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Dynamic structural evolution of iron catalysts involving competitive oxidation and carburization during CO₂ hydrogenation.

ABSTRACT: Identifying the dynamic structure of heterogeneous catalysts is crucial for the rational design of new ones. In this contribution, the structural evolution of Fe(0) catalysts during CO₂ hydrogenation to hydrocarbons has been investigated by using several (quasi) in situ techniques. Upon initial reduction, Fe species are carburized to Fe₃C and then to Fe₅C₂. The by-product of CO₂ hydrogenation, H₂O, oxidizes the iron carbide to Fe₃O₄. The formation of Fe₃O₄@(Fe₅C₂+Fe₃O₄) core-shell structure was observed at steady state, and the surface composition depends on the balance of oxidation and carburization, where water plays a key role in the oxidation. The performance of CO₂ hydrogenation was also correlated with the dynamic surface structure. Theoretical calculations and controll experiments reveal the interdependence between the phase transition and reactive environment. We also suggest a practical way to tune the competitive reactions to maintain an Fe₅C₂-rich surface for a desired C₂₊ productivity.

SUBMITTER: Zhu J

PROVIDER: S-EPMC8816344 | biostudies-literature | 2022 Feb

REPOSITORIES: biostudies-literature

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Dynamic structural evolution of iron catalysts involving competitive oxidation and carburization during CO2 hydrogenation.

Zhu Jie J Wang Peng P Zhang Xiaoben X Zhang Guanghui G Li Rongtan R Li Wenhui W Senftle Thomas P TP Liu Wei W Wang Jianyang J Wang Yanli Y Zhang Anfeng A Fu Qiang Q Song Chunshan C Guo Xinwen X

Science advances 20220204 5

Identifying the dynamic structure of heterogeneous catalysts is crucial for the rational design of new ones. In this contribution, the structural evolution of Fe(0) catalysts during CO2 hydrogenation to hydrocarbons has been investigated by using several (quasi) in situ techniques. Upon initial reduction, Fe species are carburized to Fe3C and then to Fe5C2. The by-product of CO2 hydrogenation, H2O, oxidizes the iron carbide to Fe< ...[more]

PMID: 35119927

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Project description:The valorization of CO2 to produce high-value chemicals, such as methanol and hydrocarbons, represents key technology in the future net-zero society. Herein, we report further investigation of a PdZn/ZrO2 + SAPO-34 catalyst for conversion of CO2 and H2 into propane, already presented in a previous work. The focus of this contribution is on the scale up of this catalyst. In particular, we explored the effect of mixing (1:1 mass ratio) and shaping the two catalyst functions into tablets and extrudates using an alumina binder. Their catalytic performance was correlated with structural and spectroscopic characteristics using methods such as FT-IR and X-ray absorption spectroscopy. The two scaled-up bifunctional catalysts demonstrated worse performance than a 1:1 mass physical mixture of the two individual components. Indeed, we demonstrated that the preparation negatively affects the element distribution. The physical mixture is featured by the presence of a PdZn alloy, as demonstrated by our previous work on this sample and high hydrocarbon selectivity among products. For both tablets and extrudates, the characterization showed Zn migration to produce Zn aluminates from the alumina binder phase upon reduction. Moreover, the extrudates showed a remarkable higher amount of Zn aluminates before the activation rather than the tablets. Comparing tablets and extrudates with the physical mixture, no PdZn alloy was observed after activation and only the extrudates showed the presence of metallic Pd. Due to the Zn migration, SAPO-34 poisoning and subsequent deactivation of the catalyst could not be excluded. These findings corroborated the catalytic results: Zn aluminate formation and Pd0 separation could be responsible for the decrease of the catalytic activity of the extrudates, featured by high methane selectivity and unconverted methanol, while tablets displayed reduced methanol conversion to hydrocarbons mainly attributed to the partial deactivation of the SAPO-34.

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Dynamic structural evolution of iron catalysts involving competitive oxidation and carburization during CO₂ hydrogenation.

Publications

Dynamic structural evolution of iron catalysts involving competitive oxidation and carburization during CO<sub>2</sub> hydrogenation.

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