Abstract
A promising Ni-MoOx bifunctional catalyst for halide-free methanol carbonylation is developed by H2-reduction of NiO-MoO3/SiO2 obtained via facile impregnation method. Catalyst performance is strongly dependent on the calcination/reduction temperature. Over the preferable NiMo-350-600/SiO2 catalyst obtained by calcining at 350 °C and subsequently reducing at 600 °C, a methanol conversion of 4.2 % and acetyls space-time yield of 1.37 mol kgcat−1 h−1 are achieved with 22.1 % selectivity to acetyls at 290 °C and 3 MPa. Co-existence of Ni0 and MoOx (especially MoO2) markedly decreases formation of dimethyl ether (DME) and reversely increases acetyls formation, in nature, due to the catalyst acidity modulation and the partial electron transfer from Ni0 to MoOx that tunes the CO adsorption strength on Ni0 sites. MoO3 and NiMoO4 are both favorable for formation of acetyls and DME whereas the latter mainly accounts for DME formation. MoNi4 alone favors methyl formate formation while together with MoO2 enhancing DME production.
Published Version
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