One-step supramolecular preorganization constructed crinkly graphitic carbon nitride nanosheets with enhanced photocatalytic activity

doi:10.1016/j.jmst.2021.07.014

Abstract

Abstract:

Here we report a new one-step thermal polycondensation process to form crinkly graphitic carbon nitride nanosheets (CGCNNs) via supramolecular preorganization, using a mixture of urea and melamine as the starting material. Systematical studies reveal that the newly developed CGCNNs significantly strengthen the optical absorption, widen the bandgap, and increase the Hall mobility and carrier density compared to that of its bulk counterpart, regardless of the similar chemical composition and structure. As a result, the photocatalytic hydrogen production rate is improved by 7 times. Moreover, Na doping of CGCNNs can further promote its photocatalytic activity, leading to an excellent photocatalytic hydrogen production rate of 250.9 µmol h^-1, which is approximately 10.5 times higher than its bulk counterpart. Moreover, an impressive apparent quantum efficiency of 19.12% is achieved at 420 nm. This study provides a facile strategy for the design of efficient low-cost carbon-nitride-based photocatalysts for solar fuel production.

Key words: Carbon nitride, Supramolecular preorganization, Hall mobility, Na doping, Solar hydrogen

Songcan Wang, Yuelin Li, Xin Wang, Guohao Zi, Chenyang Zhou, Boyan Liu, Gang Liu, Lianzhou Wang, Wei Huang. One-step supramolecular preorganization constructed crinkly graphitic carbon nitride nanosheets with enhanced photocatalytic activity[J]. J. Mater. Sci. Technol., 2022, 104: 155-162.

Figures/Tables 5

Scheme. 1. Schematic illustration of the conversion of cyanuric acid from urea, the hydrogen-bonded supramolecular melamine-cyanuric acid (MCA), and the final produced g-C3N4 during thermal polycondensation of a mixture of melamine and urea. Dotted lines represent the hydrogen bonds.

Fig. 1. SEM images of (a) BCN and (b) CGCNNs. (c) TEM image of CGCNNs. (d) XRD patterns of BCN and CGCNNs. (e) N2 adsorption and desorption isotherms, and (f) BET surface area of BCN and CGCNNs. Insets in (e): digial images of 4 mL of BCN and CGCNNs.

Fig. 2. (a) XPS survey spectra, (b) C 1s, (c) N 1s, and (d) FTIR spectra of BCN and CGCNNs.

Fig. 3. (a) UV-vis light absorption curves, (b) estimated bandgaps, (c) PL spectra, (d) EIS spectra, (e) enlarged EIS spectra, (f) transient photocurrent responses, (g) Hall mobility, (h) carrier density, and (i) band structure alignment of BCN and CGCNNs. Inset in (d): the equivalent circuit model.

Fig. 4. (a) Photocatalytic hydrogen production rates, (b) photocatalytic hydrogen evolution plots, and (c) AQE at 420 nm of BCN, CGCNNs, and CGCNNs-Na. (d) stability evaluation of photocatalytic hydrogen production of CGCNNs-Na.

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