Infiltration of C-ring into crystalline carbon nitride S-scheme homojunction for photocatalytic hydrogen evolution

doi:10.1016/S1872-2067(23)64448-1

Abstract

Abstract:

Enhancing the carrier separation in graphitized carbon nitride (g-C₃N₄) is advantageous for improving its photocatalytic activity. Herein, we propose a feasible method for preparing CN-C by thermal polymerization to gradually infiltrate carbon rings (C-rings) into the surface of crystalline carbon nitride (CN), enabling photogenerated electrons to be transferred rapidly between the CN inner layers and the CN/C outer layer. Successful penetration and distribution of carbon rings into carbon nitride were confirmed by secondary ion mass spectroscopy using ratio analysis of C and N elements at various depths of the prepared photocatalyst. Theoretical calculations indicated that CN and CN/C in the molecule generated different Fermi levels to form an S-scheme homojunction, establishing appropriate built-in electric fields and thus enabling interlayer charge migration. Moreover, the overlap of the conjugate plane of C-rings with carbon nitride led to the formation of photogenerated in-plane charge transfer tunnels. The two-electron transfer tunnels greatly improved the dissociation efficiency of photogenerated electrons. The prepared sample loaded with 3 wt% Pt as a co-catalyst for hydrogen production under visible light irradiation, and the prepared optimal sample CN-C showed a maximum quantum efficiency of 15.56% for photocatalytic H₂ evolution at 385 nm. This research introduces a new idea for constructing a directional transfer path for charge carriers in-plane and intralayer.

Key words: Carbon ring, S-scheme, Interlayer charge transfer, Homojunction, Photocatalytic hydrogen evolution reaction

Zhihan Yu, Chen Guan, Xiaoyang Yue, Quanjun Xiang. Infiltration of C-ring into crystalline carbon nitride S-scheme homojunction for photocatalytic hydrogen evolution[J]. Chinese Journal of Catalysis, 2023, 50: 361-371.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(23)64448-1

https://www.cjcatal.com/EN/Y2023/V50/I7/361

Figures/Tables 7

Fig. 1. (a) Schematic illustration of the CN-C synthesis process. TEM images of PCN (b) and CN-C (c). HRTEM images (d,e) and elemental distribution mapping (f,g) of CN-C (the inset shows the corresponding TEM image).

Fig. 2. (a) XRD patterns of PHI, CN-C, and PTI samples. Raman (b), FT-IR (c), and C 1s XPS (d) spectra of PCN and CN-C.

Fig. 3. (a) The atomic percentages of elements C and N in CN-C with increasing depth, obtained after multiple ion etching. The secondary y-axis (right) exhibits the atomic ratio of C to N. (b) Corresponding atomic percentages of element C in C-ring and g-C3N4. The right axis exhibits the atomic ratio of C-t-tri and N. The electrostatic potentials of CN/C (c) and CN (d). Φ indicates the work function in eV. (e) The stepwise mechanism for photocatalytic hydrogen evolution on S-scheme homojunction of CN-C.

Fig. 4. (a) UV-Vis absorption spectra of PCN and CN-C and the inset showing the Tauc plots. (b) The Mott-Schottky plots. The inset shows the electronic band structures of PCN and CN-C. (c) DOS for CN and CN/C. (d) Top view of the charge density difference of the CN/C. (The purple wireframe marks the C-rings, isovalue = 0.02 a.u.)

Fig. 5. Fs-TA absorption spectra of CN-C at different probe delay times (a) and the corresponding three-disparate image (b). CN-C kinetic decays at 535 (c), 575 (d), and 581 nm (e). (f) Time-resolved photoluminescence spectra of PCN and CN-C. (g) Schematic diagram of CN-C interlayer in photocatalytic process and in-plane two-channel electron transfer.

Table 1 Ft-TA analysis of CN-C (Exc at 400 nm, 1 mW).

λ_ex/nm	λ_probe/nm	τ₁/ps	A₁/%	τ₂/ps	A₂/%
	535	4.4	41	609.5	52
400	575	4.7	36	1015.3	51
	581	6.8	48	1615.3	56

Fig. 6. (a,b) Photocatalytic HER rate of CN, PCN, CN/C, and other CN-C-x samples with 3 wt% of Pt as the co-catalyst and 10 vol% TEOA aqueous solution as the sacrificial reagent after visible light irradiation for 1 h. (c) Photocatalytic stability of CN-C under light irradiation. (d) Wavelength-dependent AQE of CN-C with 3 wt% of Pt as the co-catalyst and 10 vol% TEOA aqueous solution as the sacrificial reagent after 1 h irradiation under an LED light source with different wavelengths.

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