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Selenium-doped hierarchically porous carbon nanosheets as an efficient metal-free electrocatalyst for CO2 reduction
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Prof. Zhang Jianling’ group from the Institute of Chemistry of Chinese Academy of Sciences propose the hierarchically macroporous, mesoporous and microporous carbon nanosheets (CNs) doped with selenium (Se) for efficient electrochemical CO2RR. Such an electrocatalyst possesses hierarchical pores for facilitating reactant or ion penetration, transport and reaction, and large surface area for easily accessible active sites, which make the total current density of CO2RR significantly increased. Owing to the Se optimized active sites towards the reduction of CO2 to CO, the Se-CNs electrocatalyst exhibits over 10-times enhanced partial current density of CO than the CNs without Se doping and high selectivity (90%) for CO2 electroreduction to CO. The result was published at Adv. Funct. Mater. (Adv. Funct. Mater., 29, 1906194, 2019). The synchrotron radiation techniques (BSRF 1W2A and 1W1B) were used to reveal the formation of porous structure and the deep atomic structure information in Se-CNs. The XANES and EXAFS results combined with X-ray photoelectron spectroscopy reveal the bonding situation of Se, C and N, which provide a strong support for the model establishment of the activity center and further theoretical calculation. Moreover, small angle X-ray scattering (SAXS) characterization of carbon materials obtained under different synthesis conditions prove that the pore size can be significantly regulated by controlling the amount of selenium introduced in the synthesis process, indicating that SeO2 plays a key role in the formation of hierarchically porous structure.

Fig. Morphological and structural characterization (a-c) of Se-CNs and its performances for electrocatalytic CO2 reduction (e-f). The compassion samples were non-porous carbon nanosheets (CNs) and bulk carbon materials (CB).

Article

Bingxing Zhang, Jianling Zhang,* Fanyu Zhang, Lirong Zheng, Guang Mo, Buxing Han, and Guanying Yang. Selenium-Doped Hierarchically Porous Carbon Nanosheets as an Efficient Metal-Free Electrocatalyst for CO2 Reduction. Adv. Funct. Mater., 2019, 29, 1906194.

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