High catalytic activity of Ti-porphyrin for NO reduction by CO: a first-principles study

Harrath, Karim; Boughdiri, Salima

doi:10.1007/s11164-017-3146-6

Cited by 8 publications

(1 citation statement)

References 49 publications

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“…But how can one control the spacing of active sites? Metal–organic frameworks (MOFs) have unique features, such as excellent tailorability, well-defined porous structures, good designability, and ultrahigh surface areas, which can be the best choice. − Moreover, the MOF materials have previously been demonstrated to be active for a range of catalytic reactions, including methane activation. ,− In addition, single-atom catalysts have aroused considerable interest in heterogeneous catalysis in the past decades due to their maximum atom utilization, unique electronic properties, and great potential for high selectivity. − Hence, MOF-supported single metal atom catalysts (SACs) can be considered as a potential material for both controlling the catalyst architecture and tuning the electronic properties.…”

Section: Introductionmentioning

confidence: 99%

Tailoring the Active-Site Spacing of a Single-Atom Catalyst for CH₄-to-CH₃OH Conversion: The Co₁/UiO-66 MOF as an Exemplary Model

Harrath,

Yao,

Jiang

et al. 2024

J. Phys. Chem. C

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Developing catalysts for the mild and selective oxidation of methane to methanol (CH 4 -to-CH 3 OH) is a challenging yet crucial endeavor for the industry. In this study, we propose a strategy to enhance the selective methane oxidation reaction, focusing on the crucial step of metal-oxo active-site formation. Our findings demonstrate that optimizing the spacing between active metal sites can facilitate efficient charge transfer from the metal sites to O 2 , thereby kinetically enhancing O 2 activation and leading to the formation of highly reactive O (oxo) species capable of activating the methane C−H bond. Through the screening of different metals at varying metal site spacings, we find that the Co single atom exhibits favorable properties and performance, characterized by the duality of a low O 2 activation energy and the radical character of the formed metal-oxo species. Utilizing a Co single-atom catalyst dispersed on the UiO-66 MOF as a probe catalyst, we have showcased the potential of tailoring the active-site spacing to enhance the activity and selectivity toward methane oxidation to methanol. Notably, the newly designed catalyst surpasses the activity of a known catalyst, achieving an observable turnover frequency (>1 s −1 site −1 ) at 350 K while also enhancing its selectivity by inhibiting continuous methane dehydrogenation. This strategic approach could provide valuable insights for further exploration of MOF-supported singleatom catalysts or other support morphologies for the selective oxidation of CH 4 to CH 3 OH with excellent activity in the gas phase.

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Section: Introductionmentioning

confidence: 99%

Tailoring the Active-Site Spacing of a Single-Atom Catalyst for CH₄-to-CH₃OH Conversion: The Co₁/UiO-66 MOF as an Exemplary Model

Harrath,

Yao,

Jiang

et al. 2024

J. Phys. Chem. C

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Reversible lewisite adsorption/desorption on the transition-metal-doped graphene: first-principle calculations

Liu

Holiharimanana

et al. 2023

Res Chem Intermed

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Arsenical compound lewisite was developed to be a potent chemical warfare agent in the blister agent class and was abandoned in the war areas. Exposure to lewisite can cause serious damage to human's skin, eyes and respiratory tract. Therefore, it is essential for scienti c researchers to design materials that can detect and remove the abandoned lewisite e ciently. In the present work, the potential of transition metals doped (TM = Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu and Zn) graphene (TM/G) to eliminate lewisite is investigated by the rst-principles calculations based on density functional theory. The adsorption geometry, adsorption energy, charge transfer, density of states and UV spectra of adsorption system of lewisite on TM/G (L@TM/G)are calculated and analyzed. Computational results demonstrate that there is a strong chemical interaction between TM/G substrate and lewisite molecule. More importantly, the adsorption of lewisite on TM/G can be regulated by introducing an electric eld with proper direction and intensity, and therefore the reversible adsorption/desorption can be achieved. In addition, the electronic and optical properties of TM/G change signi cantly after lewisite adsorption, making TM/G promising to detect lewisite agent. The work predicts that TM/G is a potential sensor and renewable adsorbent for lewisite.

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Understanding the direct methane conversion to oxygenates on graphene-supported single 3d metal atom catalysts

2023

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High catalytic activity of Ti-porphyrin for NO reduction by CO: a first-principles study

Cited by 8 publications

References 49 publications

Tailoring the Active-Site Spacing of a Single-Atom Catalyst for CH₄-to-CH₃OH Conversion: The Co₁/UiO-66 MOF as an Exemplary Model

Tailoring the Active-Site Spacing of a Single-Atom Catalyst for CH₄-to-CH₃OH Conversion: The Co₁/UiO-66 MOF as an Exemplary Model

Reversible lewisite adsorption/desorption on the transition-metal-doped graphene: first-principle calculations

Understanding the direct methane conversion to oxygenates on graphene-supported single 3d metal atom catalysts

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High catalytic activity of Ti-porphyrin for NO reduction by CO: a first-principles study

Cited by 8 publications

References 49 publications

Tailoring the Active-Site Spacing of a Single-Atom Catalyst for CH4-to-CH3OH Conversion: The Co1/UiO-66 MOF as an Exemplary Model

Tailoring the Active-Site Spacing of a Single-Atom Catalyst for CH4-to-CH3OH Conversion: The Co1/UiO-66 MOF as an Exemplary Model

Reversible lewisite adsorption/desorption on the transition-metal-doped graphene: first-principle calculations

Understanding the direct methane conversion to oxygenates on graphene-supported single 3d metal atom catalysts

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Product

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Tailoring the Active-Site Spacing of a Single-Atom Catalyst for CH₄-to-CH₃OH Conversion: The Co₁/UiO-66 MOF as an Exemplary Model

Tailoring the Active-Site Spacing of a Single-Atom Catalyst for CH₄-to-CH₃OH Conversion: The Co₁/UiO-66 MOF as an Exemplary Model