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

Abstract

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 gMeOH gcat−1 h−1 with 92.0% methanol selectivity at 325 °C and 6.0 MPa. This catalyst is also highly anti-sintering and anti-sulfur poisoning.