The steady increased CO2 concentration due to fossil fuel consumption and human activities in the atmosphere is considered a major contributor to frequent occurrence of extreme climate condition.&lt;span style="font-size:10.8333px"&gt; &lt;/span&gt;Catalytic conversion of CO2 to high value chemicals addresses both climate change and fossil fuel shortage but requires energy inputs. Abundant shale gas makes CH4 a perfect hydrogen and energy sources for CO2 conversion. CH4 and CO2 are both C1 sources and could be used as primary sources to build hydrocarbons and oxygenates. However, the challenges in selectively breaking a minimal number of C−H bonds in CH4 and coupling with activated CO2 prevents the realization of such direct coupling processes. In this report, we demonstrated that a Zn site doped in the CeO2 surface acted as an active site for the C−H bond activation in CH4 and allowed insertion of CO2 into the C-Zn bond. The insertion of CO2 into Zn−CH3 bond follows a three-centered Zn-C-C moiety and has a moderate activation barrier of 0.51 eV. Further study demonstrated that the CH3 species stabilized the Zn site can couple with the acetate species if an active Zn site ensemble is in presence in a CeO2-based catalyst. The coupling of CH3* with CH3COO* resulted in acetone. The later provided an alternative route to produce acetone and avoided emission of CO2 of the traditional process. These findings provide new approach to produce C2 and C3 oxygenates from CO2 and CH4 as the building blocks.

Using CO2 and CH4 as C1 building blocks to produce value-added product through C-C coupling

255th National Meeting (2018)

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