Ni-N bonds boost S-scheme charge transfer in NiSe/Cv-C3N5 for efficient water splitting

doi:10.1016/S1872-2067(25)64832-7

Abstract

Abstract:

Constructing heterojunction photocatalysts is a highly effective strategy for achieving overall water splitting, particularly by overcoming the challenge of sluggish electron-hole transport. This study employed a defect-induced in situ growth approach to anchor NiSe onto carbon-vacancy-rich C₃N₅ (C_v-C₃N₅), forming interfacial Ni-N bonds. The resulting NiSe/C_v-C₃N₅ heterojunction exhibited stoichiometric H₂ and O₂ evolution rates of 1956.1 and 989.1 μmol g^-1 h^-1, respectively, 8.4 times higher than a counterpart lacking interfacial bonding. Both theoretical calculations and experimental data confirmed that the Ni-N bonds were instrumental in enhancing photocatalytic performance by inducing and reinforcing S-scheme charge transfer. Illumination X-ray photoelectron spectroscopy analysis revealed that a synergistic charge transfer pathway: photoexcited electrons from the NiSe conduction band migrated sequentially to Ni atoms, then to N atoms, and ultimately recombined with holes in the C_v-C₃N₅ valence band. Moreover, these interfacial bonds significantly lowered the energy barrier and shortened the transport distance for electron transfer, amplifying the built-in interfacial electric field and accelerating charge dynamics. This study provides critical insights into the rational design of heterojunction photocatalysts for efficient water splitting.

Key words: Photocatalysis, NiSe/C_v-C₃N₅, Overall water splitting, Strong interfacial chemical bonds, Built-in electric field

Yan Cao, Lin Ye, Yangchen Yuan, Ruitao Yang, Hui Hong, Jingwen Chen, Jinyi Lu, Entian Cui, Jizhou Jiang. Ni-N bonds boost S-scheme charge transfer in NiSe/C_v-C₃N₅ for efficient water splitting[J]. Chinese Journal of Catalysis, 2025, 78: 229-241.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(25)64832-7

https://www.cjcatal.com/EN/Y2025/V78/I11/229

Figures/Tables 6

Fig. 1. (a) The synthetic procedure of NiSe/Cv-C3N5. XRD patterns (b), TEM (c), and HRTEM (d) images of NiSe/Cv-C3N5. (e) Raman spectra of NiSe, Cv-C3N5, and NiSe/Cv-C3N5. (f) Fourier-transformed EXAFS spectra in R-space for NiSe/Cv-C3N5. (g) Elemental mapping images of NiSe/Cv-C3N5.

Fig. 2. Survey spectra (a), C 1s (b), and N1s (c) XPS spectra of C3N5, Cv-C3N5, and NiSe/Cv-C3N5. Ni 2p (d) and Se 3d (e) XPS spectra of NiSe and NiSe/Cv-C3N5. (f) UV-vis DRS spectra of NiSe, Cv-C3N5, and NiSe/Cv-C3N5. SI-VB XPS (g) and SI-UPS (h) spectra of NiSe and Cv-C3N5. (i) Band structure alignments of NiSe/Cv-C3N5.

Fig. 3. (a) Photocatalytic overall water splitting performance of NiSe/Cv-C3N5. (b) Comparison of photocatalytic performance in overall water splitting. (c) 18O isotope-labelled water experiment results of NiSe/Cv-C3N5. (d) The photostability of NiSe/Cv-C3N5. (e) I-t curve of NiSe/Cv-C3N5. PL (f) and Time-resolved PL (g) spectra of NiSe/Cv-C3N5. (h) EIS plot of NiSe/Cv-C3N5.

Fig. 4. 2D pseudo-color maps of fs-TA spectra (a,d,g), transient fs-TA spectra (b,e,h), kinetic time profiles (c,f,i) of normalized transient absorption. (j) The decay pathways of electron transport in NiSe, Cv-C3N5, and NiSe/Cv-C3N5.

Fig. 5. Ni 2p (a), N 1s (c), C 1s (e), and Se 3d (f) SI-XPS spectra of NiSe/Cv-C3N5. Ni 2p (b), N 1s (d), C 1s (f), and Se 3d (h) SI-XPS spectra of NiSe/Cv-C3N5-MIX. (i) The photoinduced electron transport scheme in NiSe/Cv-C3N5.

Fig. 6. (a) Charge density distributions in NiSe/Cv-C3N5. (b) Energy barrier and transfer distance of interfacial charge transport in NiSe/Cv-C3N5. (c) Charge density difference distribution (unit in e/Bohr) of NiSe/Cv-C3N5. (d) 2D mapping of electronic location function of NiSe/Cv-C3N5. (e,f) DMPO-·O2- and DMPO-·OH spectra of NiSe/Cv-C3N5 in methanol obtained under different illumination times. (g) Gibbs free energy of water reduction on NiSe/Cv-C3N5. (h) Gibbs free energy of water oxidation on NiSe/Cv-C3N5. (i) Schematic illustration of the S-scheme charge-transfer process in NiSe/Cv-C3N5.

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Ni-N bonds boost S-scheme charge transfer in NiSe/C_v-C₃N₅ for efficient water splitting

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