Effect of Sr Incorporation and Ni Exsolution on Coke Resistance of the Ni/Sr–Al<sub>2</sub>O<sub>3</sub> Catalyst for Dry Reforming of Methane

Kim, Jeongmin; Seo, Jeong-Cheol; Jang, Won-Jun; Lee, Kyubock

doi:10.1021/acssuschemeng.3c05275

Cited by 7 publications

(1 citation statement)

References 57 publications

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“…A temperature-programmed reverse Boudouard reaction was performed for the study of the required initiation temperatures, and the apparent activation energies of catalyst regeneration by CO 2 utilization (i.e., for the spent catalyst after the first-stage isothermal methane decomposition at 600 °C, E a,CO 2 ) were calculated. The activity of the reverse Boudouard reaction is known to be strongly dependent on the morphology and crystallinity of carbon to be gasified. , In comparison to carbon film/encapsulated carbon, whisker carbon is expected to exhibit a higher removal efficiency because of the larger exposed surface area of carbon structures, enhancing accessibility of CO 2 and thus improving carbon removal efficiency . In our study, the carbon structure was varied with the composition of the catalyst samples.…”

Section: Resultsmentioning

confidence: 95%

Combined Methane Cracking for H₂ Production with CO₂ Utilization for Catalyst Regeneration Using Dual Functional Nanostructured Particles

Zeng,

Law,

Tsai

2024

ACS Sustainable Chem. Eng.

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A two-stage chemical looping approach is demonstrated for sustainable hydrogen production through methane decomposition (CH 4 → C + 2H 2 ) combined with cyclic catalyst regeneration via the reverse Boudouard reaction (C + CO 2 → 2CO). A Nibased spherical nanoparticle cluster, fabricated using a continuous aerosol-based synthetic approach, is developed for effective cyclic catalysis of the above two chemical reactions. A sufficiently high CO 2 conversion rate for catalyst regeneration (in terms of TOF CO 2 , 36.09 h −1 ) and a stably high yield of hydrogen (in terms of STY H 2 , 5.19 mmol g cat −1 min −1 ) are achievable using the 10Ni−1Ce/5Al sample. The outstanding performance of 10Ni−1Ce/ 5Al is attributed to the incorporation of CeO 2 as a promoter, which possesses a high redox ability that enhances catalytic activity.Additionally, the synergistic effect between nickel and ceria on the two-stage chemical looping is of crucial importance, where CeO 2 promotes CO 2 capture and Ni catalyzes CO 2 dissociation at the Ni−CeO 2 interface. CeO 2 -incorporated samples generating whisker carbon after methane pyrolysis demonstrate better activity for cyclic catalyst regeneration. The novelty of the work stands on developing a high-performance dual functional nanostructured catalyst using an aerosol-based synthetic route. This approach creates a massive amount of active interface, by which the two-stage reactions can be promoted under a remarkably low temperature (e.g., 600 °C). The proposed dual functional catalyst material and catalytic pathway demonstrate significant advances for effective hydrogen production combined with cyclic catalyst regeneration via CO 2 utilization, offering an eco-friendly pathway for industrial applications.

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Section: Resultsmentioning

confidence: 95%

Combined Methane Cracking for H₂ Production with CO₂ Utilization for Catalyst Regeneration Using Dual Functional Nanostructured Particles

Zeng,

Law,

Tsai

2024

ACS Sustainable Chem. Eng.

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Unbounding the Future: Designing NiAl‐Based Catalysts for Dry Reforming of Methane

Zhang,

Zhao,

Song

et al. 2024

Chemistry An Asian Journal

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Dry reforming of methane (DRM), the catalytic conversion of CH4 and CO2 into syngas (H2 + CO), is an important process closely correlated to the environment and chemical industry. NiAl‐based catalysts have been reported to exhibit excellent activity, low cost, and environmental friendliness. At the same time, the rapid deactivation caused by carbon deposition, Ni sintering, and phase transformation exerts great challenges for its large‐scale applications. This review summarizes the recent advances in NiAl‐based catalysts for DRM, particularly focusing on the strategies to construct efficient and stable NiAl‐based catalysts. Firstly, the thermodynamics and elementary steps of DRM, including the activation of reactants and coke formation and elimination, are summarized. The roles of Al2O3 and its mixed oxides as the support, and the influences of the promoters employed in NiAl‐based catalysts over the DRM performance, are then illustrated. Finally, the design of anti‐coking and anti‐sintering NiAl‐based catalysts for DRM is suggested as feasible and promising by tailoring the structure and states of Ni and the modification of Al‐based supports including small Ni size, high Ni dispersion, proper basicity, strong metal‐support interaction (SMSI), active oxygen species as well as high phase stability.

