Selective hydrogenation of CO2 into value-added hydrocarbons, particularly single products, is of great interest. However, this is a challenge because of the simultaneous occurrence of numerous competing elementary reactions. Here a GaZrOx/H-SSZ-13 composite is developed, which shows propane selectivity in hydrocarbons of 79.5%, along with butane selectivity of 9.9% and CO selectivity of 31.8%, at CO2 conversion of 43.4%. Such catalytic performance can be well maintained within 500 h. Incorporation of proper amounts of Ga into ZrO2 promotes methanol formation due to generation of high concentrations of surface oxygen vacancies with moderate CO2 adsorption strength. The large number of strong-acid sites of H-SSZ-13 seriously restricts conversion of generated methanol into aromatics at high H2 pressure, suppressing the aromatics-based cycle and favouring the alkene-based cycle instead. Accordingly, far more propene and butene are obtained than ethene, although they are rapidly hydrogenated to corresponding alkanes on the strong-acid sites of H-SSZ-13. The hydrogenation of CO2 into more valuable hydrocarbons is potentially attractive in the context of greenhouse gas removal schemes, although the efficiency of such processes is still limited. Now, a GaZrOx oxide catalyst working in combination with an H-SSZ-13 zeolite enables the highly efficient hydrogenation of CO2 to propane with minimal by-product production. 

/pdf/highly-selective-hydrogenation-of-co2-to-propane-over-gazrox-1ff3kv71.pdf

Highly selective hydrogenation of CO2 to propane over GaZrOx/H-SSZ-13 composite

Direct carbon dioxide hydrogenation to produce bulk chemicals and liquid fuels via heterogeneous catalysis

The chemical conversion of CO2 into hydrocarbon fuels and chemicals using green hydrogen not only utilizes abundant CO2 as a carbon feedstock but also enables the storage of hydrogen. Herein, we investigate the direct hydrogenation of CO2 to gasoline and olefins over a series of bifunctional iron-zeolite tandem catalysts operated at high temperatures (> 300 ℃). This process may efficiently utilize CO2 discharged from industrial combustion and green H2 produced by solid oxide electrolytic cells (SOEC). The optimized FeMnK+H-ZSM-5 catalyst offers a 70% selectivity of C5−C11 range hydrocarbons together with a 17% selectivity of C2−C4 lower olefins at 320 °C. The CO2 conversion levels and the aromatics contents could be greatly enhanced as the temperature increases from 320 ℃ to 400 ℃. The hydrocarbon distribution is mainly determined by the micropore size of the zeolites. The dynamic evolution of bifunctional catalysts and its impact on bifunctional catalysis was systematically investigated. 

Direct conversion of carbon dioxide into liquid fuels and chemicals by coupling green hydrogen at high temperature

Owing to excessive carbon dioxide (CO2) emissions, which cause severe environmental issues, the conversion and utilization of CO2 have received increasing attention. Owing to its high efficiency and potential for industrial applications, converting CO2 into high value-added chemicals via thermocatalytic hydrogenation is a highly effective route among electrocatalytic, photocatalytic, and thermocatalytic CO2 conversion. In the past two decades, our group has developed novel CO2 hydrogenation technologies to produce chemicals such as aliphatic hydrocarbons, methanol (MeOH), ethanol, and aromatics (especially para-xylene, PX). In this review, we summarize the strategy for CO2 hydrogenation conversion and the novel rational design of catalysts, including low-temperature MeOH synthesis and capsule catalysts for tandem catalysis. We also discuss the challenges and opportunities of CO2 hydrogenation, such as CO2 capture, H2 prices, and carbon taxes. We hope to inspire new ideas for CO2 hydrogenation to produce high value-added chemicals through the design of catalysts and the exploration of reaction paths. 

Recent advancements and perspectives of the CO2 hydrogenation reaction

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. 

/pdf/selective-conversion-of-co2-to-isobutane-enriched-c4-alkanes-jjgk9hha.pdf

Selective conversion of CO2 to isobutane-enriched C4 alkanes over InZrOx-Beta composite catalyst

•Cr2O3(SG)/H-SAPO-34 shows a C2=−C4= selectivity of 95.7% in CO2 hydrogenation •Ethene accounts for more than 74% of light olefins with an E/P ratio reaching 3.1 •Ethanol is formed through the reaction of H3CO∗ with CO2 and H∗ on Cr2O3(SG) •Ethanol is converted into ethene on SAPO-34 and leads to high C2=−C4= selectivity Conversion of CO2 into light olefins is an effective strategy for sustainable utilization of fossil energy and biomass. However, highly selective production of specific olefin, such as ethene, from CO2 hydrogenation is a challenge. Thus, a new catalyst consisting of Cr2O3(SG) oxide and H-SAPO-34 zeolite is fabricated. It shows C2=−C4= selectivity in hydrocarbons as high as 95.7% at 370°C and 0.5 MPa. More interestingly, around 74% of light olefins are ethene, with an ethene/propene (E/P) ratio of 3.1, which is three times that of previously reported results. This catalytic performance is well maintained for at least 600 h. In situ spectroscopy, DFT calculation, and MD simulation results reveal that ethanol, in addition to methanol, is produced on Cr2O3(SG) through successive hydrogenations of CH3COO∗ intermediate, which is generated through the reaction of H3CO∗ with CO2 and H∗. The ethanol is quickly converted into ethene on H-SAPO-34 and is responsible for the primary light olefin distribution. Conversion of CO2 into light olefins is an effective strategy for sustainable utilization of fossil energy and biomass. However, highly selective production of specific olefin, such as ethene, from CO2 hydrogenation is a challenge. Thus, a new catalyst consisting of Cr2O3(SG) oxide and H-SAPO-34 zeolite is fabricated. It shows C2=−C4= selectivity in hydrocarbons as high as 95.7% at 370°C and 0.5 MPa. More interestingly, around 74% of light olefins are ethene, with an ethene/propene (E/P) ratio of 3.1, which is three times that of previously reported results. This catalytic performance is well maintained for at least 600 h. In situ spectroscopy, DFT calculation, and MD simulation results reveal that ethanol, in addition to methanol, is produced on Cr2O3(SG) through successive hydrogenations of CH3COO∗ intermediate, which is generated through the reaction of H3CO∗ with CO2 and H∗. The ethanol is quickly converted into ethene on H-SAPO-34 and is responsible for the primary light olefin distribution. 

Highly effective conversion of CO2 into light olefins abundant in ethene

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Highly effective conversion of CO2 into light olefins abundant in ethene