The study of structure-performance relationship of iron catalyst during a full life cycle for CO2 hydrogenation

Zhang, Yulong; Cao, Chenxi; Zhang, Chao; Zhang, Zhengpai; Liu, Xianglin; Yang, Zixu; Zhu, Minghui; Meng, Bo; Xu, Jing; Han, Yi‐Fan

doi:10.1016/j.jcat.2019.08.001

Cited by 72 publications

(48 citation statements)

References 75 publications

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“…That is, the ability to catalyze C 2+ production ranks as Fe 5 C 2 > Fe 3 C >> Fe 3 O 4 . Density functional theory (DFT) investigations showed that CO 2 activation is more facile on Fe 5 C 2 and Fe 3 C than on Fe 3 O 4 (45,46), and Han and colleagues (27,39) found that the transition of Fe 5 C 2 to Fe 3 O 4 causes the deactivation in CO 2 hydrogenation. From the comparison on the performance over model catalysts and Fe NPs with different TOS (Fig.…”

Section: Surface Structurementioning

confidence: 99%

Dynamic structural evolution of iron catalysts involving competitive oxidation and carburization during CO ₂ hydrogenation

et al. 2022

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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 CO 2 hydrogenation to hydrocarbons has been investigated by using several (quasi) in situ techniques. Upon initial reduction, Fe species are carburized to Fe 3 C and then to Fe 5 C 2 . The by-product of CO 2 hydrogenation, H 2 O, oxidizes the iron carbide to Fe 3 O 4 . The formation of Fe 3 O 4 @(Fe 5 C 2 +Fe 3 O 4 ) 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 CO 2 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 Fe 5 C 2 -rich surface for a desired C 2+ productivity.

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Section: Surface Structurementioning

confidence: 99%

Dynamic structural evolution of iron catalysts involving competitive oxidation and carburization during CO ₂ hydrogenation

et al. 2022

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“…An alternative explanation for the lower carbon conversion could be the oxidation of iron phases on the catalyst surface. CO 2 and H 2 O are known to have an oxidizing effect and thereby deactivate conventional iron‐based catalysts [25,32,52] …”

Section: Resultsmentioning

confidence: 99%

Using Biomass Gasification Mineral Residue as Catalyst to Produce Light Olefins from CO, CO₂, and H₂ Mixtures

et al. 2022

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Gasification is a process to transform solids, such as agricultural and municipal waste, into gaseous feedstock for making transportation fuels. The so-called coarse solid residue (CSR) that remains after this conversion process is currently discarded as a process solid residue. In the context of transitioning from a linear to a circular society, the feasibility of using the solid process residue from waste gasification as a solid catalyst for light olefin production from CO, CO 2 , and H 2 mixtures was investigated. This CSR-derived catalyst converted biomass-derived syngas, a H 2 -poor mixture of CO, CO 2 , H 2 , and N 2 , into methane (57 %) and C 2 -C 4 olefins (43 %) at 450 °C and 20 bar. The main active ingredient of CSR was Fe, and it was discovered with operando X-ray diffraction that metallic Fe, present after pre-reduction in H 2 , transformed into an Fe carbide phase under reaction conditions. The increased formation of Fe carbides correlated with an increase in CO conversion and olefin selectivity. The presence of alkali elements, such as Na and K, in CSR-derived catalyst increased olefin production as well.

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“…The nature of the active phase of iron catalysts are still under debate due to the dynamic character of the active phases during CO 2 hydrogenation, originating from the complex interactions between the gaseous species (CO 2 , CO, H 2 ) and the iron phases [41]. It is well known that the activity, selectivity and/or stability of the catalyst depend on the type of active phases, the formation of which depends on the process conditions, the activation procedure and the catalyst composition.…”

Section: Dynamic Character Of the Catalytically Active Iron Phasesmentioning

confidence: 99%

“…The correlation between the catalyst activity and the types of phases formed suggested that the Fe5C2 phase was responsible for the formation of C2 = -C4 = olefins. Since the iron carbide phases were irreversibly oxidized to Fe3O4, the loss of this phase was the main factor leading to catalyst deactivation (Figure 6) [41]. 100), ( 110), ( 111) and (211).…”

Section: Dynamic Character Of the Catalytically Active Iron Phasesmentioning

confidence: 99%

“…The iron phases transition during the activation → reaction → deactivation → regeneration life cycle of the iron catalyst was investigated by Zhang et al [41]. After the whole life cycle (Figure 6), the catalyst still showed 91.8% of the initial activity and 97.7% of its initial selectivity toward C 2 -C 4 = olefins.…”

Section: Dynamic Character Of the Catalytically Active Iron Phasesmentioning

confidence: 99%

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Catalysts for the Conversion of CO2 to Low Molecular Weight Olefins—A Review

et al. 2021

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There is a large worldwide demand for light olefins (C2=–C4=), which are needed for the production of high value-added chemicals and plastics. Light olefins can be produced by petroleum processing, direct/indirect conversion of synthesis gas (CO + H2) and hydrogenation of CO2. Among these methods, catalytic hydrogenation of CO2 is the most recently studied because it could contribute to alleviating CO2 emissions into the atmosphere. However, due to thermodynamic reasons, the design of catalysts for the selective production of light olefins from CO2 presents different challenges. In this regard, the recent progress in the synthesis of nanomaterials with well-controlled morphologies and active phase dispersion has opened new perspectives for the production of light olefins. In this review, recent advances in catalyst design are presented, with emphasis on catalysts operating through the modified Fischer–Tropsch pathway. The advantages and disadvantages of olefin production from CO2 via CO or methanol-mediated reaction routes were analyzed, as well as the prospects for the design of a single catalyst for direct olefin production. Conclusions were drawn on the prospect of a new catalyst design for the production of light olefins from CO2.

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The study of structure-performance relationship of iron catalyst during a full life cycle for CO2 hydrogenation

Cited by 72 publications

References 75 publications

Dynamic structural evolution of iron catalysts involving competitive oxidation and carburization during CO ₂ hydrogenation

Dynamic structural evolution of iron catalysts involving competitive oxidation and carburization during CO ₂ hydrogenation

Using Biomass Gasification Mineral Residue as Catalyst to Produce Light Olefins from CO, CO₂, and H₂ Mixtures

Catalysts for the Conversion of CO2 to Low Molecular Weight Olefins—A Review

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The study of structure-performance relationship of iron catalyst during a full life cycle for CO2 hydrogenation

Cited by 72 publications

References 75 publications

Dynamic structural evolution of iron catalysts involving competitive oxidation and carburization during CO 2 hydrogenation

Dynamic structural evolution of iron catalysts involving competitive oxidation and carburization during CO 2 hydrogenation

Using Biomass Gasification Mineral Residue as Catalyst to Produce Light Olefins from CO, CO2, and H2 Mixtures

Catalysts for the Conversion of CO2 to Low Molecular Weight Olefins—A Review

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Dynamic structural evolution of iron catalysts involving competitive oxidation and carburization during CO ₂ hydrogenation

Dynamic structural evolution of iron catalysts involving competitive oxidation and carburization during CO ₂ hydrogenation

Using Biomass Gasification Mineral Residue as Catalyst to Produce Light Olefins from CO, CO₂, and H₂ Mixtures