Towards highly-selective H2O2 photosynthesis: In-plane highly ordered carbon nitride nanorods with Ba atoms implantation

doi:10.1016/S1872-2067(24)60008-2

Abstract

Abstract:

Graphitic carbon nitride (g-C₃N₄) shows great potential in photocatalytic H₂O₂ production. However, challenges arise from its low in-plane crystallinity and selectivity in two-electron oxygen reduction reaction (2e^--ORR), greatly limiting its H₂O₂ photosynthesis efficiency. Herein, we develop an ingenious strategy to simultaneously increase the in-plane crystallinity and induce the highly-selective 2e^--ORR by rationally designing barium (Ba) atom-implanted in-plane highly ordered g-C₃N₄ nanorods. The approach involves controllable synthesis of in-plane high crystallinity g-C₃N₄ nanorods with Ba implantation (BI-CN) using a BaCl₂-mediated in-plane polymerization strategy. The unique Ba-N interaction induces the oriented polymerization of 3-s-triazine units to form well-arranged in-plane structures. Experimental and theoretical calculations clarify that the implanted Ba atoms function as positive charge centers, resulting in a Pauling-type O₂ adsorption configuration. This minimizes O-O bond breaking energy, thus suppressing the four-electron oxygen reduction reaction (4e^--ORR) and facilitating a highly-selective 2e^--ORR pathway for efficient photocatalytic H₂O₂ production. Consequently, the optimized BI-CN3 photocatalyst exhibits an outstanding H₂O₂ production rate of as high as 353 μmol L^-1 h^-1, surpassing the pristine g-C₃N₄ by 6.1 times. This study concurrently optimizes the in-plane crystallinity and O₂ adsorption sites of g-C₃N₄ photocatalysts for highly-selective H₂O₂ production, providing innovative insights for designing efficient photocatalysts with diverse applications.

Key words: Hydrogen peroxide photosynthesis, Carbon nitride, Ba implantation, Highly-selective 2e^?-ORR, In-plane crystallinity

Aiyun Meng, Xinyuan Ma, Da Wen, Wei Zhong, Shuang Zhou, Yaorong Su. Towards highly-selective H₂O₂ photosynthesis: In-plane highly ordered carbon nitride nanorods with Ba atoms implantation[J]. Chinese Journal of Catalysis, 2024, 60: 231-241.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(24)60008-2

https://www.cjcatal.com/EN/Y2024/V60/I5/231

Figures/Tables 7

Fig. 1. Graphical illustration about the conventional g-C3N4 with slow electron transfer and low-selectivity H2O2 photosynthesis (1), Ba implanted in-plane highly ordered g-C3N4 photocatalyst with simultaneously accelerating electron transfer and promoting H2O2 evolution selectivity (2).

Fig. 2. (a) The ordered growth mechanism of the BI-CN by BaCl2-mediated in-plane polymerization process. (b) The calculated adsorption energy of the melamine molecules on different BaCl2 crystal planes. (c) FTIR patterns of the BI-CN at different temperatures.

Fig. 3. SEM (a), TEM (b), high-resolution TEM (c) and TEM-EDS mapping images (d) of the typical BI-CN3 sample. XRD patterns (e), FT-IR patterns (f), Solid-state 13C NMR MAS spectra (g), high-resolution XPS curves (h), UV-vis DRS spectra (i) and Nitrogen adsorption-desorption isotherms (j) for the synthesized photocatalysts.

Fig. 4. (a) Photocatalytic H2O2-production rates for various samples. (b) Cycling H2O2-generation tests of BI-CN3 photocatalyst. (c) The photocatalytic H2O2-activities for bulk CN and BI-CN3 samples in 0.1 mol L?1 Na2SO4 solution. (d) H2O2 evolution activities of BI-CN3 samples under different conditions.

Fig. 5. High-resolution XPS spectra of N 2p (a) and Ba 3d (b). (c) The optimized structure models of conventional g-C3N4 (CN) and the Ba implanted in-plane highly ordered g-C3N4 (BI-CN). The calculated density of state (DOS) for bulk CN (d) and BI-CN (e). Bader charge analysis (f) and the electrostatic potential surface distribution for the optimized bulk CN (g) and BI-CN (h) models.

Fig. 6. (a) EPR spectra of DMPO?O2?. (b) Koutecky-Levich plots for CN and BI-CN. The calculated O2 adsorption models on CN (c) and BI-CN (d) structures and their corresponding local charge density differences. (e) Calculated free energy diagrams for 2e?-ORR (H2O2 production) and 4e?-ORR (H2O evolution).

Fig. 7. Mechanism of the highly-selective 2e- ORR process for efficient photocatalytic H2O2 production on the Ba implanted in-plane highly ordered g-C3N4 nanorods.

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Towards highly-selective H₂O₂ photosynthesis: In-plane highly ordered carbon nitride nanorods with Ba atoms implantation

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