Tailored pore-confined single-site iron(III) catalyst for selective CH4 oxidation to CH3OH or CH3CO2H using O2 DOI Creative Commons

Manav Chauhan,

Bharti Rana,

Poorvi Gupta

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Nov. 12, 2024

Direct oxidation of methane to valuable oxygenates like alcohols and acetic acid under mild conditions poses a significant challenge due high C‒H bond dissociation energy, facile overoxidation CO CO2 the intricacy C−H activation/C−C coupling. In this work, we develop multifunctional iron(III) dihydroxyl catalytic species immobilized within metal-organic framework (MOF) for selective into methanol or at different reaction using O2. The active-site isolation monomeric FeIII(OH)2 MOF nodes, their confinement porous framework, electron-deficient nature facilitate chemoselective oxidation, yielding with productivities $$38,592\,\upmu {{{\rm{mol}}}}_{{{{\rm{CH}}}}_{3}{{\rm{OH}}}}{{{{\rm{g}}}}_{{{\rm{Fe}}}}}^{-1}{{{\rm{h}}}}^{-1}$$ $$81,043\,\upmu {{{\rm{mol}}}}_{{{{\rm{CH}}}}_{3}{{{\rm{CO}}}}_{2}{{\rm{H}}}}{{{{\rm{g}}}}_{{{\rm{Fe}}}}}^{-1}{{{\rm{h}}}}^{-1}$$ , respectively. Experiments theoretical calculations suggest that formation occurs via FeIII-FeI-FeIII cycle, whereas CH3CO2H is produced hydrocarboxylation in-situ generated CH3OH H2, direct CH4 carboxylation CO2. development technology value-added products highly lucrative. Here, supported mono iron(III)-dihydroxyl catalyst selectively oxidizes only oxygen, where hydrocarboxylation.

Language: Английский

Modulation of Al Sites in MWW Zeolites with Enhanced Catalytic Performance by Dual Organic Structure-Directing Agents DOI Creative Commons
Chuang Liu, Guodong Qi,

Yudan Gong

et al.

Chem & Bio Engineering, Journal Year: 2025, Volume and Issue: unknown

Published: April 10, 2025

Language: Английский

Citations

0
Deciphering the intricate mechanisms behind the selective oxidation of methane to C1 and C2 oxygenates over FeAu/γ-Al2O3 catalysts DOI

Marimuthu Prabu,

Marimuthu Manikandan,

B. Sathya Sai Rengam

et al.

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: 512, P. 162510 - 162510

Published: April 17, 2025

Language: Английский

Citations

0
Metal-zeolite catalysts promoting low-temperature methane oxidation to oxygenates DOI Open Access
Bingbing Xiang, Jialiang Li,

Bokun Chang

et al.

Chemical Synthesis, Journal Year: 2025, Volume and Issue: 5(3)

Published: April 17, 2025

Catalytic conversion of methane (CH4) into value-added chemicals provides a viable path to reduce dependency on crude oil. Despite the challenges associated with activating methane’s C–H bond and limiting side reactions, low-temperature oxidation oxygenates has emerged as promising approach, often hailed “grail reaction”. Zeolite-based metal (metal-zeolite) catalysts facilitate at low temperatures, converting while minimizing complete carbon dioxide (CO2). This review highlights recent achievements in metal-zeolite for partial coupling oxidation. With zeolite core, we explore synthesis methods, metallic active sites, reaction mechanisms, descriptors Additionally, examine critical role mono- bi-metallic species monoxide (CO). Finally, discuss opportunities under mild conditions, proposing future directions rational design catalysts, revealing mechanisms through operando or situ techniques, leveraging artificial intelligence (AI) enhanced catalytic efficiency.

Language: Английский

Citations

0
ZSM-48 zeolite catalysts for hydroisomerization of linear paraffins, diesel and sustainable aviation fuels production: synthesis, characterization, and application DOI
Yamen Aljajan,

Valentin Stytsenko,

Maria Rubtsova

et al.

Catalysis Reviews, Journal Year: 2025, Volume and Issue: unknown, P. 1 - 37

Published: April 23, 2025

Language: Английский

Citations

0
Insight into bifunctional synergistic action for n-octane dehydrocracking with Au-Sn/MWW zeolite and kinetic modeling DOI
Chenyu Guo,

Bingbing Luo,

Tengwei Chen

et al.

Chemical Engineering Science, Journal Year: 2025, Volume and Issue: unknown, P. 121836 - 121836

Published: May 1, 2025

Language: Английский

Citations

0
Decatungstate-doped Ce-MOF for methane photooxidation DOI
Cheng Yao, Wenxiong Shi, Zhiming Zhang

et al.

Chinese Chemical Letters, Journal Year: 2024, Volume and Issue: unknown, P. 110387 - 110387

Published: Sept. 1, 2024

Language: Английский

Citations

0
Tailored pore-confined single-site iron(III) catalyst for selective CH4 oxidation to CH3OH or CH3CO2H using O2 DOI Creative Commons

Manav Chauhan,

Bharti Rana,

Poorvi Gupta

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Nov. 12, 2024

Direct oxidation of methane to valuable oxygenates like alcohols and acetic acid under mild conditions poses a significant challenge due high C‒H bond dissociation energy, facile overoxidation CO CO2 the intricacy C−H activation/C−C coupling. In this work, we develop multifunctional iron(III) dihydroxyl catalytic species immobilized within metal-organic framework (MOF) for selective into methanol or at different reaction using O2. The active-site isolation monomeric FeIII(OH)2 MOF nodes, their confinement porous framework, electron-deficient nature facilitate chemoselective oxidation, yielding with productivities $$38,592\,\upmu {{{\rm{mol}}}}_{{{{\rm{CH}}}}_{3}{{\rm{OH}}}}{{{{\rm{g}}}}_{{{\rm{Fe}}}}}^{-1}{{{\rm{h}}}}^{-1}$$ $$81,043\,\upmu {{{\rm{mol}}}}_{{{{\rm{CH}}}}_{3}{{{\rm{CO}}}}_{2}{{\rm{H}}}}{{{{\rm{g}}}}_{{{\rm{Fe}}}}}^{-1}{{{\rm{h}}}}^{-1}$$ , respectively. Experiments theoretical calculations suggest that formation occurs via FeIII-FeI-FeIII cycle, whereas CH3CO2H is produced hydrocarboxylation in-situ generated CH3OH H2, direct CH4 carboxylation CO2. development technology value-added products highly lucrative. Here, supported mono iron(III)-dihydroxyl catalyst selectively oxidizes only oxygen, where hydrocarboxylation.

Language: Английский

Citations

0