La0.4Sr0.6CoO3-Catalyzed Selective Oxidation of Ethylbenzene to Acetophenone without Solvent: A New Reactive Oxygen Species Transformation Mechanism Mediated by •O2– Derived from 1O2 DOI

Weiwen Mao,

Jiaheng Qin,

Miao Li

et al.

ACS Sustainable Chemistry & Engineering, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 20, 2024

Developing a green, stable, and cost-effective heterogeneous catalyst clarifying its catalytic mechanism for the selective oxidation of C–H bonds without solvent to carbonyl compounds hold significant theoretical practical value. Herein, we synthesize perovskite catalysts using sol–gel method catalyze ethylbenzene. Notably, La0.4Sr0.6CoO3-800 (800 °C is calcination temperature catalyst) demonstrates remarkable efficacy, converting 73% ethylbenzene into acetophenone with selectivity 93%. Characterization analyses reveal that incorporation strontium moderately disrupts internal balance structure, leading increased oxygen vacancies enhanced adsorption capacity. Moreover, electron paramagnetic resonance mechanistic studies prove molecular on surface converted singlet (1O2) superoxide radical anions (•O2–). The presence 1O2 significantly aids in production •O2–, thereby effectively promoting This research introduces new reactive species (ROS) transformation provides valuable insights hydrocarbons.

Language: Английский

Screening of Cu-Based Catalysts for Selective Methane to Methanol Conversion DOI
Erwei Huang, Ping Liu

The Journal of Physical Chemistry C, Journal Year: 2024, Volume and Issue: 128(19), P. 7876 - 7883

Published: May 3, 2024

Developing selective catalysts for methane conversion to value-added chemicals has been considered a promising approach efficient utilization of abundant natural gas resources. Here, we present descriptor-based screening high and methanol selectivity at the interfaces between metal oxide clusters Cu2O/Cu(111) support [MOx/Cu2O/Cu(111), M = Mg, Fe, Co, Ni, Cu, Zn, Ti, Zr, Sn, Ce] on exposure mixture CH4/O2/H2O. The activation energy direct conversion, *OH + *CH4 → *CH3OH *H, ratio adsorption oxygen water, Eads(O2)/Eads(H2O), are identified as effective descriptors selectivity, respectively. By providing exceptional hydroxyl sites with high-lying O 2p states, MgO/Cu2O/Cu(111) catalyst is found be most system among systems studied, being able provide highest selectivity.

Language: Английский

Citations

1
Direct Methane to Methanol Conversion Technologies Methods, Applications, and Future Prospects DOI

Saeed Gandomi,

Mohammad Reza Rahimpour

Elsevier eBooks, Journal Year: 2024, Volume and Issue: unknown

Published: Jan. 1, 2024

Language: Английский

Citations

1
Economic Analysis of Direct Methane to Methanol DOI

Liza Ainalén Dosso

Elsevier eBooks, Journal Year: 2024, Volume and Issue: unknown

Published: Jan. 1, 2024

Language: Английский

Citations

0
Photocatalytic CH4 Upgrading to Multicarbon Products DOI
Shuya Hao, Qing Han, Gengfeng Zheng

et al.

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(22), P. 16673 - 16686

Published: Oct. 29, 2024

Methane is both a greenhouse gas and an abundant C1 fuel resource that exists in nature. The selective photocatalytic upgrading of methane into multicarbon (C2+) chemicals can mitigate the effect promote utilization value methane, which C–C coupling step key to production products. Achieving this targeted under ambient temperature pressure conditions requires efficient activation C–H bonds as well balancing adsorption desorption various free radicals intermediates facilitate coupling. In Review, we delve recent advances C2+ importance catalyst design, including active site assembly, crystal surface, valence reconstruction, first emphasized. Then, discuss how coreactants such carbon dioxide monoxide be introduced enhance chain growth pathways. Furthermore, also summarize developments looping systems photoelectrocatalysis. Finally, conclude with outlook for future advancement field. This Review aims provide general framework investigating reactions toward products, thereby suggesting research directions environmentally friendly strategies.

Language: Английский

Citations

0
La0.4Sr0.6CoO3-Catalyzed Selective Oxidation of Ethylbenzene to Acetophenone without Solvent: A New Reactive Oxygen Species Transformation Mechanism Mediated by •O2– Derived from 1O2 DOI

Weiwen Mao,

Jiaheng Qin,

Miao Li

et al.

ACS Sustainable Chemistry & Engineering, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 20, 2024

Developing a green, stable, and cost-effective heterogeneous catalyst clarifying its catalytic mechanism for the selective oxidation of C–H bonds without solvent to carbonyl compounds hold significant theoretical practical value. Herein, we synthesize perovskite catalysts using sol–gel method catalyze ethylbenzene. Notably, La0.4Sr0.6CoO3-800 (800 °C is calcination temperature catalyst) demonstrates remarkable efficacy, converting 73% ethylbenzene into acetophenone with selectivity 93%. Characterization analyses reveal that incorporation strontium moderately disrupts internal balance structure, leading increased oxygen vacancies enhanced adsorption capacity. Moreover, electron paramagnetic resonance mechanistic studies prove molecular on surface converted singlet (1O2) superoxide radical anions (•O2–). The presence 1O2 significantly aids in production •O2–, thereby effectively promoting This research introduces new reactive species (ROS) transformation provides valuable insights hydrocarbons.

Language: Английский

Citations

0