Dynamic confinement catalysis in Fe-based CO2 hydrogenation to light olefins

Wang, Linkai; Han, Yu; Wei, Jian; Ge, Qingjie; Lu, Shijian; Mao, Yanpeng; Sun, Jian

doi:10.1016/j.apcatb.2023.122506

Cited by 33 publications

(7 citation statements)

References 57 publications

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“…The apparent dehydrogenation activation energy is determined as 73.98 ± 2.61 kJ/mol for MgH 2 @CNTs-Pd. This reduction in activation energy for MgH 2 @CNTs-Pd compared to pure MgH 2 (measured at 151.9 ± 14.9 kJ/mol) indicates that the introduction of CNTs-Pd facilitates Mg–H dissociation, thereby lowering the barrier for hydrogen formation and release from MgH 2 . Importantly, these activation energy values are notably lower than those reported for common oxides and alloy catalysts, such as Nb 2 O 5 (101 kJ/mol), TiO 2 (161 kJ/mol), and FeNi (93.6 kJ/mo) .…”

Section: Results and Discussionmentioning

confidence: 77%

CNTs-Pd as Efficient Bidirectional Catalyst for Improving Hydrogen Absorption/Desorption Kinetics of Mg/MgH₂

Duan,

Wu,

Liang

et al. 2024

Energy Fuels

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The hydrogen storage potential and cost-effectiveness of MgH 2 have rendered it a desirable material for hydrogen storage. However, its application has been hindered by limitations in thermal stability and dehydrogenation kinetics. In this study, the carbon nanotube-Pd bifunctional catalyst was prepared by using hydrothermal and calcination technology, significantly improving the kinetics of Mg/MgH 2 during hydrogen adsorption/desorption. The activation energy for the Mg@ CNTs-Pd was reduced to 42.73 kJ/mol, as determined by fitting the Avrami−Erofeev model with the Arrhenius equation. Additionally, the activation energy during dehydrogenation was found to be 73.98 kJ/mol based on the Johnson−Mehl−Avrami−Kolmogorov equation and the Arrhenius equation. It is worth noting that the dynamic enhancement persists even after 10 cycles. This groundbreaking research has paved the way for potential applications of MgH 2 as a hydrogen storage material, providing it with broader development opportunities.

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Section: Results and Discussionmentioning

confidence: 77%

CNTs-Pd as Efficient Bidirectional Catalyst for Improving Hydrogen Absorption/Desorption Kinetics of Mg/MgH₂

Duan,

Wu,

Liang

et al. 2024

Energy Fuels

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“…The capture, storage, and utilization of CO 2 has become an urgent need to solve this problem. As such, the conversion of CO 2 into value-added products such as methanol, − dimethyl ether (DME), jet fuel, and low-carbon olefins through catalytic hydrogenation is gradually gaining widespread attention. Dimethyl ether displays significant potential as an alternative fuel, primarily due to its high cetane number, superior combustion efficiency and low emissions of nitrogen oxide and hydrocarbon during the combustion process …”

Section: Introductionmentioning

confidence: 99%

Optimizing CO₂ Hydrogenation to DME through Tailored Interfacial Interactions: Weakening Synergy in CuZnZr and Al-Modified SBA-15 Catalysts

Sun,

Xia,

et al. 2024

Ind. Eng. Chem. Res.

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The direct dimethyl ether (DME) synthesis reaction via CO 2 hydrogenation typically requires a bifunctional catalyst that effectively combines a methanol synthesis catalyst with a methanol dehydration catalyst, but the effect of the relationship between the two catalysts on the catalytic performance has not been as well studied. In this study, we developed a CuZnZr/Al−S(10)-PG bifunctional catalyst physically mixed with Almodified SBA-15 and the traditional CuZnZr catalyst for the hydrogenation of CO 2 to DME. A pivotal discovery is that the modulation of interaction intensity between these two constituents significantly influences the electronic configuration of each component. Through X-ray photoelectron spectroscopy characterization and methanol dehydration experiments, it was confirmed that diminishing the synergistic interplay between CuZnZr and Almodified SBA-15, which regulated the electronic structure of the Cu−Zn interface and enhanced the Cu−Zn interfacial interaction, played a crucial role in enhancing the catalyst's performance in CO 2 hydrogenation to DME. This finding contests established beliefs about the necessity of strong synergistic interactions in such systems and provides new insights for designing rational bifunctional catalysts.

