Comprehensive investigation on robust photocatalytic hydrogen production over C3N5

doi:10.1016/S1872-2067(21)63813-5

Abstract

Abstract:

Carbon nitride has drawn numerous eyes in the past decade, whereas the photocatalytic performance is significantly limited by its wide band-gap (~2.7 eV for C₃N₄) simultaneously. Recently, C₃N₅ with narrower band-gap has been reported, however, a systematically investigation on its photoactivity for H₂ production has not been reported. The present work demonstrates the synthesis of C₃N₅ by thermal treatment of 3-amino-1,2,4-triazole, and the photocatalytic performance for H₂ production of C₃N₅is investigated comprehensively. Photocatalytic H₂ production rate of C₃N₅ is ~2.2 times higher than that of C₃N₄ with 1.0 wt% Pt as co-catalyst, and series of experiments are carried out to explore the behind elements accounting for the high photoactivity. Combining the results of DRS, PL and photocurrent, it is found that C₃N₅ possesses wider visible light absorption region, lower band-gap and quicker photogenerated e ^-/h ⁺ separation efficiency. Moreover, characterizations including in-situ DRIFTS are adopted to monitor the adsorption property of H₂O on C₃N₅, which plays a significant role in surface water reduction reaction, and higher amount of adsorbed H₂O molecules on C₃N₅ is confirmed. The present work exhibits new insights into the high photocatalytic performance of N-rich carbon nitride catalysts.

Key words: C₃N₅, Photocatalysis, H₂ production, In-situ DRIFTS, Water adsorption

Cong Peng, Lixiao Han, Jinming Huang, Shengyao Wang, Xiaohu Zhang, Hao Chen. Comprehensive investigation on robust photocatalytic hydrogen production over C₃N₅[J]. Chinese Journal of Catalysis, 2022, 43(2): 410-420.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63813-5

https://www.cjcatal.com/EN/Y2022/V43/I2/410

Figures/Tables 11

Scheme 1. XRD patterns of C3N5 and Pt-C3N5.

Fig. 1. XRD patterns of C3N5 and Pt-C3N5.

Fig. 2. TEM and HRTEM images of C3N5 (a,b) and 1.0 wt% Pt-C3N5 (c,d).

Fig. 3. XPS spectra of C3N5 and Pt-C3N5.

Fig. 4. (a) FTIR spectrum of C3N5; (b) DRS spectra of C3N5 and Pt-C3N5 (Insert: photographs of C3N5 and Pt-C3N5).

Fig. 5. (a) Comparison of H2 production activity over C3N5, Pt-C3N5, P-Pt-C3N5 and Pt-C3N4, with 1.0 wt% Pt loading amount; Effects of Pt loading amount (b), concentration of catalyst (c) and TEOA (d) on H2 production activity over Pt-C3N5. Conditions: λ > 420 nm, 45 mg catalyst and 10 mol% TEOA for (b), 1.0 wt% Pt and 10 vol% TEOA for (c), 45 mg catalyst and 1.0 wt% Pt for (d).

Fig. 6. Plots of transformed Kubelka-Munk function versus photon energy (a) and VB-XPS spectra (b) for C3N5 and C3N4. Mott-Schottky plots of C3N5 (c) and C3N4 (d).

Fig. 7. PL (a), photocurrent-time (b) and EIS (c) curves of C3N5, 1.0 wt% Pt-C3N5 and C3N4.

Fig. 8. TGA (a), contact angle (b) and in-situ DRIFTS (c,d) of C3N5 and C3N4.

Fig. 9. AQY values (a) and long-term stability (b) for H2 production over 1.0 wt% Pt-C3N5 under the above mentioned selected conditions.

Fig. 10. Comparison of XRD patterns (a) and DRS spectra (b) of C3N5 before and after photocatalytic reaction.

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Comprehensive investigation on robust photocatalytic hydrogen production over C₃N₅

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