Efficient electroreduction of CO2 to CO by Ag-decorated S-doped g-C3N4/CNT nanocomposites at industrial scale current density

被引:58
作者
Chen, J. [1 ]
Wang, Z. [1 ,2 ]
Lee, H. [1 ,3 ]
Mao, J. [1 ]
Grimes, C. A. [4 ]
Liu, C. [1 ]
Zhang, M. [1 ]
Lu, Z. [2 ]
Chen, Y. [1 ]
Feng, S. -P. [1 ]
机构
[1] Univ Hong Kong, Dept Mech Engn, Pokfulam, Pokfulam Rd, Hong Kong 999077, Peoples R China
[2] Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen, Peoples R China
[3] Sun Yat Sen Univ, Dept Photon, Kaohsiung 80424, Taiwan
[4] Flux Photon Corp, 5950 Shiloh Rd East, Alpharetta, GA 30005 USA
关键词
CO2; reduction; Electrocatalyst; Nanocomposites; Flow cell; GRAPHITIC CARBON NITRIDE; METAL-FREE ELECTROCATALYST; TOTAL-ENERGY CALCULATIONS; AB-INITIO; ATMOSPHERIC CO2; REDUCTION; NANOTUBES; DIOXIDE; CONVERSION; COMPOSITE;
D O I
10.1016/j.mtphys.2019.100176
中图分类号
T [工业技术];
学科分类号
08 ;
摘要
In recent years, the application of graphitic carbon nitride (g-C3N4) for electrochemical CO2 reduction reaction (eCO(2)RR) has aroused strong interest. However, this material is still facing severe activity issue towards eCO(2)RR so far, and studies on its catalytic mechanism have not been sufficiently implemented either. Herein, we report an Ag-decorated sulfur-doped graphitic carbon nitride/carbon nanotube nanocomposites (Ag-S-C3N4/CNT) for efficient eCO(2)RR to carbon monoxide (CO). The resulting Ag-S eC(3)N(4)/CNT catalyst exhibits a notable performance in eCO(2)RR, yielding a high current density of similar to 21.3 mA/cm(2) at similar to 0.77 VRHE and maximum CO Faradaic efficiency over 90% in H-type cell. Strikingly, when combining with flow cell configuration, the fabricated nanocomposites permit an industrial scale and cost-effective eCO(2)RR, showing a current density larger than 200 mA/cm(2) and the Faradaic efficiency of CO over 80% in a wide potential window, delivering the best eCO(2)RR performance among the C3N4-derivatives. Moreover, the catalytic mechanism of this nanocomposite has been further explored through density functional theory (DFT) and electrochemical methods carefully. Our work not only sheds light on industrial scale eCO(2)RR to CO but also leads to new insights on the application of C3N4-based composite materials in electrocatalytic processes. (c) 2019 Elsevier Ltd. All rights reserved.
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页数:10
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