Regulation of functional groups on graphene quantum dots directs selective CO2 to CH4 conversion

Tianyu Zhang, Weitao Li, Kai Huang, Huazhang Guo, Zhengyuan Li, Yanbo Fang, Ram Manohar Yadav, Vesselin Shanov, Pulickel M. Ajayan, Liang Wang (), Cheng Lian () and Jingjie Wu ()
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Tianyu Zhang: University of Cincinnati
Weitao Li: Shanghai University
Kai Huang: East China University of Science and Technology
Huazhang Guo: Shanghai University
Zhengyuan Li: University of Cincinnati
Yanbo Fang: University of Cincinnati
Ram Manohar Yadav: Rice University
Vesselin Shanov: University of Cincinnati
Pulickel M. Ajayan: Rice University
Liang Wang: Shanghai University
Cheng Lian: East China University of Science and Technology
Jingjie Wu: University of Cincinnati

Nature Communications, 2021, vol. 12, issue 1, 1-9

Abstract: Abstract A catalyst system with dedicated selectivity toward a single hydrocarbon or oxygenate product is essential to enable the industrial application of electrochemical conversion of CO2 to high-value chemicals. Cu is the only known metal catalyst that can convert CO2 to high-order hydrocarbons and oxygenates. However, the Cu-based catalysts suffer from diverse selectivity. Here, we report that the functionalized graphene quantum dots can direct CO2 to CH4 conversion with simultaneous high selectivity and production rate. The electron-donating groups facilitate the yield of CH4 from CO2 electro-reduction while electron-withdrawing groups suppress CO2 electro-reduction. The yield of CH4 on electron-donating group functionalized graphene quantum dots is positively correlated to the electron-donating ability and content of electron-donating group. The graphene quantum dots functionalized by either –OH or –NH2 functional group could achieve Faradaic efficiency of 70.0% for CH4 at −200 mA cm−2 partial current density of CH4. The superior yield of CH4 on electron-donating group- over the electron-withdrawing group-functionalized graphene quantum dots possibly originates from the maintenance of higher charge density of potential active sites (neighboring C or N) and the interaction between the electron-donating group and key intermediates. This work provides insight into the design of active carbon catalysts at the molecular scale for the CO2 electro-reduction.

Date: 2021
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DOI: 10.1038/s41467-021-25640-1

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