Enhanced photocatalytic H2O2 production over Pt(II) deposited boron containing metal-organic framework via suppressing the simultaneous decomposition

doi:10.1016/S1872-2067(22)64163-9

Abstract

Abstract:

Photocatalytic H₂O₂ evolution has received extensive attention as an environmentally friendly method, which is a dynamic process of formation and decomposition. At present, researches mainly focus on the H₂O₂ formation, while the decomposition of H₂O₂ is rarely studied. In addition, platinum as a cocatalyst plays an important role in enhancing the photocatalytic activity, but the effects of platinum valence state on the activity, especially towards H₂O₂ formation and decomposition, has not been studied in detail to the best of our knowledge. In this work, platinum with different valence state were deposited onto boron containing metal organic frameworks (UiO-67-B), and the roles of Pt(0), Pt(II) and Pt(IV) in the photocatalytic H₂O₂ process were explored in detail. Both the experimental results and theoretical calculations indicate that the presence of Pt(II) plays an important role not only in promoting the H₂O₂ formation but also in inhibiting the H₂O₂ decomposition.

Key words: Boron doping, H₂O₂ decomposition, H₂O₂ production, Metal-organic frameworks, Platinum valence state, Photocatalysis

Yujie Li, Yuanyuan Liu, Zeyan Wang, Peng Wang, Zhaoke Zheng, Hefeng Cheng, Ying Dai, Baibiao Huang. Enhanced photocatalytic H2O2 production over Pt(II) deposited boron containing metal-organic framework via suppressing the simultaneous decomposition[J]. Chinese Journal of Catalysis, 2023, 45: 132-140.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(22)64163-9

https://www.cjcatal.com/EN/Y2023/V45/I2/132

Figures/Tables 6

Fig. 1. (a) XRD patterns of UiO-67-B, UiO-67-B/Pt(0), UiO-67-B/Pt(II) and UiO-67-B/Pt(IV). High-resolution XPS spectra of Pt 4f (b) and Cl 2p (c) for UiO-67-B/Pt(0), UiO-67-B/Pt(II) and UiO-67-B/Pt(IV). (d) The optimized structure model for UiO-67-B/Pt(II). (e) FTIR spectra for UiO-67-B and UiO-67-B/Pt(II).

Fig. 2. (a) Time course of H2O2 production over UiO-67-B, UiO-67-B/Pt(0), UiO-67-B/Pt(II) and UiO-67-B/Pt(IV). (b) Comparison of H2O2 production over UiO-67-B/Pt(II) and other photocatalysts reported in recent studies. (c) Time course of H2O2 production over UiO-67-B/Pt(II) with different platinum contents (x% is the mass ratio of platinum to UiO-67-B). Reaction conditions for H2O2 production: 0.3 g L-1 catalyst, 90 mL water + 10 mL isopropanol, simulated sunlight.

Fig. 3. N2 adsorption-desorption isotherms (a) and TPD curves (b) of O2 for UiO-67-B, UiO-67-B/Pt(0), UiO-67-B/Pt(II) and UiO-67-B/Pt(IV). HAADF-STEM images of UiO-67-B/Pt(II) (c) and UiO-67-B/Pt(0) (d). (e) The formation (Kf, blue histogram) and decomposition rate constant (Kd, cyan histogram) for H2O2 over UiO-67-B, UiO-67-B/Pt(0), UiO-67-B/Pt(II) and UiO-67-B/Pt(IV). (f) The photocatalytic decomposition of H2O2 (C0 = 1 mmol L-1) over UiO-67-B, UiO-67-B/Pt(0), UiO-67-B/Pt(II) and UiO-67-B/Pt(IV).

Fig. 4. (a) Time-resolved PL decay spectra for UiO-67-B, UiO-67-B/Pt(0), UiO-67-B/Pt(II) and UiO-67-B/Pt(IV). (b) ESR signals of DMPO-?O2- over UiO-67-B, UiO-67-B/Pt(0), UiO-67-B/Pt(II) and UiO-67-B/Pt(IV) under simulated sunlight irradiation. Transient photocurrent response (c) and EIS plots (d) for UiO-67-B, UiO-67-B/Pt(0), UiO-67-B/Pt(II) and UiO-67-B/Pt(IV).

Fig. 5. (a) Electronic spatial distribution of UiO-67-B/Pt(II) at CBM and VBM. (b) The optimized models and adsorption energy of O2 molecules over UiO-67-B and UiO-67-B/Pt(II). (c) Free energy diagrams for H2O2 generation on UiO-67-B and UiO-67-B/Pt(II).

Fig. 6. Plausible mechanism of H2O2 formation and decomposition over UiO-67-B (a) and UiO-67-B/Pt(II) (b).

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