Phase transformation of iron oxide to carbide and Fe<sub>3</sub>C as an active center for the RWGS reaction

Liu, Yang; Murthy, Palle Ramana; Zhang, Xiao; Wang, Haiyan; Shi, Chuan

doi:10.1039/d1nj04120g

Cited by 28 publications

(23 citation statements)

References 25 publications

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“…In the case of Fe wool and Fe wool@SiO 2 , at ∼350 °C, the X CO 2 was <7% and S CO was ∼97%. This result agrees with previous reports, which show that Fe is an active catalyst for reverse water gas shift (RWGS) reaction. − Upon addition of the Siralox in the catalytic bed, the X CO 2 rose to ∼20%, whereas S CH 4 was found to be <1%. The powder XRD analysis of the spent catalysts (Fe wool and the Fe wool@SiO 2 ) is shown in Figure S14 (details discussed in the SI).…”

Section: Resultssupporting

confidence: 93%

“…Similarly, after 4 h of catalysis, a new contribution is observed at 706.8 eV in the Fe 2p XPS region, which can also be attributed to Fe 3 C (Figure S18, details in the SI). For iron, upon exposure to the CO and H 2 , the formation of iron carbide is evident during the Fischer–Tropsch process. ,, In the case of the Fe wool@Ni catalyst, one can assume that CO 2 gets adsorbed both on Ni and Fe. Considering that Ni particles catalyze both the RWGS and the methanation reactions, at higher reaction temperatures, in a CO-rich atmosphere, iron can form the Fe 3 C phase.…”

Section: Resultsmentioning

confidence: 99%

“…This hydrogen further accelerates the O removal from the Fe surfaces and facilitates the carbide formation in hydrogen-rich conditions (H 2 /CO 2 = 4) . It is reported that iron carbide is an active phase in the RWGS reaction . Hence, Fe wool@Ni catalyzes both the RWGS and the methanation reactions, but with the additional contribution of the Fe 3 C active phase, the overall methane selectivity of the catalyst decreases.…”

Section: Resultsmentioning

confidence: 99%

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Fe@SiO₂@Ni: An Iron-Based Composite Material for Magnetically Induced Hydrogenation Reactions in Gas and Solution Phases

Ghosh,

Ourlin,

Mazarío

et al. 2023

Chem. Mater.

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Recently, magnetically induced catalytic CO2 hydrogenation has gained attention due to its high energy efficiency and better heat management of exothermic processes compared to thermal heating. Ferromagnetic nanoparticles combining heating and catalytic properties are shown to be efficient, but the complex synthesis procedure limits their potential as industrial products. In this work, commercially available iron (Fe) wool was chemically modified by a sol–gel coating of a silica (SiO2) layer followed by nickel (Ni) particle deposition and employed as a catalyst for magnetically induced gas-phase CO2 hydrogenation reaction. The composite material was thoroughly characterized by combined X-ray photoelectron spectroscopy (XPS), focused ion beam scanning electron microscopy (FIB-SEM), and magnetic and specific absorption rate (SAR) measurements as well as its catalytic activity. This material shows an enhanced catalytic activity (higher CO2 conversion and CH4 selectivity) compared to Ni-only-coated iron wool, which could be attributed to the stabilization of the composite catalyst. Adding a Siralox filler in the catalytic bed further improves CO2 conversion, CH4 selectivity, and catalyst stability. Furthermore, this composite catalyst is demonstrated to be active for solution-phase model hydrogenation and hydrodeoxygenation reactions, thus anticipating its potential for a broader range of catalytic applications in organic chemistry.

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Section: Resultssupporting

confidence: 93%

Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

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Fe@SiO₂@Ni: An Iron-Based Composite Material for Magnetically Induced Hydrogenation Reactions in Gas and Solution Phases

Ghosh,

Ourlin,

Mazarío

et al. 2023

Chem. Mater.

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“…As per the literature, , this α-Fe 2 O 3 under N 2 atmosphere may convert to Fe 3 C (cohenite) as follows: 3Fe 2 O 3 + 5H 2 + 2CH 4 = 2Fe 3 C + 9H 2 O 3Fe 2 O 3 + 13H 2 + 2CO 2 = 2Fe 3 C + 13H 2 O …”

Section: Resultsmentioning

confidence: 74%

Solid-State Reaction of Ferrocene Controlled by Co-Precursor and Reaction Atmosphere Leading to Hematite and Cohenite Nanomaterials: A Reaction Kinetic Study

