Hydrogenation of CO<sub>2</sub> into aromatics over ZnZrO–Zn/HZSM-5 composite catalysts derived from ZIF-8

Tian, Haifeng; Jiao, Jiapeng; Zha, Fei; Guo, Xiaojun; Chang, Yaoguang; Chen, Hongshan

doi:10.1039/d1cy01570b

Cited by 19 publications

(8 citation statements)

References 60 publications

(70 reference statements)

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“…The concentration of Ov is a critical factor regulating the adsorption and activation of the target moieties . When a suitable quantity of Zn was supplemented into UiO-66, the surface concentration of Ov increased, which would provide more active sites for the activation of H–H and C–O bonds, the H 2 molecule dissociation, and the CO 2 molecule adsorption . According to the above calculation, the Zn-Zr 5 UiO-66 model had good performance on H 2 molecule dissociation and CO 2 molecule adsorption.…”

Section: Resultsmentioning

confidence: 90%

Reaction Mechanisms and Catalytic Performance of CO₂ to Aromatics Over M(ZnO, Ga₂O₃, In₂O₃)-UiO-66 Catalysts Without Zeolite

Tian,

Gao,

Yang

et al. 2023

ACS Sustainable Chem. Eng.

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Tandem catalysts comprising HZSM-5 zeolite and metallic oxides are common choices for the hydrogenation of CO2 to aromatics, a process of high strategic value in view of carbon capture, utilization, and storage. Nevertheless, due to time-consuming procedures for the preparation of HZSM-5 and the frequent inactivation of reactions resulting from carbon deposition, lately, researchers have focused their efforts on the modification of HZSM-5. Meanwhile, it is still a huge challenge to find novel catalysts, free from HZSM-5, for successfully hydrogenating CO2 to an aromatic moiety. In this work, tandem catalysts based on metal–organic frameworks (MOFs) and metal oxides were demonstrated to have high selectivity to prepare aromatics from CO2 without using HZSM-5, which has introduced a new way for developing catalysts for facile hydrogenation of CO2 to aromatics. The tandem catalysts were extensively studied for their physicochemical attributes by X-ray diffraction (XRD), scanning electron microscopy (SEM), NH3 temperature-programmed desorption (NH3-TPD), pyridine infrared radiation (Py-IR), H2 temperature-programmed reduction (H2-TPR), CO2 temperature-programmed desorption (CO2-TPD), X-ray photoelectron spectroscopy (XPS), and N2 isothermal adsorption–desorption methods. The effects of the amount and type of metal oxides as well as the influence of reaction conditions on the performance of the catalyst were also examined. The experimental outcome demonstrated that under optimum reaction conditions, the CO2 conversion rate of the 8% ZnO-UiO-66 catalyst was 25.0%, with a selectivity of 76.5% for benzene, toluene, and xylene (BTX). Meanwhile, the side reactions can also be effectively inhibited, and a high selectivity (67.4%) of aromatics can be achieved under atmospheric pressure. The adsorption properties of the ZnO-UiO-66 catalyst for H2 and CO2 were also studied by density functional theory (DFT) and in situ DRIFTS. In addition, the mechanism of the reaction that converts CO2 to aromatics via hydrogenation is also discussed. The attainment of the energy barrier and transition state for the hydrogenation of CO2 to aromatics was achieved through a minimal energy search of the transition state of LST/QST.

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Section: Resultsmentioning

confidence: 90%

Reaction Mechanisms and Catalytic Performance of CO₂ to Aromatics Over M(ZnO, Ga₂O₃, In₂O₃)-UiO-66 Catalysts Without Zeolite

Tian,

Gao,

Yang

et al. 2023

ACS Sustainable Chem. Eng.

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“…The catalytic behavior of ZnAlO x &Si-H-ZSM-5 would be interesting to industry, because ethene, propene and PX are the most important commodity hydrocarbon chemicals. Modified nano-hierarchical-pore HZSM-5 zeolite (Zn/Z5) prepared via steam-assisted crystallization using ZIF-8 as a sacrificial template and Zn source was incorporated with ZnZrO to realize the CO 2 conversion to aromatics 103 . The Zn/Z5 zeolite with a smaller particle size, larger specific surface area, mesopore volume and suitable acidic distribution, was in favor of the improved physical transport of intermediates and further aromatization.…”

Section: Ees Catalysis Accepted Manuscriptmentioning

confidence: 99%

“…Tian et al applied a ZnZrO component prepared with ZIF-8 as the precursor via a simple calcination process for CO 2 conversion. 103 The positive correlation between the concentration of oxygen vacancies and the adsorption and activation capacity of CO 2 was disclosed by the generalized gradient approximation (GGA) of density functional theory (DFT) simulation results. A CO 2 conversion of 15.2% and aromatic selectivity of 63.9% can be achieved under optimal reaction conditions.…”

Section: Methanol Synthesis Catalystsmentioning

confidence: 99%

“…The well-matched CO 2 and H 2 activation derived from the synergy between ZrO 2 and ZnO plays a crucial role in the excellent performance for CO 2 conversion to aromatics. Tian et al applied a ZnZrO component prepared with ZIF-8 as precursor via a simple calcination process for CO 2 conversion103 . The positive correlation between the concentration of oxygen vacancies and the adsorption and activation capacity of CO 2 was disclosed by the generalized gradient approximation (GGA) of density functional theory (DFT) simulation results.…”

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confidence: 99%

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A review of the recent progress on direct heterogeneous catalytic CO₂ hydrogenation to gasoline-range hydrocarbons

Shang¹,

Liu²,

Su³

et al. 2023

EES. Catal.

