Photo-Driven Aerobic Methane Nitration

被引：4

作者：

He, Xuefeng ^{[1
]}

Zhang, Lina ^{[1
]}

Chen, Jiawei ^{[1
]}

Liu, Huichong ^{[1
]}

Su, Yuming ^{[1
]}

Li, Han ^{[1
]}

Cao, Yonghua ^{[1
]}

Dral, Pavlo O. ^{[1
,2
,3
]}

Wang, Cheng ^{[1
,2
]}

机构：

[1] Xiamen Univ, Coll Chem & Chem Engn, Dept Chem, State Key Lab Phys Chem Solid Surfaces,iChem, Xiamen 361005, Peoples R China

[2] Xiamen Univ, Innovat Lab Sci & Technol Energy Mat Fujian Prov I, Xiamen 361005, Peoples R China

[3] Xiamen Univ, Fujian Prov Key Lab Theoret & Computat Chem, Xiamen 361005, Peoples R China

来源：

INORGANIC CHEMISTRY | 2023年 / 62卷 / 26期

基金：

中国国家自然科学基金;

关键词：

ABSORPTION CROSS-SECTIONS; PARTIAL OXIDATION; ALKYL NITRATE; LIGHT ALKANES; TEMPERATURE-DEPENDENCE; THERMAL-DECOMPOSITION; ATMOSPHERIC CHEMISTRY; SELECTIVE OXIDATION; PRESSURE-DEPENDENCE; HYDROGEN-PEROXIDE;

D O I：

10.1021/acs.inorgchem.3c01210

中图分类号：

O61 [无机化学];

学科分类号：

070301 ; 081704 ;

摘要：

Aphoto-driven method has been developed to selectivelyconvert methane to methyl nitrates (CH3ONO2)using visible light, via the chlorine radical hydrogen atom-transfercycle and nitration. The NO2 was recyclable through hydrolysis,and CH3OH can be obtained. Conversionof methane to liquid oxygenates is challenging but ofgreat value. Here, we report the oxidation of methane (CH4) to methanol (CH3OH) assisted by nitrogen dioxide (NO2) as a photo-mediator and using molecular oxygen (O-2) as the terminal oxidant. Similar photoreactions are widely studiedin atmospheric chemistry but were not previously used in preparativemethane conversion. We used visible light to excite NO2 generated by heating aluminum nitrate Al(NO3)(3) and drove its reaction with methane and O-2 to producemethyl nitrate (CH3ONO2), which is then hydrolyzedto CH3OH. Nitric acid (HNO3) and nitrate (NO3 (-)) were produced and recycled back to Al(NO3)(3), completing a chemical loop. HCl can catalyzethis photochemical process via relay hydrogen atom-transfer reactions,with up to 17% methane conversion and 78% CH3ONO2 selectivity. This simple photochemical system provides new opportunitiesin selective methane transformation.

引用

页码：10343 / 10350

页数：8

共 98 条

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