Anchoring single Co sites on bipyridine-based covalent triazine framework for efficient photocatalytic oxygen evolution

doi:10.1016/S1872-2067(23)64552-8

Abstract

Abstract:

The photocatalytic oxygen evolution reaction (OER) is a half-reaction of water splitting for oxygen evolution, faces the drawback of sluggish kinetics. Developing highly efficient photocatalysts for OER represents a significant challenge in the field of water splitting advancement. Herein we report the bipyridine-based covalent triazine framework (CTF-Bpy) with the periodic metal coordination sites and suitable band gap position for efficient photocatalytic oxygen evolution. Single Co sites are introduced into CTF-Bpy as cocatalyst through a facile immersion treatment. The obtained CTF-Bpy-Co exhibited remarkable photocatalytic oxygen evolution performance, achieving an initial rate of up to 3359 μmol g^-1 h^-1 within the first hour and an average rate of 1503 μmol g^-1 h^-1 over 5 h under visible light irradiation (λ ≥ 420 nm), which exceeds most of the reported porous organic polymers. Moreover, CTF-Bpy-Co can achieve continuous oxygen evolution for a duration of 40 h and the total oxygen production amount of up to 180 μmol. Charge density difference using density functional theory calculations confirm that the Co single site is the reaction site that drives the photooxidation of water to generate oxygen.

Key words: Covalent triazine framework, Bipyridine, Single Co site, Photocatalytic oxygen evolution

Ruixue Sun, Xunliang Hu, Chang Shu, Lirong Zheng, Shengyao Wang, Xiaoyan Wang, Bien Tan. Anchoring single Co sites on bipyridine-based covalent triazine framework for efficient photocatalytic oxygen evolution[J]. Chinese Journal of Catalysis, 2023, 55: 159-170.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(23)64552-8

https://www.cjcatal.com/EN/Y2023/V55/I12/159

Figures/Tables 6

Fig. 1. (a) Schematic representation of the preparation of CTF-Bpy and CTF-Bpy-Co. Solid state 13C CP/MAS spectrum (b), experimental and Pawleyrefined PXRD patterns (c) of CTF-Bpy. (d) N2 sorption isotherms and pore size distribution (inset) of CTF-Bpy.

Fig. 2. (a) The XPS spectra (N 1s) of CTF-Bpy and CTF-Bpy-Co. (b) The XPS spectra (Co 2p) of CTF-Bpy-Co. The Co K-edge XANES (c) and k3-weighted Fourier-transformed Co K-edge EXAFS (d) spectra of CTF-Bpy-Co, CoO, Co2O3, and Co foils and the wavelet transform (WT) spectra of CTF-Bpy-Co. (e) The HAADF and the element mapping images of CTF-Bpy-Co.

Fig. 3. (a) Photocatalytic OER rate of CTF-Bpy-Co with different theoretical contents of Co2+. (b) The average photocatalytic oxygen evolution rate with different contents of Co2+ in the initial 5 h. (c) Comparison of photocatalytic oxygen evolution rate. (d) Apparent quantum yield (AQY) of photocatalytic OER of CTF-Bpy-Co under different irradiation wavelengths. (e) Photocatalytic OER of CTF-Bpy-Co with different dosage in the same photocatalytic condition. (f) Long-time photocatalytic OER performance of CTF-Bpy-Co under visible light irradiation. (Photocatalytic conditions: Temperature = 15 °C, λ ≥ 420 nm).

Fig. 4. UV-Visible absorption spectra and Tauc plots (inset) (a), energy diagram of CTF-Bpy (blue) and CTF-Bpy-Co (pink) (b) from experimental results. (c) Transient photocurrent response under visible light irradiation. (d) Fitting Nyquist plot using equivalent circuits from EIS.

Fig. 5. TAS spectra obtained from suspensions of CTF-Bpy (a) and CTF-Bpy-Co (b) in H2O. The data were obtained using an excitation wavelength of 365 nm. TA kinetics and corresponding fitting curves of CTF-Bpy and CTF-Bpy-Co at 600 nm (c) and 700 nm (d).

Fig. 6. (a) The mechanism of photocatalytic oxidation reaction on CTF-Bpy-Co. (b) Differential charge density diagram between triazine and Bpy-Co sites on CTF-Bpy-Co. (c) Differential charge density diagram between Co and CTF-Bpy sites on CTF-Bpy-Co. Yellow region represents the electron accumulation area, and the blue region represents the electron dissipation area.

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