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On the Selection of Catalysts’ Support with High Oxygen Delivery Capacity for DRM Application: Interest of Praseodymium as Dopant of Ceria

Herráez-Santos,

Goma-Jiménez,

Yeste-Sigüenza

et al. 2024

Top Catal

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In the present work, a series of supports with varying compositions (ranging from pure CeO2 to pure PrO2-y) was designed to investigate their ability to release oxygen (with the concomitant formation of oxygen vacancies) under diverse reducing atmospheres: hydrogen (H2), helium (He), and in the presence of a carbonaceous substance that mimics eventual carbon deposits formed under practical reaction conditions (DRM). Oxygen vacancies were generated effectively in all three atmospheres (following the order He < H2 < carbon material). With regard to the influence of the composition, the capability to generate oxygen vacancies clearly increased with the Pr content, for whatever the conditions tested. Notably, the non-stoichiometry obtained with the support of pure praseodymia in both inert and reducing atmospheres is very remarkable, as it approaches the maximum non-stoichiometry value of the well-established theoretical Bevan cluster. This leads to consider this formulation as a very promising support for applications in catalysis and other fields where oxygen vacancies play a crucial role. Dry Reforming of Methane requires catalytic supports that possess highly mobile oxygen, enabling it to actively participate in the reactions step involved or potentially gasify undesirable carbon deposits generated during parallel reactions. Consequently, designing and elucidating the behavior of ceria-praseodymium-based supports with high reducibility and generation of oxygen vacancies (oxygen storage and release capacity) holds particular relevance in this context. Actually, the very preliminary results comparing two counterpart formulations (5%Ni/PrO2-y versus 5%Ni/Al2O3) already confirm the suitability of the choice of pure praseodymia in terms of activity, stability and very high selectivity towards H2 and CO, reaching a very close value to the ideal H2/CO ratio of 1.

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Effect of Sr Incorporation and Ni Exsolution on Coke Resistance of the Ni/Sr–Al₂O₃ Catalyst for Dry Reforming of Methane

Cited by 7 publications

References 57 publications

Combined Methane Cracking for H₂ Production with CO₂ Utilization for Catalyst Regeneration Using Dual Functional Nanostructured Particles

Combined Methane Cracking for H₂ Production with CO₂ Utilization for Catalyst Regeneration Using Dual Functional Nanostructured Particles

Unbounding the Future: Designing NiAl‐Based Catalysts for Dry Reforming of Methane

On the Selection of Catalysts’ Support with High Oxygen Delivery Capacity for DRM Application: Interest of Praseodymium as Dopant of Ceria

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Effect of Sr Incorporation and Ni Exsolution on Coke Resistance of the Ni/Sr–Al2O3 Catalyst for Dry Reforming of Methane

Cited by 7 publications

References 57 publications

Combined Methane Cracking for H2 Production with CO2 Utilization for Catalyst Regeneration Using Dual Functional Nanostructured Particles

Combined Methane Cracking for H2 Production with CO2 Utilization for Catalyst Regeneration Using Dual Functional Nanostructured Particles

Unbounding the Future: Designing NiAl‐Based Catalysts for Dry Reforming of Methane

On the Selection of Catalysts’ Support with High Oxygen Delivery Capacity for DRM Application: Interest of Praseodymium as Dopant of Ceria

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Effect of Sr Incorporation and Ni Exsolution on Coke Resistance of the Ni/Sr–Al₂O₃ Catalyst for Dry Reforming of Methane

Combined Methane Cracking for H₂ Production with CO₂ Utilization for Catalyst Regeneration Using Dual Functional Nanostructured Particles

Combined Methane Cracking for H₂ Production with CO₂ Utilization for Catalyst Regeneration Using Dual Functional Nanostructured Particles