Selective Photo-oxidation of Methane to Methanol with Oxygen over Dual-Cocatalyst-Modified Titanium Dioxide DOI Creative Commons
Hui Song, Xianguang Meng, Shengyao Wang

et al.

ACS Catalysis, Journal Year: 2020, Volume and Issue: 10(23), P. 14318 - 14326

Published: Nov. 23, 2020

Direct and selective oxidation of CH4 with dioxygen to methanol is a "dream reaction" in modern catalysis yet remains great challenge. Here, we report that TiO2 loaded dual cocatalysts, is, nanometals cobalt oxide (CoOx) nanoclusters, capable selectively catalyzing CH3OH at room temperature under photoexcitation using abundant inexpensive O2 as an oxidant. The best activity for the formation primary products, CH3OOH CH3OH, up 50.8 μmol 2 h 95% selectivity. Mechanistic studies elucidate superior selectivity result from synergistic effect CoOx. Nanometals enhance conversion by promoting separation photoexcited electron reduction O2. CoOx mediates mild process suppressing highly oxidative •OH radicals can further oxidize HCHO CO2, thereby preserving high toward oxygenated products. This work provides prototype designing efficient photocatalysts conditions.

Language: Английский

Methane Oxidation to Methanol DOI Creative Commons
Nicholas F. Dummer, David J. Willock, Qian He

et al.

Chemical Reviews, Journal Year: 2022, Volume and Issue: 123(9), P. 6359 - 6411

Published: Dec. 2, 2022

The direct transformation of methane to methanol remains a significant challenge for operation at larger scale. Central this is the low reactivity conditions that can facilitate product recovery. This review discusses issue through examination several promising routes and an evaluation performance targets are required develop process We explore methods currently used, emergence active heterogeneous catalysts their design reaction mechanisms provide critical perspective on future operation. Initial experiments discussed where identification gas phase radical chemistry limited further development by approach. Subsequently, new class catalytic materials based natural systems such as iron or copper containing zeolites were explored milder conditions. key issues these technologies conversion often overoxidation products. Despite this, interest high in wider appeal effective route products from C–H activation, particularly with need transition net carbon zero renewable sources exciting.

Language: Английский

Citations

170
Toward efficient single-atom catalysts for renewable fuels and chemicals production from biomass and CO2 DOI Creative Commons
Yubing Lu, Zihao Zhang, Huamin Wang

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2021, Volume and Issue: 292, P. 120162 - 120162

Published: March 20, 2021

Language: Английский

Citations

165
Synergetic interaction between neighboring platinum and ruthenium monomers boosts CO oxidation DOI Creative Commons
Peng Zhou,

Xingang Hou,

Yuguang Chao

et al.

Chemical Science, Journal Year: 2019, Volume and Issue: 10(23), P. 5898 - 5905

Published: Jan. 1, 2019

The synergetic effect between neighboring Pt and Ru monomers supported on N vacancy-rich g-C3N4 promotes the catalytic CO oxidation.

Language: Английский

Citations

153
Prospects of Heterogeneous Hydroformylation with Supported Single Atom Catalysts DOI

Jonas Amsler,

Bidyut Bikash Sarma, Giovanni Agostini

et al.

Journal of the American Chemical Society, Journal Year: 2020, Volume and Issue: 142(11), P. 5087 - 5096

Published: March 6, 2020

The potential of oxide-supported rhodium single atom catalysts (SACs) for heterogeneous hydroformylation was investigated both theoretically and experimentally. Using high-level domain-based local-pair natural orbital coupled cluster singles doubles with perturbative triples contribution (DLPNO-CCSD(T)) calculations, stability catalytic activity were Rh atoms on different oxide surfaces. Atomically dispersed, supported synthesized MgO CeO2. While the CeO2-supported catalyst is found to be highly active, this not case MgO, most likely due increased confinement, as determined by extended X-ray absorption fine structure spectroscopy (EXAFS), that diminishes reactivity complexes MgO. This agrees well our computational investigation, where we find carbonyl hydride flat surfaces such CeO2(111) have activities comparable those molecular complexes. For a step edge MgO(301) surface, however, calculations show significantly reduced activity. At same time, predict stronger adsorption at higher coordinated site leads more stable catalyst. Keeping balance between appears main challenge catalysts. In addition chemical bonding complex support, confinement experienced active plays an important role

Language: Английский

Citations

152
Selective Photo-oxidation of Methane to Methanol with Oxygen over Dual-Cocatalyst-Modified Titanium Dioxide DOI Creative Commons
Hui Song, Xianguang Meng, Shengyao Wang

et al.

ACS Catalysis, Journal Year: 2020, Volume and Issue: 10(23), P. 14318 - 14326

Published: Nov. 23, 2020

Direct and selective oxidation of CH4 with dioxygen to methanol is a "dream reaction" in modern catalysis yet remains great challenge. Here, we report that TiO2 loaded dual cocatalysts, is, nanometals cobalt oxide (CoOx) nanoclusters, capable selectively catalyzing CH3OH at room temperature under photoexcitation using abundant inexpensive O2 as an oxidant. The best activity for the formation primary products, CH3OOH CH3OH, up 50.8 μmol 2 h 95% selectivity. Mechanistic studies elucidate superior selectivity result from synergistic effect CoOx. Nanometals enhance conversion by promoting separation photoexcited electron reduction O2. CoOx mediates mild process suppressing highly oxidative •OH radicals can further oxidize HCHO CO2, thereby preserving high toward oxygenated products. This work provides prototype designing efficient photocatalysts conditions.

Language: Английский

Citations

152