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“…At present, several pathways have been developed to convert CO 2 , such as catalytic reduction into methanol, , CO, formic acid, olefins, − hydrocarbons, , aromatics (Aro), − etc., by thermal catalytic hydrogenation. Among these pathways, CO 2 conversion into aromatics over the hybrid OX-zeolite catalyst is remarkably attractive in consideration of aromatics as the most important platform chemicals.…”

Section: Introductionmentioning

confidence: 99%

Promotional Effect of Dispersant Modification to ZnCr on CO₂ Hydrogenation into Aromatics over Hybrid Catalysts

Zhang

Zheng

Wang

et al. 2022

Ind. Eng. Chem. Res.

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The hybrid catalyst through coupling metal oxides and zeolite is a strategy for converting CO2 to the targeted hydrocarbons containing aromatics. Herein, we framed an active hybrid catalyst comprising ZnCr oxide and HZSM-5 zeolite for conversion of CO2 to aromatics. The usage of dispersants (PEG or TPABr) in the process of preparing ZnCr oxide is certainly effective to improve the yield of aromatics. Over the hybrid catalyst ZnCr-TPABr + HZSM-5 with TPABr as a dispersant, the total hydrocarbon (HCt) selectivity increases to 37.4% at 330 °C, obviously higher than that over the hybrid catalyst ZnCr-none + HZSM-5 without a dispersant (29.5%), wherein C5+ hydrocarbons in the HCt account for above 69%. Moreover, the proportion of aromatics in C5+ products is improved to 87.9 from 79.4%. Multitechnique characterizations demonstrate that the usage of the TPABr dispersant induces smaller crystal sizes, the formation of more nonstoichiometric ZnCr x O y spinels and oxygen vacancies, and the accumulation of ZnO on the surface of the ZnCr-TPABr oxide, which are in favor of the adsorption of CO2 and the formation of the intermediate methanol or its precursor, methoxyl, finally leading to the improved catalytic performance.

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Hydrogenation of CO₂ into aromatics over ZnZrO–Zn/HZSM-5 composite catalysts derived from ZIF-8

Abstract: The direct conversion of CO2 to aromatics is a great strategic significance for the realization of carbon capture, utilization and storage. However, the efficient conversion of CO2 is still challenging...

Cited by 19 publications

References 60 publications

Reaction Mechanisms and Catalytic Performance of CO₂ to Aromatics Over M(ZnO, Ga₂O₃, In₂O₃)-UiO-66 Catalysts Without Zeolite

Reaction Mechanisms and Catalytic Performance of CO₂ to Aromatics Over M(ZnO, Ga₂O₃, In₂O₃)-UiO-66 Catalysts Without Zeolite

A review of the recent progress on direct heterogeneous catalytic CO₂ hydrogenation to gasoline-range hydrocarbons

Promotional Effect of Dispersant Modification to ZnCr on CO₂ Hydrogenation into Aromatics over Hybrid Catalysts

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Hydrogenation of CO2 into aromatics over ZnZrO–Zn/HZSM-5 composite catalysts derived from ZIF-8

Abstract: The direct conversion of CO2 to aromatics is a great strategic significance for the realization of carbon capture, utilization and storage. However, the efficient conversion of CO2 is still challenging...

Cited by 19 publications

References 60 publications

Reaction Mechanisms and Catalytic Performance of CO2 to Aromatics Over M(ZnO, Ga2O3, In2O3)-UiO-66 Catalysts Without Zeolite

Reaction Mechanisms and Catalytic Performance of CO2 to Aromatics Over M(ZnO, Ga2O3, In2O3)-UiO-66 Catalysts Without Zeolite

A review of the recent progress on direct heterogeneous catalytic CO2 hydrogenation to gasoline-range hydrocarbons

Promotional Effect of Dispersant Modification to ZnCr on CO2 Hydrogenation into Aromatics over Hybrid Catalysts

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Product

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Hydrogenation of CO₂ into aromatics over ZnZrO–Zn/HZSM-5 composite catalysts derived from ZIF-8

Reaction Mechanisms and Catalytic Performance of CO₂ to Aromatics Over M(ZnO, Ga₂O₃, In₂O₃)-UiO-66 Catalysts Without Zeolite

Reaction Mechanisms and Catalytic Performance of CO₂ to Aromatics Over M(ZnO, Ga₂O₃, In₂O₃)-UiO-66 Catalysts Without Zeolite

A review of the recent progress on direct heterogeneous catalytic CO₂ hydrogenation to gasoline-range hydrocarbons

Promotional Effect of Dispersant Modification to ZnCr on CO₂ Hydrogenation into Aromatics over Hybrid Catalysts