One step method of structure engineering porous graphitic carbon nitride for efficient visible-light photocatalytic reduction of Cr(VI)

doi:10.1016/j.jmst.2020.09.008

Abstract

Abstract:

Porous g-C₃N₄ nanosheets (PCN) were prepared by the nickel-assisted one-step thermal polymerization method. Hydrogen (H₂) which was produced by the reaction between nickel (Ni) foam and ammonia (NH₃) defined the structure and properties of PCN. During the formation of PCN, the participation of H₂ not only enhanced the spacing between layers but also boosted the specific surface area that more active sites were exposed. Additionally, H₂ promoted pores formation in the nanosheets, which was beneficial to the transfer of photons through lamellar structure and improved the absorption efficiency of visible light. Remarkably, the obtained PCN possessed better Cr(VI) photocatalytic reduction efficiency than pure g-C₃N₄. The reaction rate constant (k) of PCN (0.013 min^-1) was approximately twice that of bare g-C₃N₄ (0.007 min^-1). Furthermore, the effects of original pH and concentration of Cr(VI)-containing solution on removal efficiency of Cr(VI) were explored. A possible photocatalytic mechanism was proposed based on the experiments of radical scavengers and photoelectrochemical characterizations.

Key words: Porous carbon nitride, Nickel foam, Hydrogen, Cr(VI), Photocatalysis

Xueru Chen, Yin Zhang, Dashui Yuan, Wu Huang, Jing Ding, Hui Wan, Wei-Lin Dai, Guofeng Guan. One step method of structure engineering porous graphitic carbon nitride for efficient visible-light photocatalytic reduction of Cr(VI)[J]. J. Mater. Sci. Technol., 2021, 71: 211-220.

Figures/Tables 11

Scheme 1. Schematic illustration of the preparation process of PCN.

Fig. 1. XRD patterns (a) and the relative enlarged view of (002) peaks (b) of g-C3N4 and PCN; XRD patterns of Ni foam and Ni species at 500 ℃ and 550 ℃ (c); FT-IR spectra of g-C3N4 and PCN (d).

Table 1 Elemental analysis of g-C3N4 and PCN.

Sample	C (wt%)	N (wt%)	H (wt%)	C/N atomic ratio	C/H atomic ratio
g-C₃N₄	35.01	62.01	1.918	0.659	1.521
PCN	34.97	61.80	2.023	0.660	1.441

Table 2 Specific surface area, pore volume and pore size of g-C3N4 and PCN.

Sample	S_BET (m² g^-1)	Total pore volume (cm³ g^-1)	Average pore diameter (nm)
PCN	75	0.52	27
g-C₃N₄	12	0.10	33

Fig. 2. XPS spectra of g-C3N4 and PCN: high-resolution C 1s (a) and high-resolution N 1s (b).

Fig. 3. TEM images of g-C3N4(a) and PCN (b, c); Magnified picture acquired from the rectangular area labelled in b (d).

Fig. 4. UV-vis absorption spectra (a), Tauc plot for band gap determination (b) and photoluminescence spectra (c); Time-resolved fluorescence decay spectra monitored at 460 nm by time-correlated single-photon counting (d) of g-C3N4 and PCN.

Fig. 5. Electrochemical impedance spectra (a), transient photocurrent response (b), Mott-Schottky plot (c) and band structure alignment (d) of g-C3N4 and PCN.

Fig. 6. Cr(VI) photocatalytic reduction performance (a) and the corresponding ln(Ci0/Cit) versus time curves (b) over PCN.

Fig. 7. Effects of original pH (a) and initial concentration of Cr(VI)-containing solution (c) on the photocatalytic performance and corresponding ln(Ci0/Cit) versus time curves (b, d).

Scheme 2. The possible mechanism for photocatalytic reduction of Cr(Ⅵ) over PCN.

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