Chinese Journal of Catalysis ›› 2025, Vol. 69: 219-229.DOI: 10.1016/S1872-2067(24)60195-6
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Jian-Zhou Xiao, Zhi-Hao Zhao, Nan-Nan Zhang, Hong-Tu Che, Xiu Qiao, Guang-Ying Zhang, Xiaoyu Chu, Ya Wang, Hong Dong*(), Feng-Ming Zhang*(
)
Received:
2024-09-18
Accepted:
2024-11-05
Online:
2025-02-18
Published:
2025-02-10
Contact:
E-mail: About author:
First author contact:1 Contributed equally to this work.
Supported by:
Jian-Zhou Xiao, Zhi-Hao Zhao, Nan-Nan Zhang, Hong-Tu Che, Xiu Qiao, Guang-Ying Zhang, Xiaoyu Chu, Ya Wang, Hong Dong, Feng-Ming Zhang. Linkage engineering in covalent organic frameworks for overall photocatalytic H2O2 synthesis from water and air[J]. Chinese Journal of Catalysis, 2025, 69: 219-229.
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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(24)60195-6
Fig. 1. (a) The structure diagram of TTA-Azo-COF, TTA-COF and TTA-COF-AR. PXRD patterns and refined profiles of TTA-Azo-COF (b), TTA-COF (c) and TTA-COF-AR (d). N2 adsorption-desorption isotherms and pore size distribution pro?les (insert) for TTA-Azo-COF (e), TTA-COF (f) and TTA-COF-AR (g).
Fig. 2. FT-IR (a), Raman (b) and 13C CP/MAS ssNMR (c) spectra of TTA-COF, TTA-COF-AR and TTA-Azo-COF. The HR-XPS N 1s spectra of TTA-COF (d), TTA-COF-AR (e) and TTA-Azo-COF (f). TEM, HR-TEM images and lattice fringes of TTA-COF (g), TTA-COF-AR (h) and TTA-Azo-COF (i).
Fig. 3. UV-vis DRS spectra (a), optical bandgap (b) and energy band structures (c) for TTA-COF, TTA-COF-AR and TTA-Azo-COF. (d) The photocatalytic performance of H2O2 production using visible light for TTA-COF, TTA-COF-AR and TTA-Azo-COF. (e) The photocatalytic performance of H2O2 production under different atmosphere conditions. (f) The comparison of H2O2 photosynthesis rate by TTA-Azo-COF with other reported photocatalysts under similar reaction conditions. (g) Comparison of H2O2 production rates by TTA-COF, TTA-COF-AR and TTA-Azo-COF under different conditions. (h) Photocatalytic H2O2 synthesis cycles stability of TTA-COF, TTA-COF-AR and TTA-Azo-COF. (i) The dependence of AQY on incident light wavelength.
Fig. 4. (a) The RRDE measurement of TTA-COF, TTA-COF-AR and TTA-Azo-COF at 1600 r min?1 in O2-saturated 0.1 mol L?1 KOH. (b) The Koutecky-Levich plots obtained by RDE measurements. The transient photocurrent response density (c), EIS Nyquist plots (d), PL spectra (e) and TRPL decay spectra (f) of TTA-COF, TTA-COF-AR and TTA-Azo-COF. (g) EPR spectra of TTA-COF, TTA-COF-AR and TTA-Azo-COF under visible-light irradiation (λ > 420 nm) conditions. (h,i) EPR spectra of DMPO-·O2? of TTA-COF, TTA-COF-AR and TTA-Azo-COF under visible-light irradiation (λ > 420 nm) and dark conditions.
Fig. 5. Time-dependence in-situ DRIFTS spectra of TTA-COF (a), TTA-COF-AR (b) and TTA-Azo-COF (c) under visible-light irradiation with water vapor and O2 atmosphere. (d) Possible reaction sites for ORR in TTA-Azo-COF. (e,f) Adsorption configuration of *OO and *OOH key intermediates on TTA-Azo-COF. (g) Free energy diagrams of TTA-Azo-COF for the photosynthesis of H2O2 by ORR pathway in different reaction sites. (h,i) Calculated energy profile for reduction of oxygen into H2O2 and oxidation of water into H2O2 or O2 on TTA-COF, TTA-COF-AR and TTA-Azo-COF.
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