Hexanuclear ring cobalt complex for photochemical CO2 to CO conversion

doi:10.1016/S1872-2067(22)64144-5

Abstract

Abstract:

Photosynthesis in nature has been deemed as the most significant biochemical reaction, which maintains a relatively stable content of O₂ and CO₂ in the atmosphere. Herein, for a deeper comprehension of natural photosynthesis, an artificial photosynthesis model reaction of photochemical CO₂ to CO conversion (CO₂ +2 H⁺ + 2e^- → CO + H₂O) catalyzed by a homogeneous hexanuclear ring cobalt complex {K₂[CoO₃PCH₂N(CH₂CO₂)₂]}₆ (Co6 complex) is developed. Using the [Ru(bpy)₃]²⁺ as a photosensitizer and TEOA as a sacrificial electron donor, an optimal turnover frequency of 503.3 h^‒1 and an apparent quantum efficiency of 0.81% are obtained. The good photocatalytic CO₂ reduction performance is attributed to the efficient electron transfer between Co6 complex and [Ru(bpy)₃]²⁺, which boosts the photogenerated carriers separation of the photosensitizer. It is confirmed by the j-V curves, light-assisted UV-vis curves, steady-state photoluminescence spectra and real-time laser flash photolysis experiments. In addition, the proposed catalytic mechanism for CO₂ reduction reaction catalyzed by the Co6 complex is explored by the potassium thiocyanate poison experiment, Pourbaix diagram and density functional theory calculations.

Key words: Photosynthesis, Homogeneous catalysis, CO₂ reduction reaction, Density functional theory, Hexanuclear ring cobalt complex

Xiangyu Meng, Rui Li, Junyi Yang, Shiming Xu, Chenchen Zhang, Kejia You, Baochun Ma, Hongxia Guan, Yong Ding. Hexanuclear ring cobalt complex for photochemical CO₂ to CO conversion[J]. Chinese Journal of Catalysis, 2022, 43(9): 2414-2424.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(22)64144-5

https://www.cjcatal.com/EN/Y2022/V43/I9/2414

Figures/Tables 8

Fig. 1. Ball and stick model of Co6 complex (K cations and H atoms were omitted for clarity).

Fig. 2. (a) Measured and simulated PXRD patterns. (b-d) XPS survey, high resolution Co 2p and C 1s XPS spectra of Co6 complex.

Fig. 3. (a) Single variable control experiments of CO2RR. (b) Different concentrations of Co6 complex for CO2RR. (c) TOFs for Co6 complex with different concentrations. (d-f) Kinetic curves for gas evolution amount, TONs and CO selectivity over 20 µmol L?1 Co6 complex.

Fig. 4. Proposed photocatalytic CO2RR general mechanism.

Fig. 5. (a,b) Pourbaix diagram of Co6 complex under reduction state and oxidation state. (c) LSV curve of [Ru(bpy)3]2+. (d) Electrode potential comparison.

Fig. 6. Calculated free energy diagram for CO evolution over the single Co site (a,b) and double Co sites (c,d) in the Co6 complex.

Fig. 7. Possible mechanism of Co6 complex for photocatalytic CO2RR.

Fig. 8. (a,b) j-V curves and result. Steady state PL spectra (c) and light assisted UV-vis curves (d) of samples.

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Hexanuclear ring cobalt complex for photochemical CO₂ to CO conversion

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