Selective conversion of CO<sub>2</sub> to isobutane-enriched C<sub>4</sub> alkanes over InZrO<sub>x</sub>-Beta composite catalyst.

Wang, Han; Fan, Sheng; Guo, Shujia; Wang, Sen; Qin, Zhangfeng; Dong, Mei; Zhu, Huaqing; Fan, Weibin et al. · Nat Commun · 2023

basic_science · Level V

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Abstract

Direct conversion of CO2 to a single specific hydrocarbon with high selectivity is extremely attractive but very challenging. Herein, by employing an InZrOx-Beta composite catalyst in the CO2 hydrogenation, a high selectivity of 53.4% to butane is achieved in hydrocarbons (CO free) under 315 °C and 3.0 MPa, at a CO2 conversion of 20.4%. Various characterizations and DFT calculation reveal that the generation of methanol-related intermediates by CO2 hydrogenation is closely related to the surface oxygen vacancies of InZrOx, which can be tuned through modulating the preparation methods. In contrast, the three-dimensional 12-ring channels of H-Beta conduces to forming higher methylbenzenes and methylnaphthalenes containing isopropyl side-chain, which favors the transformation of methanol-related intermediates to butane through alkyl side-chain elimination and subsequent methylation and hydrogenation. Moreover, the catalytic stability of InZrOx-Beta in the CO2 hydrogenation is considerably improved by a surface silica protection strategy which can effectively inhibit the indium migration.