Synergetic piezo-photocatalysis of g-C3N4/PCN-224 core-shell heterojunctions for ultrahigh H2O2 generation

doi:10.1016/S1872-2067(23)64629-7

Abstract

Abstract:

Hydrogen peroxide (H₂O₂) is a high-value-added chemical for multitudinous industrial applications. Being compared with traditional anthraquinone processes, it is an eco-friendly and promising strategy to accomplish catalytic reduction of molecular oxygen for H₂O₂ production with the aid of mechanical and solar energy. It was the first attempt to combine a porphyrin-based metal-organic framework (PCN-224) and piezoelectric semiconductor (g-C₃N₄) to fabricate heterostructures (abbreviated as CP-x) with core-shell structure for piezo-photocatalytic H₂O₂ production. The introduction of PCN-224 not only widened light absorption range and accelerated electron transfer, but also facilitated the hydrogenation and generation of OOH^*, which was more prone to direct two-electron O₂ reduction. Furthermore, benefitting from the synergism of the piezo-photocatalysis, an exceptional piezo-photocatalytic H₂O₂ evolution rate of 5.97 mmol g^-1 h^-1 with solar-to-chemical conversion (SCC) efficiency of 0.14% was achieved by the optimum CP-5 heterojunction. This achievement significantly surpassed the previously reported g-C₃N₄-based and MOF-based materials. The use of rainwater as proton sources also allowed an impressive H₂O₂ generation rate (2.78 mmol g^-1 h^-1), thereby this outcome was of great significance to the rainwater utilization. This work contributed an in-depth understanding of piezo-photocatalytic O₂ reduction and provided an alternative way for the development of porphyrinic MOFs heterojunctions for synthesis of H₂O₂.

Key words: Porphyrin MOF, g-C₃N₄, H₂O₂, Piezo-photocatalysis, Mechanism

Linghui Meng, Chen Zhao, Hongyu Chu, Yu-Hang Li, Huifen Fu, Peng Wang, Chong-Chen Wang, Hongwei Huang. Synergetic piezo-photocatalysis of g-C₃N₄/PCN-224 core-shell heterojunctions for ultrahigh H₂O₂ generation[J]. Chinese Journal of Catalysis, 2024, 59: 346-359.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(23)64629-7

https://www.cjcatal.com/EN/Y2024/V59/I4/346

Figures/Tables 6

Fig. 1. Synthesis and structure characterization of g-C3N4, PCN-224, and CP-5. (a) representation of the basic synthetic scheme of CP-x catalysts; HRTEM images of g-C3N4 (b), PCN-224 (c) and CP-5 (d); (e,f) PXRD patterns and FTIR spectra of pristine g-C3N4, PCN-224 and CP-x; (g) N 1s high-resolution XPS spectra of g-C3N4, PCN-224 and CP-5; (h) UV-vis DRS spectra of g-C3N4, PCN-224 and CP-x materials.

Fig. 2. (a) Performance of H2O2 production by g-C3N4, PCN-224 and CP-5 under different conditions. (b) Reusability of CP-5 for the piezo-photocatalytic production of H2O2. (c) XPS of the CP-5 before and after ten cycles of catalytic experiment. (d-f) Piezo-photocatalytic production of H2O2 over CP-5 with different frequency, powers and initial pH values. (g) A comparison of H2O2 catalytic generation performances between CP-5 and other g-C3N4-based photocatalysts or piezo-photocatalysts in recent 6 years (Table S4). (h) An attempt to catalytically prepare H2O2 over the CP-5 by natural rainwater as a proton source. (i) Diameters of inhibition zones of CP-5. (j) E. coli deactivation by the different volumes of resulting H2O2 solution. Conditions: catalyst = 0.7g L-1, pH = 5.6, ultrasound frequency = 40 kHz, ultrasound power = 480 W.

Fig. 3. (a) Trapping experiments of radical scavengers for piezo-photocatalytic H2O2 generation by CP-5 heterojunction. (b) Trapping experiments of p-BQ for piezo-photocatalytic H2O2 generation by g-C3N4, PCN-224 and CP-5 heterojunction. (c) Quantitative analysis of ·O2- radicals generated in g-C3N4 and CP-5 piezo-photocatalytic system via NBT probe test. ESR spectra of ·O2- (d) and ·OOH (e) during the photoreaction by g-C3N4, PCN-224 and CP-5. (f) Koutecky-Levich plots of the ORR data measured by RDE analysis for g-C3N4 and CP-5. Conditions: catalyst = 0.7 g L-1, NBT = 50 μmol L-1, initial pH = 5.6.

Fig. 4. (a) PL (λexcitation = 350 nm, room temperature) spectra of g-C3N4 and CP-x. EIS (b) and LSV (c) spectra of g-C3N4, PCN-224 and CP-x. (d) TRPL spectra of g-C3N4, PCN-224 and CP-5. (e) Displacement-voltage curve of CP-5. (f) Phase curve of CP-5. KPFM potential images of CP-5 in the dark (g) and under light illumination (h). (i) The corresponding surface potential of CP-5 measured under different conditions.

Fig. 5. (a) The charge difference density between g-C3N4 and PCN-224 (the yellow represents the electron accumulation area, and the light blue represents the electron dissipation area). Work functions of g-C3N4 (b) and PCN-224 (c). (d) Free energy profiles for piezo-photocatalytic H2O2 evolution reactions over g-C3N4, PCN-224 and CP-5 heterojunction. H+ (e) and O2 (f) adsorption energies on g-C3N4, PCN-224 and CP-5.

Fig. 6. Schematic diagram of the piezocatalytic (a), photocatalytic (b), and piezo-photocatalytic synergistically promoting (c) the H2O2 production.

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Synergetic piezo-photocatalysis of g-C₃N₄/PCN-224 core-shell heterojunctions for ultrahigh H₂O₂ generation

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