Nanoscale lamination effect by nitrogen-deficient polymeric carbon nitride growth on polyhedral SrTiO3 for photocatalytic overall water splitting: Synergy mechanism of internal electrical field modulation

doi:10.1016/S1872-2067(23)64414-6

Abstract

Abstract:

The light penetration effect will weaken the driving force of charge separation from phase to surface by the built-in electric field of nanoscale photocatalysts, like low-dimensional materials. Therefore, in this study, a novel nanoscale lamination catalyst design method was proposed using a polymeric carbon nitride (PCN)-nano polyhedral SrTiO₃ core-shell structure catalyst (PCN-SrTiO₃). The results showed that the nanoscale lamination effect could be generated by the formation of the N-Sr bond, which could regulate the built-in electric field of the PCN simultaneously. Moreover, detailed characterization indicated that the N-Sr bond, which facilitates the generation of N vacancies in PCN, could act as a novel channel for charge transfer. Both surface and interior core N-deficient PCN have been discovered, resulting in more positive and negative VB positions, respectively. Synchronously, the light absorption ability of the PCN-SrTiO₃ samples increased. Consequently, the enhanced photocatalytic overall water splitting could be ascribed to the synergism of the built-in electric field regulation caused by the N-Sr formation-induced nanoscale lamination effect, which was favorable for energy flow adaption on the spatiotemporal scale.

Key words: Photocatalytic overall water splitting, Nanoscale lamination effect, Built-in electric field, N-deficient PCN, Nano polyhedral SrTiO₃

Zhidong Wei, Jiawei Yan, Weiqi Guo, Wenfeng Shangguan. Nanoscale lamination effect by nitrogen-deficient polymeric carbon nitride growth on polyhedral SrTiO₃ for photocatalytic overall water splitting: Synergy mechanism of internal electrical field modulation[J]. Chinese Journal of Catalysis, 2023, 48: 279-289.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(23)64414-6

https://www.cjcatal.com/EN/Y2023/V48/I5/279

Figures/Tables 8

Fig. 1. XRD (a), data-processing Raman spectra (b), and TEM, HADDF as well as element mapping results (c) of the prepared samples.

Fig. 2. SEM images of nano polyhedron SrTiO3 (a,b) and 0.5g-SrTiO3-PCN (c,d) under a style of backscattering, and 3D-HRTEM images of 0.5g-SrTiO3-PCN at different angles (e).

Fig. 3. XPS results of the prepared samples. (a) N 1s; (b) FT-IR spectra; (c) EPR results; (d) Cross Polarization Solid-state 13C MAS NMR spectra of selected samples as well as a possible structural change in heptazine units before and after N-Sr bond formation.

Fig. 4. Normalized Sr K-edge XANES spectra (a), the Fourier transform (FT) of EXAFS k2χ(k) spectra and the magnitude R-space experimental data fitting (b-f), and wavelet transform (WT) of k3-weighted EXAFS signals of the selected samples (g-j).

Fig. 5. UV-vis spectra (a), the VB position variation (b) after being calculated based on XPS VB, Mott-Schottky results.

Fig. 6. Photocatalytic overall water splitting performance with PtOx and CoOx as co-catalysts. 0.25g-SrTiO3-PCN (a), 0.5g-SrTiO3-PCN (b), recycle activity of 0.5g-SrTiO3-PCN results (c), 1 g-SrTiO3-PCN (d), 2g-SrTiO3-PCN (e), as well as 3g-SrTiO3-PCN (f).

Fig. 7. (a) The model of PCN deposited on the facets of SrTiO3 and the isosurface map of charge density differences at different visual angles. The C, N, O, Ti, and Sr atoms are represented as brown, silver, light blue, red, and green, respectively. (b) The SPV results of PCN, STO, and 0.5g-SrTiO3-PCN. (c) Theory work function of SrTiO3. (d) AFM results of SrTiO3 (SKPM pattern). (e) Mott-Schottky results of PCN; AFM results of PCN (SKPM pattern) (f) and the theoretical mechanisms (g) of the built-in electric field formation by PCN and SrTiO3.

Fig. 8. (a) AFM results of 0.5g-SrTiO3-PCN (SKPM pattern). The SPV intensity (b) and the zeta potential (c) of each sample.

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Nanoscale lamination effect by nitrogen-deficient polymeric carbon nitride growth on polyhedral SrTiO₃ for photocatalytic overall water splitting: Synergy mechanism of internal electrical field modulation

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