Interfacial Ni-N bond in g-C3N4/CoNi2S4 for enhanced photocatalytic CO2 conversion

doi:10.1016/S1872-2067(25)64923-0

Abstract

Abstract:

Cocatalyst loading has been extensively adopted in photocatalysis for enhancing photocatalytic performance. However, the sluggish interfacial charge dynamics between cocatalyst and photocatalyst has restricted the wide applications of such a strategy. Herein, we introduce the Ni-N interfacial bonds between lamellar nitrogen-vacancy-rich g-C₃N₄/CoNi₂S₄ nanoparticles (CN-V_N/CoNi₂S₄) composite material to bridge the photogenerated charge carrier separation at their interface. Specifically, extended X-ray absorption fine structure analysis reveals that these Ni-N interfacial bonds are originated from the bonding of CoNi₂S₄ with the nitrogen atoms adjacent to the nitrogen vacancies (V_N) in g-C₃N₄. Experimental evidence and theoretical calculations reveal that Ni-N interfacial bonds cannot only cause an intimate contact interface between CN-V_N/CoNi₂S₄, but also modulate the charge distribution on the CN-V_N and CoNi₂S₄, further boosting the photogenerated charge carrier separation. More interestingly, this tailored interfacial microenvironment significantly reduces the energy barrier for key intermediates formation while modulates the rate-determining step from *COOH generation to CO desorption, enabling efficient and controllable CO production. This work establishes a methodological framework for engineering advanced photocatalysts, enabling high-efficiency conversion of solar energy into clean fuels.

Key words: Photocatalysis, Interfacial chemical bonds, In-situ growth, Nitrogen-vacancy, CO₂ conversion

Haonan Li, Wa Gao, Kangli Ma, Jian Lei, Olim Ruzimuradov, Akhtam Samiev, Ya Chen, Jingxiang Low, Yue Li. Interfacial Ni-N bond in g-C₃N₄/CoNi₂S₄ for enhanced photocatalytic CO₂ conversion[J]. Chinese Journal of Catalysis, 2026, 82: 266-277.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(25)64923-0

https://www.cjcatal.com/EN/Y2026/V82/I3/266

Figures/Tables 5

Fig. 1. (a) Schematic illustration of the preparation procedure of CN-VN/CoNi2S4. (b) TEM image of CN-VN. TEM (c), HRTEM (d), and elemental mappings images for C, N, Co, Ni and S (e) of CN-VN/CoNi2S4-3. (f) XRD patterns of CoNi2S4, g-C3N4, CN-VN and CN-VN/CoNi2S4 with different CoNi2S4 contents. (g) ESR spectra of CN-VN and CN-VN/CoNi2S4-3. (h) FTIR of CoNi2S4, g-C3N4, CN-VN and CN-VN/CoNi2S4-3.

Fig. 2. High-resolution XPS spectra of N 1s (a), Co 2p (b), and Ni 2p (c) for CN-VN, CoNi2S4 and CN-VN/CoNi2S4. Ni K-edge XANES (d) and Co K-edge XANES (e) profiles of different samples. Ni K-edge k3-weighted FT-EXAFS (f) and Co K-edge k3-weighted FT-EXAFS (g) spectra of different samples. WT-EXAFS contour plot of Ni k3-weighted (h) and Co k3-weighted (i) for CoNi2S4 and CN-VN/CoNi2S4.

Fig. 3. (a) CO2 TPD profiles of g-C3N4, CN-VN and CN-VN/CoNi2S4-3. (b) UV-vis-NIR DRS of g-C3N4, CN-VN, CoNi2S4 and CN-VN/CoNi2S4-3. (c) EIS Nyquist plots of CN-VN and CN-VN/CoNi2S4-3. Transient photocurrent density (d) and TR-PL spectra (e) of CN-VN and CN-VN/CoNi2S4-3. (f) EPR spectra for CN-VN, CoNi2S4, and CN-VN/CoNi2S4-3 catalysts of DMPO-?O2? adducts under light illumination.

Fig. 4. Comparison of the CO production after 5 h of photocatalytic CO2 conversion reaction (a) and corresponding average productivity (b) of CN-VN, CoNi2S4 and CN-VN/CoNi2S4. (c) CO production from photocatalytic CO2 reduction over CN-VN based photocatalysts. (d) Photocatalytic stability test of the CN-VN/CoNi2S4-3 for CO production. (e) CO productivity of the CN-VN/CoNi2S4-3 under different reaction conditions. (f) Mass spectrometry analysis of the photocatalytic CO2 conversion products over CN-VN/CoNi2S4-3 using 13CO2 as reactant.

Fig. 5. In-situ DRIFTS spectra for photocatalytic CO2 conversion over g-C3N4 (a), CN-VN (b), and CN-VN/CoNi2S4-3 (c). (d) Gibbs free energy diagram of CoNi2S4, CN-VN and CN-VN/CoNi2S4 at different catalytic sites. (e) Schematic diagram of proposed mechanism for photocatalytic reaction over CN-VN/CoNi2S4.

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Interfacial Ni-N bond in g-C₃N₄/CoNi₂S₄ for enhanced photocatalytic CO₂ conversion

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