Regulation on polymerization degree and surface feature in graphitic carbon nitride towards efficient photocatalytic H2 evolution under visible-light irradiation

doi:10.1016/j.jmst.2021.05.019

Abstract

Abstract:

A kind of graphitic carbon nitride (TSC-550) with high polymerization degree and improved surface property was prepared by a new precursor of thiosemicarbazide. The sulfur motif and high nitrogen content in thiosemicarbazide promoted the polymerization of thiosemicarbazide to form graphitic carbon nitride framework with high degree of polymerization, which significantly influenced the electronic structure and surface chemical properties. TSC-550 possessed a narrow bandgap of 2.19 eV that facilitated the utilization of visible light, and possessed a less positive charge, acidic surface that resulted in enhanced hydrogen adsorption ability in water solution, which promoted the H₂ evolution kinetics. In addition, the extended π-conjugated electronic system promoted the separation and migration of photo-generated charge carries in plane of TSC-550 framework, as well as the increasing interlayer C-N interactions in TSC-550 created conductive paths across the layers to tunnel interlayers for rapid electron transportation. As a result, TSC-550 nanosheets showed excellent photocatalytic H₂ production activity, the AQY achieved 36.4% at 425 nm.

Key words: Degree of polymerization, Graphitic carbon nitride, Photocatalysis, Solar energy, Hydrogen

Cheng Cheng, Chung-Li Dong, Jinwen Shi, Liuhao Mao, Yu-Cheng Huang, Xing Kang, Shichao Zong, Shaohua Shen. Regulation on polymerization degree and surface feature in graphitic carbon nitride towards efficient photocatalytic H₂ evolution under visible-light irradiation[J]. J. Mater. Sci. Technol., 2022, 98: 160-168.

Figures/Tables 7

Fig. 1. (a) XRD patterns, (b) FTIR spectra, high-resolution XPS spectra of (c) C 1s and (d) N 1s for TSC-550 and TU-550.

Fig. 2. (a) N K-edge XANES, (b) C K-edge XANES and (c) EPR spectra for TSC-550 and TU-550; (d) proposed structure of thiosemicarbazide-derived graphitic carbon nitride.

Fig. 3. (a) UV-vis spectra, (b) Tauc plots, (c) VB XPS spectra and (d) eletronic band structure alignments for TSC-550 and TU-550.

Fig. 4. (a) Steady-state PL spectra, (b) time-resolved transient PL decay spectra, (c) C K-edge and (d) N K-edge XANES spectra with or without illumination for TSC-550 and TU-550.

Fig. 5. (a) Apparent Zeta potential, (b) CV curves, (c) EIS plots and (d) time courses of transient photocurrent density curves for TSC-550 and TU-550.

Fig. 6. (a) Photocatalytic H2-production activities for TU-550, 550 and TSC-550+K2HPO4 under visible-light irradiation (λ > 420 nm); (b) wavelength-dependent AQYs for TSC-550 at different wavelengths (425, 440, 480, 520 and 550 nm); (c) photocatalytic H2-production activities for TSC-550 under different light-spectrum irradiation (λ > 420, 450, 480, 500, 530 and 560 nm); (d) photocatalytic H2-production stability test for TSC-550 under visible-light irradiation (λ > 420 nm). “TSC-550+K2HPO4” represented the photocatalytic H2-production activity for TSC-550 by adding 0.08 mol of K2HPO4 in the reaction solution while keeping other measurement conditions the same.

Fig. 7. (a) TEM image of TSC-550NS, (b) N2 adsorption-desorption isotherms for TSC-550 and TSC-550NS, (c) photocatalytic H2-evolution activities for TSC-550, TSC-550+K2HPO4, TSC-550NS and TSC-550NS+K2HPO4 under visible-light irradiation (λ > 420 nm), (d) wavelength-dependent AQYs for TSC-550NS at different wavelength (425, 440, 480, 520 and 550 nm). “TSC-550NS+K2HPO4” represented the photocatalytic H2-production activity for TSC-550 by adding 0.08 mol of K2HPO4 in the reaction solution while keeping other measurement conditions the same.

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Regulation on polymerization degree and surface feature in graphitic carbon nitride towards efficient photocatalytic H₂ evolution under visible-light irradiation

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