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“…Although there has been significant research on SAPO-34 and SSZ-13 within MeOH-mediated CO 2 conversion, their catalytic activity in CO 2 -FT reactions remains veiled. Most CO 2 -FT reactions with iron-based catalysts produce broad distributions of hydrocarbons, including those with high carbon numbers (over C 15 ), and even when combined with various zeolites, the tendency is still to yield mainly long-chain hydrocarbons. − Here, we explore a hybrid catalytic system consisting of Na/ZnFe 2 O 4 (ZFO) and a CHA-zeolite, demonstrating how CHA-zeolites can modify the hydrocarbon distribution generated from CO 2 hydrogenation reaction over ZFO. The ZFO catalyst by itself produces long-chain hydrocarbons up to C 17 , , but the incorporation of CHA-zeolites shifts the distribution toward a greater proportion of C 2 –C 4 hydrocarbons.…”

Section: Introductionmentioning

confidence: 99%

Selective Light Hydrocarbon Production from CO₂ Hydrogenation over Na/ZnFe₂O₄ and CHA-Zeolite Hybrid Catalysts

Ra,

Kim,

Lee

et al. 2024

ACS Catal.

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Carbon dioxide hydrogenation to value-added fuels and chemicals has been studied widely as a means to recycle the most-troublesome greenhouse gas. The reaction produces hundreds of different chemicals, and therefore, selectivity control toward specific desired products is of paramount importance. In this study, a hybrid catalyst system consisting of Na/ZnFe2O4 (ZFO) and a CHA-zeolite (SSZ-13 or SAPO-34) is developed to maximize C2–C4 light hydrocarbon production. Utilizing the compact 3.8 Å pore size of CHA-zeolites, the Na/ZnFe2O4 catalyst-produced long-chain hydrocarbons are efficiently shortened to C2–C4 hydrocarbons with over 55% selectivity in the hybrid systems. Notably, ZFO + SAPO-34 shows a preference for light olefins, while ZFO + SSZ-13 uniquely enhances selectivity for C3 products. The difference is attributed to the much stronger acid sites present in SSZ-13 than in SAPO-34, which promote hydrogenation of olefins and the ethylene-to-propane conversion reaction in particular. Further modification of SSZ-13 with steam treatment leads to the dealumination of its framework and an enhanced activity of the ethylene-to-propane reaction, yielding 32.8% of C3-selectivity. Accordingly, a hybrid catalytic system combining a CO2 Fischer–Tropsch catalyst with a CHA-zeolite is a promising route to produce light hydrocarbons from CO2 hydrogenation more selectively than single catalysts. This work also demonstrates that acidity control could be a powerful tool to manipulate the reaction pathway that occurs on zeolite catalysts.

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Dynamic confinement catalysis in Fe-based CO2 hydrogenation to light olefins

Cited by 33 publications

References 57 publications

CNTs-Pd as Efficient Bidirectional Catalyst for Improving Hydrogen Absorption/Desorption Kinetics of Mg/MgH₂

CNTs-Pd as Efficient Bidirectional Catalyst for Improving Hydrogen Absorption/Desorption Kinetics of Mg/MgH₂

Optimizing CO₂ Hydrogenation to DME through Tailored Interfacial Interactions: Weakening Synergy in CuZnZr and Al-Modified SBA-15 Catalysts

Selective Light Hydrocarbon Production from CO₂ Hydrogenation over Na/ZnFe₂O₄ and CHA-Zeolite Hybrid Catalysts

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Dynamic confinement catalysis in Fe-based CO2 hydrogenation to light olefins

Cited by 33 publications

References 57 publications

CNTs-Pd as Efficient Bidirectional Catalyst for Improving Hydrogen Absorption/Desorption Kinetics of Mg/MgH2

CNTs-Pd as Efficient Bidirectional Catalyst for Improving Hydrogen Absorption/Desorption Kinetics of Mg/MgH2

Optimizing CO2 Hydrogenation to DME through Tailored Interfacial Interactions: Weakening Synergy in CuZnZr and Al-Modified SBA-15 Catalysts

Selective Light Hydrocarbon Production from CO2 Hydrogenation over Na/ZnFe2O4 and CHA-Zeolite Hybrid Catalysts

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Resources

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CNTs-Pd as Efficient Bidirectional Catalyst for Improving Hydrogen Absorption/Desorption Kinetics of Mg/MgH₂

CNTs-Pd as Efficient Bidirectional Catalyst for Improving Hydrogen Absorption/Desorption Kinetics of Mg/MgH₂

Optimizing CO₂ Hydrogenation to DME through Tailored Interfacial Interactions: Weakening Synergy in CuZnZr and Al-Modified SBA-15 Catalysts

Selective Light Hydrocarbon Production from CO₂ Hydrogenation over Na/ZnFe₂O₄ and CHA-Zeolite Hybrid Catalysts