Electronic modulation of InNi3C0.5/Fe3O4 by support precursor toward efficient CO2 hydrogenation to methanol

APPLIED CATALYSIS B-ENVIRONMENTAL(2022)

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摘要
Carbon neutrality is spurring worldwide impetus on the exploration of CO2 hydrogenation to methanol, but groundbreaking catalyst presents a grand challenge. An outstanding InNi3C0.5/Fe3O4 catalyst is tailored by finely tuning the electronic metal-support interaction (EMSI) that is controlled by Fe3O4 precursor. The one using Fe3O4-N (from ferric nitrate) stands out against the ones using Fe3O4-A (ferrous acetate) and Fe3O4-C (ferric chloride), achieving a turnover frequency (421.6 h(-1)) 2.3-3.1 times as high as that of the two others. There is a correlation between the oxygen deficiency of Fe3O4 and the EMSI-governed activity. The EMSI effect is enhanced substantially by the highly oxygen-deficient Fe3O4-N. Enhanced EMSI makes InNi3C0.5 electron-enriched and thus enables CO2 to be dissociated easily. The InNi3C0.5/Fe3O4-N achieves a high methanol space time yield of 2.60 g(MeOH) g(cat)(-1) h(-1) with 92.0% methanol selectivity at 325 degrees C and 6.0 MPa. This catalyst is also highly anti-sintering and anti-sulfur poisoning.
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关键词
CO2 hydrogenation to methanol, Intermetallic catalysis, Electronic metal-support interaction, Oxygen deficiency, Indium-nickel intermetallic, Iron oxides
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