Role of active oxygen species in Fe-doped ZrO2 catalyst during CO2 assisted ethane dehydrogenation reaction

Zheng, Yingbin; Zhang, Xinbao; Li, Junjie; An, Jie; Zhu, Xiangxue; Li, Xiujie

doi:10.1016/j.jcat.2023.115130

Cited by 8 publications

(2 citation statements)

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“…Those Co 0 species were coated by coke layers during dehydrogenation reactions using lower feeding CO 2 /C 2 H 6 ratios (Figure a,c), consequently the dry-reforming reaction was suppressed. Co 0 species maintained a higher activity due to the rapid removal of deposited coke species by increasing co-feeding CO 2 concentration. , The amount of Co nanoclusters over spent Co/S-1 after the reaction with a feeding CO 2 /ethane ratio of 4.0 slightly decreased (Figure S9). However, the HR-TEM images in Figures a and S10 illustrate that both oxidative and metallic Co nanoparticles were deposited over the Silicalite-1 surface.…”

Section: Resultsmentioning

confidence: 99%

Evolution of Co Species in CO₂-Assisted Ethane Dehydrogenation: Competing Cleavage of C–H and C–C Bonds

Zheng,

Li,

Zhang

et al. 2024

ACS Catal.

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Integrating CO 2 into alkane dehydrogenation reactions provides an effective strategy to improve the metal catalyst stability. The structural evolution of supported metal species, particularly in a mild oxidation atmosphere, plays an important role in catalytic performance.Here, the influence of the introduction of CO 2 on the state of Co species and the corresponding dehydrogenation performance over Co/Silicalite-1 was investigated in detail. The manipulation of the CO 2 /C 2 H 6 feeding ratios dictated the selective bond breakage of either C−H or C−C in ethane, which was derived from the differentiated nanostructuring of Co species during reactions through a series of designed control-reaction tests and characterization results. At a CO 2 /C 2 H 6 feeding ratio of 4.0, Co nanoparticles underwent a transformation into active metallic Co species, which facilitated dry-reforming reaction with an ethene selectivity below 2%. When the CO 2 /C 2 H 6 feeding ratio was below 2.0, the generation of active metallic Co species was suppressed and the dehydrogenation reaction dominated over the Co 2+ sites. The effective suppression of reduction and sintering of active Co 2+ species led to a stable dehydrogenation performance lasting over 120 h, with ethene selectivity consistently exceeding 95% during this period. The elucidation of the state changes of Co species holds significant implications for the design of dehydrogenation catalysts.

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Section: Resultsmentioning

confidence: 99%

Evolution of Co Species in CO₂-Assisted Ethane Dehydrogenation: Competing Cleavage of C–H and C–C Bonds

Zheng,

Li,

Zhang

et al. 2024

ACS Catal.

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“…CaO showed no reduction peaks during H 2 -TPR, indicating that it did not affect the identification of other reducible species. 23,24 In the H 2 -TPR patterns of the FC and CZ catalysts, two reduction peaks were observed (Figure 3a). For CZ, the first peak at 285 °C and the second peak at 532 °C were attributed to the weak and strong interaction of ZrO 2 with CaO, respectively.…”

Section: ■ Experimental Sectionmentioning

confidence: 99%

In Situ Capture and Conversion of CO₂ to CO Using CaZrO₃ Promoted Fe–CaO Dual-Functional Material

Gao,

Yuan,

Yang

et al. 2024

ACS Sustainable Chem. Eng.

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The urgent need to address global warming has led researchers to investigate various methods for capturing and utilizing CO 2 . One promising approach is the integration of calcium looping (CaL) and reverse water−gas shift (RWGS) reactions. Therefore, dual functional materials enriched with CaZrO 3 were introduced as effective catalysts, exhibiting a sustainable catalytic CO 2 conversion to 100% CO selectivity and a remarkable CO 2 adsorption capacity (16.69 mmol g DFM −1 ), CO yield (9.64 mmol g DFM −1), even under low hydrogen concentration (15% H 2 ) in CaL and RWGS processes. Surface chemistry analysis revealed that oxygen vacancies, acting adsorption sites, and lattice oxygen of CaZrO 3 can be activated by hydrogen. This activation, linked to the formation of strong basic sites with Zr 4+ -O 2− , significantly enhanced CO 2 conversion efficiency. The synergistic promotion mechanism was validated through in situ X-ray diffraction, DRIFTS, and Raman spectroscopy techniques. The bidentate formate mechanism was predominant, indicating that bicarbonates and hydroxyl synergistic promote CO 2 conversion in the high-temperature CaL−RWGS process. 10FCZ−5 showed good long-time stability, and the material maintained a high dispersion of Fe species after 10 cycles, demonstrating excellent absorbent capacity (11 mmol g DFM −1) and CO yield (6.2 mmol g DFM −1 ).

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Regulation of catalytic reaction performance of CO2 with ethane by metal cation substitution on CeO2 support

Li,

Kang,

et al. 2024

Chemical Engineering Journal

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Role of active oxygen species in Fe-doped ZrO2 catalyst during CO2 assisted ethane dehydrogenation reaction

Cited by 8 publications

References 47 publications

Evolution of Co Species in CO₂-Assisted Ethane Dehydrogenation: Competing Cleavage of C–H and C–C Bonds

Evolution of Co Species in CO₂-Assisted Ethane Dehydrogenation: Competing Cleavage of C–H and C–C Bonds

In Situ Capture and Conversion of CO₂ to CO Using CaZrO₃ Promoted Fe–CaO Dual-Functional Material

Regulation of catalytic reaction performance of CO2 with ethane by metal cation substitution on CeO2 support

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Role of active oxygen species in Fe-doped ZrO2 catalyst during CO2 assisted ethane dehydrogenation reaction

Cited by 8 publications

References 47 publications

Evolution of Co Species in CO2-Assisted Ethane Dehydrogenation: Competing Cleavage of C–H and C–C Bonds

Evolution of Co Species in CO2-Assisted Ethane Dehydrogenation: Competing Cleavage of C–H and C–C Bonds

In Situ Capture and Conversion of CO2 to CO Using CaZrO3 Promoted Fe–CaO Dual-Functional Material

Regulation of catalytic reaction performance of CO2 with ethane by metal cation substitution on CeO2 support

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Evolution of Co Species in CO₂-Assisted Ethane Dehydrogenation: Competing Cleavage of C–H and C–C Bonds

Evolution of Co Species in CO₂-Assisted Ethane Dehydrogenation: Competing Cleavage of C–H and C–C Bonds

In Situ Capture and Conversion of CO₂ to CO Using CaZrO₃ Promoted Fe–CaO Dual-Functional Material