Kundu,

Chakraborty,

Bhattacharjee

2023

J. Phys. Chem. C

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The present article investigates the thermal decomposition of ferrocene in the presence of oxalic acid dihydrate in oxidative and inert atmospheres. A mixture of ferrocene and oxalic acid dihydrate on thermal decomposition in O 2 and N 2 atmospheres produces hematite and cohenite nanomaterials, respectively. These decompositions are complex and reflected through multiple overlapped reaction steps in the thermogravimetry profiles, and peak deconvolution method is adopted to separate the reaction steps involved. It is found that the synthesis of hematite is a two-step process, while that of cohenite is a one-step process. Model-free integral isoconversional methods are adopted to estimate the values of activation energy for these thermal reactions. The most probable reaction mechanism and the reaction rate of thermal decomposition are determined by an intercept-based model fitting method. The reaction mechanism is found to be different for different steps. To verify the suitability of the adopted kinetic models, the experimental conversion curves are compared with the reversely constructed ones and the agreement is quite reasonable. The conversion dependence of thermodynamic parameters is obtained using the estimated kinetic parameters. Comparing the estimated values of the kinetic and thermodynamic parameters, the effect of the reaction atmosphere on the thermal decomposition process of ferrocene is realized. Utilizing the kinetic and thermodynamic parameters conversion-dependent nucleation rates of the reaction steps have been estimated. The present study describes how different nanomaterials of iron can be synthesized starting with the same precursor material, how the reaction (solid and gaseous) atmosphere affects the reaction profile and the residual material, and finally, how kinetic calculations help in understanding the solid state reaction process involved. This study suggests the use suitable combination of precursor, co-precursor, and gaseous reaction atmosphere for the solid-state thermal synthesis of iron-based nanoparticles using organo-iron compounds. The study also highlights the successful application of the peak-deconvolution method.

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“…Reduction and conversion of CO 2 into small organic molecules or hydrocarbons can not only alleviate global warming caused by the greenhouse effect, but also provide a new way to meet future energy demand. 1 Hydrogenation products of CO 2 mainly include methanol (CH 3 OH), 2–5 methane (CH 4 ), 6,7 formic acid (HCOOH), 8–10 dimethyl ether (CH 3 OCH 3 ), 11–13 and CO. 14–18 CO is used to produce liquid fuels such as olefin and polyol through the Fischer–Tropsch (FT) process and other mature processes. 19–24 Methanol is a liquid solar fuel, and it is highly significant to realize the hydrogenation of CO 2 to methanol.…”

Section: Introductionmentioning

confidence: 99%

Mechanism of CO₂ hydrogenation over a Zr₁–Cu single-atom catalyst

Liu

Wang

et al. 2022

New J. Chem.

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Phase transformation of iron oxide to carbide and Fe₃C as an active center for the RWGS reaction

Abstract: Fe3C was produced from iron oxide and identified as active and stable in the reverse water gas shift reaction.

Cited by 28 publications

References 25 publications

Fe@SiO₂@Ni: An Iron-Based Composite Material for Magnetically Induced Hydrogenation Reactions in Gas and Solution Phases

Fe@SiO₂@Ni: An Iron-Based Composite Material for Magnetically Induced Hydrogenation Reactions in Gas and Solution Phases

Solid-State Reaction of Ferrocene Controlled by Co-Precursor and Reaction Atmosphere Leading to Hematite and Cohenite Nanomaterials: A Reaction Kinetic Study

Mechanism of CO₂ hydrogenation over a Zr₁–Cu single-atom catalyst

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Phase transformation of iron oxide to carbide and Fe3C as an active center for the RWGS reaction

Abstract: Fe3C was produced from iron oxide and identified as active and stable in the reverse water gas shift reaction.

Cited by 28 publications

References 25 publications

Fe@SiO2@Ni: An Iron-Based Composite Material for Magnetically Induced Hydrogenation Reactions in Gas and Solution Phases

Fe@SiO2@Ni: An Iron-Based Composite Material for Magnetically Induced Hydrogenation Reactions in Gas and Solution Phases

Solid-State Reaction of Ferrocene Controlled by Co-Precursor and Reaction Atmosphere Leading to Hematite and Cohenite Nanomaterials: A Reaction Kinetic Study

Mechanism of CO2 hydrogenation over a Zr1–Cu single-atom catalyst

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Phase transformation of iron oxide to carbide and Fe₃C as an active center for the RWGS reaction

Fe@SiO₂@Ni: An Iron-Based Composite Material for Magnetically Induced Hydrogenation Reactions in Gas and Solution Phases

Fe@SiO₂@Ni: An Iron-Based Composite Material for Magnetically Induced Hydrogenation Reactions in Gas and Solution Phases

Mechanism of CO₂ hydrogenation over a Zr₁–Cu single-atom catalyst