Theoretical design and experimental study of pyridine-incorporated polymeric carbon nitride with an optimal structure for boosting photocatalytic CO2 reduction

doi:10.1016/S1872-2067(22)64159-7

Abstract

Abstract:

Herein, pyridine-incorporated polymeric carbon nitride (PCN) was explored for boosting photocatalytic CO₂ reduction. First, theoretical calculations were performed on PCN models with pyridine molecules located at different positions to determine the optimal structure of pyridine-incorporated PCN with the lowest total energy, smallest bandgap, and most efficient CO₂ adsorption and activation processes. Subsequently, pyridine-incorporated PCN with the optimal structure was prepared experimentally by copolymerizing urea and 2-aminopyridine (AP). A high CO evolution rate with a selectivity of 99.6% was achieved by combining CN-5%AP with a Co(bpy)₂ co-catalyst, which resulted an apparent quantum efficiency of 2.86% at λ = 420 nm. The high performance of pyridine-incorporated PCN mainly originated from its strong CO₂ adsorption ability and facilitation of the CO₂-to-CO reduction reaction. This work paves the way for the precise design and preparation of photocatalysts with high CO₂ reduction efficiency.

Key words: Photocatalytic CO₂ reduction, Theoretical first and then experiment, Polymeric carbon nitride, Density functional theory, Pyridine

Chengcheng Chen, Fangting Liu, Qiaoyu Zhang, Zhengguo Zhang, Qiong Liu, Xiaoming Fang. Theoretical design and experimental study of pyridine-incorporated polymeric carbon nitride with an optimal structure for boosting photocatalytic CO₂ reduction[J]. Chinese Journal of Catalysis, 2023, 46: 91-102.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(22)64159-7

https://www.cjcatal.com/EN/Y2023/V46/I3/91

Figures/Tables 7

Fig. 1. The DFT model structures of BCN (a), CN-N2 (b) and CN-N3 (c), calculated band gaps of BCN (d), CN-N2 (e) and CN-N3(f), and density of states of BCN (g), CN-N2 (h) and CN-N3 (i).

Fig. 2. The DFT model structure of CO2 molecule on BCN (a), CO2 on CN-N2 (b), CO2 on CN-N3 (c), together with the electron density difference of CO2 on BCN(d), CO2 on CN-N2(e), CO2 on CN-N3 (f).

Fig. 3. XPS high resolution C 1s (a) and N 1s (b) spectra of BCN, CN-5%AP and CN-10%AP. (c) The XANES C K-edge profiles of BCN and CN-5%AP. (d) Solid-state 13C MAS NMR spectra of BCN and CN-5%AP. (e) TGA curves of urea, AP, and their mixture (the inset is the enlarge profile range from 200 to 300 °C). (f) High resolution mass spectrum of the product prepared by heating the mixture consisting of urea and 5% AP at 200 °C for 30 min.

Scheme 1. Speculated formation mechanism of the pyridine incorporated PCN containing the CN-N2 structure.

Fig. 4. DRS spectra (a), the Kubelk-Munk function (b) and PL emission spectra (c) of BCN, CN-3%AP, CN-5%AP and CN-7%AP. (d) Time-resolved PL decay spectra of BCN and CN-5%AP.

Fig. 5. CO release rate (a) and selectivity (b) of BCN and CN-x%AP under the illumination of a LED of 3 W. (c) A comparison in CO release rate between BCN and CN-5%AP under irradiation of the 300 W Xe lamp. (d) The AQE of CN-5%AP.

Fig. 6. CO2 TPD (a) and CO2 absorption uptake (b) of BCN and CN-5%AP and reaction coordination path (c) over BCN and CN-N2. (d) In situ FTIR spectra for the adsorption and activation of CO2 on CN-5%AP.

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Theoretical design and experimental study of pyridine-incorporated polymeric carbon nitride with an optimal structure for boosting photocatalytic CO₂ reduction

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