Higher alcohol (HA) has drawn considerable interest as it can be applied in several fields with great demands, such as solvents, fuels and intermediates in the synthesis of chemicals. Currently, the HA is primarily produced by fermentation process of biomass-derived sugars and ethylene hydration process over solid acidic catalysts, which are not sustainable due to the dependence on grain and fossil fuels. Herein, a novel strategy is proposed to fabricate K-NiMoS catalysts for higher alcohol synthesis with tunable size and dispersion of MoS2 nanocrystal by hydrothermal deposition method of surfactant-encapsulated polyoxomolybdate clusters, and high synergism as the introduction of nickel by incipient wetness impregnation method. A higher conversion (9.5 %) and alcohols selectivity (49.4 %) can be identified for K,Ni-Mo/MMO, accompanied by lower CO2 and hydrocarbons selectivity, respectively. Notably, the ethanol selectivity dramatically increases from 10.6 to 22.2 %, and the C2-C3 alcohols are the main products, which are about 69.4 % in all oxygenates on K,Ni-Mo/MMO. The K,Ni-Mo/MMO also exhibits a high space time yield (STY) of 253 mg/g catalyst/h for C2+ oxygenates, which is about 3.2 times than that of IM-K,Ni-Mo/MMO. The most probable MoS2 slabs on K,Ni-Mo/MMO-S have a smaller mean length (6.66 vs. 9.33 nm) and much lower stacking (2.49 vs. 2.96) than those of IM-K,Ni-Mo/MMO-S (Figure 1). The existence of larger MoO3 particles in IM-K,Ni-Mo/MMO-S may be responsible for the formation of longer and thicker MoS2 crystalline stacks. Therefore, the more active sites can be exposed to reactants on K,Ni-Mo/MMO-S. The excellent performance should ascribed to the better dispersion of MoS2 slab in the K,Ni-Mo/MMO-S. In conclusion, this article reports a novel method for preparing supported K-NiMoS catalysts with tunable size and morphology of active phases to achieve highly performance. The authors acknowledge the financial supports from the NSFC (No. 21576288 and U1662104).

Enhanced higher alcohol synthesis via tuning the metal-support interaction using surfactant-encapsulated polymolybdate precursor

254th National Meeting (2017)

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