Chinese Journal of Catalysis ›› 2021, Vol. 42 ›› Issue (9): 1608-1616.DOI: 10.1016/S1872-2067(20)63776-7
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Fang Lia,b, Xiaoyang Yuea, Haiping Zhouc, Jiajie Fand, Quanjun Xianga,b,*()
Received:
2021-01-12
Accepted:
2021-02-01
Online:
2021-09-18
Published:
2021-05-16
Contact:
Quanjun Xiang
About author:
* Tel/Fax: +86-28-83207063; E-mail: xiangqj@uestc.edu.cnSupported by:
Fang Li, Xiaoyang Yue, Haiping Zhou, Jiajie Fan, Quanjun Xiang. Construction of efficient active sites through cyano-modified graphitic carbon nitride for photocatalytic CO2 reduction[J]. Chinese Journal of Catalysis, 2021, 42(9): 1608-1616.
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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(20)63776-7
Fig. 1. (a) Schematic of MCN-0.5 synthesis; (b,c) TEM images of MCN-0.5; (d) STEM images of MCN-0.5; STEM image (e) and elemental mapping images (f-i) of MCN-0.5 corresponding to C, N, O, and K. During the thermal polymerization process, the OH- released when KOH melted reacted with the amino groups at the edge of g-C3N4 to introduce cyano groups, and ethanol molecules acted as intercalation molecules and were released in the form of gas, leaving pores in the nanosheets.
Fig. 2. (a,b) SEM images of MCN-0.5; (c,d) SEM images of MCN. The introduction of cyano groups did not affect the morphology of the porous nanosheets of the photocatalyst.
Fig. 3. (a) Solid-state 13C NMR spectra of MCN-0.5 and TCN-0.5. (b) FTIR spectra of MCN-0.5 and MCN. (c) XRD patterns of MCN-0.5 and MCN. (d) UV-vis DRS spectra of MCN-0.5, MCN, and TCN (inset exhibits the plots of the calculated band gaps).
Fig. 5. The yields of CO (a) and CH4 (b) reduced by CO2, CO and CH4 evolution rate (c), and turnover numbers (TONs) of CO (d) generation over MCN-0.5, MCN, and TCN.
Fig. 6. (a) FTIR spectra of MCN-0.5, MCN-0.5 (spent), and MCN-0.5-HCl; (b) CO evolution rate over MCN-0.5 and MCN-0.5-HCl and corresponding SEM images (inset) of MCN-0.5 and MCN-0.5-HCl; (c,d) TEM images of MCN-0.5 loaded with Pt nanoparticles (MCN-0.5-Pt); (e,f) TEM images of MCN deposited with Pt nanoparticles (MCN-Pt). MCN-0.5-Pt and MCN-Pt were prepared by the photo-reduction method.
Fig. 7. CO2 adsorption isotherms of MCN (a) and MCN-0.5 (b) at 273 K and 298 K; In situ DRIFT spectra of MCN-0.5 under dark environment (c) and light irradiation (d).
Fig. 9. (a) TRPL spectra of MCN-0.5, MCN, and TCN; (b) EPR spectra of MCN-0.5 and MCN; EIS Nyquist curves (c), and transient photocurrent response plots (d) of MCN-0.5, MCN, and TCN.
Fig. 10. Proposed mechanism of MCN-0.5 for photocatalytic CO2 conversion. The cyano group was grafted onto the MCN-0.5 as an electron acceptor. Besides, the cyano group possesses good electron-withdrawing properties, improving carrier separation, and acting as an active site to participate in the photocatalytic CO2 reduction reaction.
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