Highly Selective Photoelectroreduction of Carbon Dioxide to Ethanol over Graphene/Silicon Carbide Composites

Guanghui Feng; Shibin Wang; Shenggang Li; Ruipeng Ge; Xuefei Feng; Junwei Zhang; Yanfang Song; Xiao Dong; Jiazhou Zhang; Gaofeng Zeng; Qiang Zhang; Guijun Ma; Yi-De Chuang; Xixiang Zhang; Jinghua Guo; Yuhan Sun; Wei Wei; Wei Chen

doi:10.1002/anie.202218664

Highly Selective Photoelectroreduction of Carbon Dioxide to Ethanol over Graphene/Silicon Carbide Composites

Angew Chem Int Ed Engl. 2023 Apr 3;62(15):e202218664. doi: 10.1002/anie.202218664. Epub 2023 Mar 2.

Authors

Guanghui Feng^{1

2}, Shibin Wang^{1

3}, Shenggang Li^{1

2

4}, Ruipeng Ge^{1

4}, Xuefei Feng⁵, Junwei Zhang⁶, Yanfang Song¹, Xiao Dong¹, Jiazhou Zhang^{1

4}, Gaofeng Zeng^{1

2}, Qiang Zhang⁶, Guijun Ma⁴, Yi-De Chuang⁵, Xixiang Zhang⁶, Jinghua Guo⁵, Yuhan Sun^{1

2

4}, Wei Wei^{1

2

4}, Wei Chen^{1

2}

Affiliations

¹ Low-Carbon Conversion Science and Engineering Center, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai, 201210, P. R. China.
² University of Chinese Academy of Sciences, Beijing, 100049, P. R. China.
³ Institute of Industrial Catalysis, State Key Laboratory Breeding Base of Green-Chemical Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, 310032, P. R. China.
⁴ School of Physical Science and Technology, ShanghaiTech University, Shanghai, 201203, P. R. China.
⁵ Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.
⁶ Division of Physical Science and Engineering, King Abdullah University of Science and Technology, Thuwal, 23955-6900, Saudi Arabia.

PMID: 36787047
DOI: 10.1002/anie.202218664

Abstract

Using sunlight to produce valuable chemicals and fuels from carbon dioxide (CO₂ ), i.e., artificial photosynthesis (AP) is a promising strategy to achieve solar energy storage and a negative carbon cycle. However, selective synthesis of C₂ compounds with a high CO₂ conversion rate remains challenging for current AP technologies. We performed CO₂ photoelectroreduction over a graphene/silicon carbide (SiC) catalyst under simulated solar irradiation with ethanol (C₂ H₅ OH) selectivity of>99 % and a CO₂ conversion rate of up to 17.1 mmol g_cat ^-1 h^-1 with sustained performance. Experimental and theoretical investigations indicated an optimal interfacial layer to facilitate the transfer of photogenerated electrons from the SiC substrate to the few-layer graphene overlayer, which also favored an efficient CO₂ to C₂ H₅ OH conversion pathway.

Keywords: CO2 Photoelectroreduction; Ethanol Selectivity; Graphene/Silicon Carbide; Promoting C−C Coupling.

Abstract

Grants and funding