Sulfur-mediated photodeposition synthesis of NiS cocatalyst for boosting H2-evolution performance of g-C3N4 photocatalyst

doi:10.1016/S1872-2067(20)63633-6

Abstract

Abstract:

Modification of nickel sulfide cocatalysts is considered to be a promising approach for efficient enhancement of the photocatalytic hydrogen production performance of g-C₃N₄. Providing more NiS cocatalyst to function as active sites of g-C₃N₄ is still highly desirable. To realize this goal, in this work, a facile sulfur-mediated photodeposition approach was developed. Specifically, photogenerated electrons excited by visible light reduce the S molecules absorbed on g-C₃N₄ surface to S^2-, and subsequently NiS cocatalyst is formed in situ on the g-C₃N₄ surface by a combination of Ni²⁺ and S^2- due to their small solubility product constant (K_sp = 3.2 × 10^-19). This approach has several advantages. The NiS cocatalyst is clearly in situ deposited on the photogenerated electron transfer sites of g-C₃N₄, and thus provides more active sites for H₂ production. In addition, this method utilizes solar energy with mild reaction conditions at room temperature. Consequently, the synthesized NiS/g-C₃N₄ photocatalyst achieves excellent hydrogen generation performance with the performance of the optimal sample (244 μmol h^-1 g^-1) close to that of 1 wt% Pt/g-C₃N₄ (316 μmol h^-1 g^-1, a well-known excellent photocatalyst). More importantly, the present sulfur-mediated photodeposition route is versatile and facile and can be used to deposit various metal sulfides such as CoS_x, CuS_x and AgS_x on the g-C₃N₄ surface, and all the resulting metal sulfide-modified g-C₃N₄ photocatalysts exhibit improved H₂-production performance. Our study offers a novel insight for the synthesis of high-efficiency photocatalysts.

Key words: g-C3N4, NiS, Co-catalyst, Sulfur-mediated photodeposition, H2, Photocatalysis

Min Wang, Jingjing Cheng, Xuefei Wang, Xuekun Hong, Jiajie Fan, Huogen Yu. Sulfur-mediated photodeposition synthesis of NiS cocatalyst for boosting H₂-evolution performance of g-C₃N₄ photocatalyst[J]. Chinese Journal of Catalysis, 2021, 42(1): 37-45.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(20)63633-6

https://www.cjcatal.com/EN/Y2021/V42/I1/37

Figures/Tables 9

Fig. 1. (A) Schematic illustration of the synthesis of NiS/g-C3N4 in an ethanol system; (B) Schematics of g-C3N4 suspension (a), S2-/g-C3N4 suspension (b), Ni/g-C3N4 suspension (c), and NiS/g-C3N4 suspension (d) and corresponding redox potentials; (C) Schematic illustration of the formation of the NiS/g-C3N4 sample and the proposed photocatalytic hydrogen-generation mechanism of NiS/g-C3N4.

Fig. 2. FESEM/EDS images of various samples. (A) g-C3N4; (B) NiS/g-C3N4(1 wt%); (C) NiS/g-C3N4(3 wt%); (D) NiS/g-C3N4(5 wt%). TEM (E) and HRTEM (F) images of NiS/g-C3N4(1 wt%).

Fig. 3. XRD patterns of various samples. (a) g-C3N4; (b) NiS/g-C3N4(0.1 wt%); (c) NiS/g-C3N4(0.3 wt%); (d) NiS/g-C3N4(1 wt%); (e) NiS/g- C3N4(3 wt%).

Fig. 4. (A) Full-range XPS spectra and the high-resolution XPS spectra of C 1s (B), N 1s (C), O 1s (D), Ni 2p (E) and S 2p (F) for various samples. (a) g-C3N4; (b) NiS/g-C3N4(0.3 wt%); (c) NiS/g-C3N4(1 wt%); (d) NiS/g-C3N4(3 wt%).

Table 1 Elemental content (at%) of the various samples based on the XPS results.

Sample	C	N	O	Ni	S
g-C₃N₄	43.95	53.06	2.99	0	0
NiS/g-C₃N₄(0.3 wt%)	44.78	49.77	4.07	0.65	0.73
NiS/g-C₃N₄(1 wt%)	44.33	45	7.30	1.7	1.67
NiS/g-C₃N₄(3 wt%)	42.62	43.96	8.46	2.18	2.78

Fig. 5. (A) FTIR spectra, and (B) UV-vis absorption spectra and photographs (inset) of various samples: (a) g-C3N4, (b) NiS/g-C3N4(0.05 wt%), (c) NiS/g-C3N4(0.1 wt%), (d) NiS/g-C3N4(0.3 wt%), (e) NiS/g-C3N4(1 wt%) and (f) NiS/g-C3N4(3 wt%).

Fig. 6. (A) Photocatalytic H2-evolution rate of various samples. (B) Recycling test of NiS/g-C3N4(0.3 wt%) sample; (C) Transient photocurrent responses; (D) Electrochemical impedance spectra curves. (a) g-C3N4; (b) NiS/g-C3N4(0.05 wt%); (c) NiS/g-C3N4(0.1 wt%); (d) NiS/g-C3N4(0.3 wt%); (e) NiS/g-C3N4(1 wt%); (f) NiS/g-C3N4(3 wt%); (g) NiS/g-C3N4(0.3 wt%, wet-chemistry method); (h) Pt/g-C3N4(1 wt%).

Fig. 7. FESEM/EDS results for various samples. (A) CoSx/g-C3N4; (B) CuSx/g-C3N4; (C) AgSx/g-C3N4.

Fig. 8. (A) UV-vis absorption spectra and photographs (inset) and (B) Photocatalytic H2 evolution rate for various samples. (a) g-C3N4; (b) CoSx/g-C3N4; (c) CuSx/g-C3N4; (d) AgSx/g-C3N4.

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Sulfur-mediated photodeposition synthesis of NiS cocatalyst for boosting H₂-evolution performance of g-C₃N₄ photocatalyst

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