Oxygen vacancies mediated ultrathin Bi4O5Br2 nanosheets for efficient piezocatalytic peroxide hydrogen generation in pure water

doi:10.1016/S1872-2067(23)64591-7

Abstract

Abstract:

The industrial anthraquinone method for H₂O₂ production has the serious flaws, such as high pollution and energy consumption. Piezocatalytic H₂O₂ evolution has been proven as a promising strategy, but its progress is hindered by unsatisfied energy conversion efficiency. Hence, we report the efficient piezocatalytic H₂O₂ generation in pure water over oxygen vacancies mediated ultrathin Bi₄O₅Br₂ nanosheets (~5 nm). Oxygen vacancies and thin nanostructure not only enhance the piezoelectric properties of Bi₄O₅Br₂, but also advance the separation and transfer of piezoinduced charges. Moreover, density functional theory (DFT) calculations also prove that the introduction of oxygen vacancies enhances the O₂ adsorption and activation ability with largely decreased Gibbs free energy of the reaction pathway. Profiting from these advantages, ultrathin Bi₄O₅Br₂ nanosheets optimized by oxygen vacancies exhibit a prominent H₂O₂ evolution rate of 620 µmol g^-1 h^-1 in pure water and 2700 µmol g^-1 h^-1 in sacrificial system, dominated by a two-step single electron reaction, which exceeds most of reported piezocatalysts. This work demonstrates that oxygen vacancies and ultrathin structure can synergistically enhance the piezocatalytic performance, which presents perspectives into exploring the strategies of defects and nanostructure fabrication for promoting piezocatalytic activity.

Key words: Bi₄O₅Br₂, Oxygen vacancies, Ultrathin nanosheets, Piezocatalysis, H₂O₂ generation

Hao Cai, Fang Chen, Cheng Hu, Weiyi Ge, Tong Li, Xiaolei Zhang, Hongwei Huang. Oxygen vacancies mediated ultrathin Bi₄O₅Br₂ nanosheets for efficient piezocatalytic peroxide hydrogen generation in pure water[J]. Chinese Journal of Catalysis, 2024, 57: 123-132.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(23)64591-7

https://www.cjcatal.com/EN/Y2024/V57/I2/123

Figures/Tables 6

Fig. 1. SEM (a) and HRTEM (d) images of BOB-OV2. AFM images of BOB (b,e) and BOB-OV2 (c,f). (g-j) EDX images of BOB-OV2.

Fig. 2. (a) XRD patterns of as-prepared samples. XPS spectra of BOB and BOB-OV2: survey spectra (b), O 1s (c), Bi 4f (d), Br 3d (e). (f) EPR spectra of BOB and BOB-OV2.

Fig. 3. (a,b) H2O2 yield of as-prepared samples. (c) H2O2 yield under different conditions over BOB-OV2. (d) H2O2 yield with different capture agents over BOB-OV2. (e) H2O2 yield at different atmosphere over BOB-OV2. (f) H2O2 yield with different ultrasonication powers. (g) Cycling experiments for piezocatalytic H2O2 formation over BOB-OV2. (h) Piezocatalytic H2O2 production performance comparison over different piezocatalysts [16,34????????-43].

Fig. 4. DRS spectra (a), the corresponding Tauc plots (b) and the Mott-Schottky plots (c) of the BOB and BOB-OV2. The butterfly amplitude-voltage loops of BOB (d) and BOB-OV2 (g). The phase angle loops of BOB (e) and BOB-OV2 (h). Piezoelectric potential distribution of BOB (f) and BOB-OV2 (i) under same force by COMSOL finite element simulation.

Fig. 5. RRDE curves (a) and the corresponding electron transfer numbers curves (b) of BOB-OV2. (c) EPR spectra of superoxide free radical intensity over BOB and BOB-OV2. KPFM images of BOB (d) and BOB-OV2 (e), the corresponding surface electric potential of BOB (g) and BOB-OV2 (h). Piezoelectric current response (f) and EIS Nyquist plots (i) of BOB and BOB-OV2.

Fig. 6. Charge difference and associated electron transfer of O2 adsorbed on BOB (a) and BOB-OV2 (b). (c) The Planar-averaged electron density difference of O2 adsorbed on BOB and BOB-OV2. The models of O2 adsorbed on BOB (d) and BOB-OV2 (e), and the corresponding bond length and Bader charge after the adsorption of oxygen (f). (g) Diagrams of the H2O2 production reaction path of Gibbs free energy on BOB and BOB-OV2 surfaces. (h) The histogram of oxygen adsorption energy of BOB and BOB-OV2.

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Oxygen vacancies mediated ultrathin Bi₄O₅Br₂ nanosheets for efficient piezocatalytic peroxide hydrogen generation in pure water

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