fuels. In this contribution, opportunities are discussed for the application of zeolite-supported bifunctional catalysts in the conversion of biomass sources into chemicals and fuels via hydrodeoxygenation (HDO). Such metal/zeolite catalyst systems play a prominent role in many of these biomass HDO routes. Emphasis is put on the current progress in metal/zeolite-catalysed HDO of three selected, promising routes involving biomass-derived platform molecules and the model compounds that mimic more complex feeds. Four key concepts of metal/zeolite catalysts, such as combining metal and Brønsted acid sites, site-ratio balancing, proximity between metal and acid functions and shape selectivity are discussed in order to provide a comprehensive overview. In addition, two challenges related to the accessibility of the active sites and catalyst stability in the liquid phase, typically a hot, highly polar, and protic reaction medium, are discussed. Finally, the open challenges and perspectives regarding the development of metal/zeolite catalysts for biomass HDO reactions are examined.
8 December 2023 in Angewandte Chemie International Edition
Rational design of low‐cost and efficient transition‐metal catalysts for low‐temperature CO2 activation is significant and poses great challenges. Herein, a strategy via regulating the local electron density of active sites is developed to boost CO2 methanation that normally requires >350 °C for commercial Ni catalysts. An optimal Ni/ZrO2 catalyst affords an excellent low‐temperature performance hitherto, with a CO2 conversion of 84.0 %, CH4 selectivity of 98.6 % even at 230 °C and GHSV of 12,000 mL g−1 h−1 for 106 h, reflecting one of the best CO2 methanation performance to date on Ni‐based catalysts. Combined a series of in situ spectroscopic characterization studies reveal that re‐constructing monoclinic‐ZrO2 supported Ni species with abundant oxygen vacancies can facilitate CO2 activation, owing to the enhanced local electron density of Ni induced by the strong metal‐support interactions. These findings might be of great aid for construction of robust catalysts with an enhanced performance for CO2 emission abatement and beyond.
A self-prepared 0.85 wt% Ru/ZrO 2 @C catalyst shows an excellent stability for hydrogenation of levulinic acid to γ-valerolactone upon catalyst reuse experiments.