Citation: WANG Zeng-zhu, HUANG Shou-ying, SHEN Yong-li, WANG Sheng-ping, MA Xin-bin. In situ DRIFTS study on the oxidative carbonylation of methanol to dimethyl carbonate over Cuβ catalyst[J]. Journal of Fuel Chemistry and Technology, ;2012, 40(10): 1212-1221. shu

In situ DRIFTS study on the oxidative carbonylation of methanol to dimethyl carbonate over Cuβ catalyst

1.
Key Lab for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China

Corresponding author: WANG Sheng-ping,
Received Date: 27 March 2012
Available Online: 25 May 2012
Fund Project: 国家自然科学基金(20876112,20936003) (20876112,20936003) 高等学校博士学科点专项科研基金(20090032110021) (20090032110021) 高等学校学科创新引智计划(B06006)。 (B06006)

The mechanism of oxidative carbonylation of methanol to dimethyl carbonate (DMC) over Cuβ catalyst was investigated by using in situ DRIFTS; the adsorption of single methanol, carbon monoxide and DMC as well as their mixtures on the Cuβ catalyst were considered. The results indicated that methoxide species are formed when methanol is adsorbed on the catalyst due to presence of CuO_<em>x. Only one type of active sites that are located in the six-membered ring of β zeolite is found, over which adsorbed methanol can be oxidized to methoxide and water. DMC is adsorbed on the catalyst through the contact of the oxygen atom in carbonyl group with the active sites. There were two pathways for the oxidative carbonylation: by the mono-methoxide pathway, carbon monoxide can react with mono-methoxide species to form monomethyl carbonate (MMC) and MMC then reacts with methoxide to form DMC, or by the di-methoxide pathway, DMC is formed through inserting of carbon monoxide in the di-methoxide species; latter one is more favorable over the Cuβ catalyst.
- Cuβ,
- oxidative carbonylation,
- DMC,
- mechanism,
- in situ DRIFTS
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