Electronic modulation of InNi3C_(0. 5)/Fe3O4 by support precursor toward efficient CO2 hydrogenation to methanol
Guofeng Zhao 1Xue-Rong Shi 2Chao Meng1
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作者信息
1. Shanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai 200062, China
2. Department of Materials Engineering, Shanghai University of Engineering Science, Shanghai 201620, China
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Abstract
Carbon neutrality is spurring worldwide impetus on the exploration of CO2 hydrogenation to methanol, but groundbreaking catalyst presents a grand challenge. An outstanding InNi3C_(0.5)/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 InNi3C_(0.5) electron-enriched and thus enables CO2 to be dissociated easily. The InNi3C_(0.5)/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 °C and 6.0 MPa. This catalyst is also highly anti-sintering and anti-sulfur poisoning.
Key words
CO2 hydrogenation to methanol/Intermetallic catalysis/Electronic metal-support interaction/Oxygen deficiency/Indium-nickel intermetallic/Iron oxides