Construction of intramolecular and interfacial built-in electric field in a donor-acceptor conjugated polymers-based S-scheme heterojunction for high photocatalytic H2 generation

doi:10.1016/S1872-2067(23)64602-9

Abstract

Abstract:

Engineering a robust built-in electric field (IEF) is favorable for boosting carrier separation and achieving high photocatalytic performance. Herein, we developed a donor-acceptor conjugated polymer-based S-scheme heterojunction, utilizing both intramolecular and interfacial IEF to enhance carrier separation and achieve superior photocatalytic performance. Specifically, the intramolecular IEF was established by introducing 1,6-dibromopyrene into carbon nitride (CN) to form 1,6-dibromopyrene grafted CN (CNPy). Concurrently, the S-scheme heterojunction was formed by coupling CNPy with CdSe nanoparticles to create an interfacial IEF. Experimental findings demonstrated that the combined effect of intramolecular and interfacial IEF within the CdSe/CNPy heterojunction significantly improved the carrier separation and retained strong redox capacity. Benefiting from these advantages, the optimized composite, 100%CdSe/CNPy-0.2, showed the highest H₂ generation rate of 1.16 mmol•g^-1•h^-1, surpassing those of pure CNPy-0.2, CdSe and 100%CdSe/CN by 58, 2.2 and 2.32 times, respectively. This study introduces an innovative design strategy for IEF-regulated conjugated polymer-based materials, paving the way for efficient solar-to-chemical energy conversion.

Key words: g-C₃N₄, Intramolecular built-in electric field, Interfacial built-in electric field, S-Scheme heterostructure, Photocatalyst

Lele Wang, Wenyao Cheng, Jiaxin Wang, Juan Yang, Qinqin Liu. Construction of intramolecular and interfacial built-in electric field in a donor-acceptor conjugated polymers-based S-scheme heterojunction for high photocatalytic H₂ generation[J]. Chinese Journal of Catalysis, 2024, 58: 194-205.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(23)64602-9

https://www.cjcatal.com/EN/Y2024/V58/I3/194

Figures/Tables 11

Scheme 1. Possible reaction pathway for the incorporation of 1,6-dibromopyrene into g-C3N4 networks, and the synthetic process of CdSe/CNPy composites.

Fig. 1. (a) XRD patterns of CN and CNPy samples. (b,c) FTIR spectra of CN and CNPy samples. (d) Molecular fragments of CNPy samples.

Fig. 2. (a) XPS survey spectra of CN and CNPy-0.2 sample. (b,c) The high-resolution C 1s and N 1s spectra for the CN and CNPy-0.2 sample. (d) Quantitative elemental analysis based on the XPS spectra of CN, CNPy-0.2 sample. (e) Schematic representation of D-A distribution in CNPy samples. The surface charge density (f), DRS spectra (g) and photocatalytic HER (h,i) of CN and CNPy samples.

Fig. 3. (a) XRD patterns of CdSe, CdSe/CN and CdSe/CNPy-0.2 samples. (b) XPS survey spectra of CdSe, 100%CdSe/CN and 100%CdSe/CNPy-0.2 samples. Quantitative elemental analysis from the XPS spectra of Cd 3d (c), Se 3d (d), C 1s (e) and N 1s (f).

Fig. 4. (a,c,e) SPV images (CPD = (Φs-Φp)/e). (b,d,f) Line profiles of the SPV difference.

Fig. 5. SEM and TEM images of CN (a,d), CNPy-0.2 (b,e), CdSe (c,f) and 100%CdSe/CNPy-0.2 (g,h) samples. (i-l) TEM element mapping images in 100%CdSe/CNPy-0.2 sample.

Fig. 6. (a,b) Photocatalytic hydrogen evolution and reaction rates of the CN, CNPy, CdSe, CdSe/CN and CdSe/CNPy samples. (c,d) Hydrogen evolution performance of different sacrificial agents or different lights. (e) The cycling photocatalytic hydrogen evolution of 100% CdSe/CNPy-0.2. (f) Degradation of tetracycline using different catalysts. (g) Degradation rate and (h) the cycling TC degradation of 100% CdSe/CNPy-0.2 sample. (i) XRD patterns of 100% CdSe/CNPy-0.2 sample before and after the reaction.

Fig. 7. Photocurrent response (a), Nyquist plots (b), steady state PL emission spectra (c) and surface photovoltage (d) of different samples including CN, CNPy-0.2, CdSe, 100% CdSe/CN and 100% CdSe/CNPy samples.

Fig. 8. (a) UV-vis diffuse reflectance spectra. Taus plots (b), Mott-Schottky plots (c), electronic bandgap structures (d) of CN, CNPy-0.2 and CdSe samples. EPR spectra of DMPO-·O2- (e) and DMPO-·OH (f) of CNPy-0.2, CdSe and 100%CdSe/CNPy-0.2 sample.

Fig. 9. The high-resolution analysis from the XPS spectra of C 1s (a), N 1s (b), Cd 3d (c) and Se 3d (d).

Fig. 10. The charge transfer mechanism of CdSe/CNPy composites before (a) and after (b) photoexcitation. (c) Photocatalytic HER mechanism of CdSe/CNPy composites under light excitation.

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Construction of intramolecular and interfacial built-in electric field in a donor-acceptor conjugated polymers-based S-scheme heterojunction for high photocatalytic H₂ generation

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