Maximizing Active Fe Species in ZSM-5 Zeolite Using Organic-Template-Free Synthesis for Efficient Selective Methane Oxidation DOI Creative Commons
Qingpeng Cheng, Guanna Li,

Xueli Yao

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(10), P. 5888 - 5898

Published: Feb. 14, 2023

The selective oxidation of CH4 in the aqueous phase to produce valuable chemicals has attracted considerable attention due its mild reaction conditions and simple process. As most widely studied catalyst for this reaction, Fe-ZSM-5 demonstrates high intrinsic activity selectivity; however, prepared using conventional methods a limited number active Fe sites, resulting low conversion per unit mass catalyst. This study reports facile organic-template-free synthesis strategy that enables incorporation more into zeolite framework with higher dispersion degree compared methods. Because incorporated way is readily transformed isolated extra-framework species under thermal treatment, overall effect method (Fe-HZ5-TF) 3 times as many catalytically sites Fe-ZSM-5. When used 0.5 M H2O2 at 75 °C, Fe-HZ5-TF produced C1 oxygenate yield 109.4 mmol gcat-1 h-1 (a HCOOH selectivity 91.1%), surpassing other catalysts reported date. Spectroscopic characterization density functional theory calculations revealed are mononuclear form [(H2O)3Fe(IV)═O]2+ bound Al pairs framework. differs from Fe-ZSM-5, where binuclear acts site. Analysis product evolution during suggests radical-driven pathway explain activation site subsequent oxygenates.

Language: Английский

Methane selective oxidation to methanol by metal-exchanged zeolites: a review of active sites and their reactivity DOI
Muhammad Haris Mahyuddin, Yoshihito Shiota, Kazunari Yoshizawa

et al.

Catalysis Science & Technology, Journal Year: 2019, Volume and Issue: 9(8), P. 1744 - 1768

Published: Jan. 1, 2019

A review of the recent progress in revealing structures, formation, and reactivity active sites Fe-, Co-, Ni- Cu-exchanged zeolites as well outlooks on future research challenges opportunities is presented.

Language: Английский

Citations

168
Activation and conversion of alkanes in the confined space of zeolite-type materials DOI
Pablo del Campo, Cristina Martı́nez, Avelino Corma

et al.

Chemical Society Reviews, Journal Year: 2021, Volume and Issue: 50(15), P. 8511 - 8595

Published: Jan. 1, 2021

Microporous zeolite-type materials are able to activate and efficiently convert stable C1+alkanes. This review analyzes, at the molecular level, role of active sites contribution diffusion, shape-selectivity confinement effects.

Language: Английский

Citations

136
Highly Selective Oxidation of Methane into Methanol over Cu-Promoted Monomeric Fe/ZSM-5 DOI
Tao Yu, Zhi Li, Lu Lin

et al.

ACS Catalysis, Journal Year: 2021, Volume and Issue: 11(11), P. 6684 - 6691

Published: May 21, 2021

The selective oxidation of methane into methanol is paramount importance but poses significant challenges in achieving high productivity and selectivity, especially under mild reaction conditions. We show that a Cu-modified monomeric Fe/ZSM-5 catalyst highly efficient material for the direct conversion liquid phase using H2O2 as an oxidant at low temperatures, which exhibits excellent 431 molMeOH·mol–1Fe·h–1 (with selectivity ∼80% over Cu-Fe(2/0.1)/ZSM-5 catalyst). Combining control experiments comprehensive characterization results by among others, Mössbauer spectroscopy, electron paramagnetic resonance well density functional theory calculations, we found Cu species play pivotal role facilitating formation •OH radicals, quickly react with •CH3 radicals to form CH3OH. These findings provide valuable insights rational design metal–zeolite combinations methanol.

Language: Английский

Citations

110
Chemical looping-based energy transformation via lattice oxygen modulated selective oxidation DOI
Zhao Sun, Christopher K. Russell, Kevin J. Whitty

et al.

Progress in Energy and Combustion Science, Journal Year: 2023, Volume and Issue: 96, P. 101045 - 101045

Published: Feb. 10, 2023

Language: Английский

Citations

84
Maximizing Active Fe Species in ZSM-5 Zeolite Using Organic-Template-Free Synthesis for Efficient Selective Methane Oxidation DOI Creative Commons
Qingpeng Cheng, Guanna Li,

Xueli Yao

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(10), P. 5888 - 5898

Published: Feb. 14, 2023

The selective oxidation of CH4 in the aqueous phase to produce valuable chemicals has attracted considerable attention due its mild reaction conditions and simple process. As most widely studied catalyst for this reaction, Fe-ZSM-5 demonstrates high intrinsic activity selectivity; however, prepared using conventional methods a limited number active Fe sites, resulting low conversion per unit mass catalyst. This study reports facile organic-template-free synthesis strategy that enables incorporation more into zeolite framework with higher dispersion degree compared methods. Because incorporated way is readily transformed isolated extra-framework species under thermal treatment, overall effect method (Fe-HZ5-TF) 3 times as many catalytically sites Fe-ZSM-5. When used 0.5 M H2O2 at 75 °C, Fe-HZ5-TF produced C1 oxygenate yield 109.4 mmol gcat-1 h-1 (a HCOOH selectivity 91.1%), surpassing other catalysts reported date. Spectroscopic characterization density functional theory calculations revealed are mononuclear form [(H2O)3Fe(IV)═O]2+ bound Al pairs framework. differs from Fe-ZSM-5, where binuclear acts site. Analysis product evolution during suggests radical-driven pathway explain activation site subsequent oxygenates.

Language: Английский

Citations

45