Regulating interfacial coupling of 1D crystalline g-C3N4 nanorods with 2D Ti3C2Tx MXene for boosting photocatalytic CO2 reduction

doi:10.1016/S1872-2067(23)64513-9

Abstract

Abstract:

Two-dimensional (2D) layered photocatalysts coupled with 2D Ti₃C₂T_x (T = OH, O, or F) MXene cocatalysts in 2D/2D configuration have been extensively studied for use in artificial photosynthesis. Unfortunately, the overall photoreaction efficiency of these cocatalysts is often limited by weak 2D/2D interfacial van der Waals interactions, high interfacial electrostatic barriers, and slow interfacial charge transfer. In this study, 1D crystalline g-C₃N₄ (CCN) nanorods are grown along the c-axis using the molten-salt method and assembled onto a 2D Ti₃C₂T_x substrate by freeze-drying-assisted interfacial coupling, forming a unique Schottky junction photocatalyst in a 1D/2D configuration with interfacial hydrogen bonds. Transfer of photoelectrons in the CCN nanorods could along the radial π-conjugated plane to the hydrogen-bonded 2D Ti₃C₂T_x in the 1D/2D configuration is more efficient than the slow interlayer charge transfer in catalysts with a conventional 2D/2D configuration. Consequently, the optimized 1D-CCN/2D-Ti₃C₂T_x hybrid photocatalyst assembled by freeze-drying (TC/CCN-FD) exhibited an outstanding photocatalytic CO₂ reduction activity at a rate of 2.13 μmol g^-1 h^-1, being 5.6 and 8.9 times more efficient than the pristine 1D CCN and 2D bulk g-C₃N₄ counterparts, respectively. Moreover, the selectivity towards the multielectron reduction product (CH₄) was significantly enhanced over TC/CCN-FD owing to the faster interfacial charge transfer across the CCN/Ti₃C₂T_x interface and the higher density of photoelectrons on the Ti₃C₂T_x cocatalysts. This work will inspire further studies on suppressing the interfacial charge transfer barrier by matching the interfacial crystal orientation and strengthening the interfacial interactions.

Key words: Ti₃C₂T_x, Crystalline carbon nitride, 1 dimension/2 dimension, Photocatalytic CO₂ reduction, Cocatalyst

Ruiyu Zhong, Yujie Liang, Fei Huang, Shinuo Liang, Shengwei Liu. Regulating interfacial coupling of 1D crystalline g-C₃N₄ nanorods with 2D Ti₃C₂T_x MXene for boosting photocatalytic CO₂ reduction[J]. Chinese Journal of Catalysis, 2023, 53: 109-122.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(23)64513-9

https://www.cjcatal.com/EN/Y2023/V53/I10/109

Figures/Tables 12

Scheme 1. Schematic of the synthesis of the TC/CCN-FD catalyst.

Fig. 1. SEM images of CCN (a), Ti3C2Tx (b), and TC/CCN-FD (c,d).

Fig. 2. TEM (a), HRTEM (b), HAADF-STEM (c) images, along with the corresponding EDS elemental maps (d?h) of TC/CCN-FD.

Fig. 3. XRD patterns (a), Raman (b), FTIR (c), and EPR (d) spectra of the as-prepared samples.

Fig. 4. XPS spectrum (a), and high-resolution XPS C 1s (b), Ti 2p (c), N 1s (d), O 1s (e), and F 1s (f) spectra.

Fig. 5. N2 adsorption-desorption isotherms (a) and CO2 adsorption curves (b) of CCN, TC/CCN-FD, TC/CCN-MM, and Ti3C2Tx samples. The inset in (a) shows the corresponding pore size distribution profiles.

Fig. 6. UV-vis DRS (a), the plots of (αhυ)1/2 vs. (hυ) (b), the Mott-Schottky curves (c) and the band structure alignment (d) of CCN, TC/CCN-FD and Ti3C2Tx samples.

Fig. 7. PL (a), TRPL (b) spectra, transient photocurrent responses (c), and EIS Nyquist plots (d) of prepared samples.

Fig. 8. (a) CO2 reduction products of various samples obtained under full spectrum irradiation. (b) Stability test of the photocatalytic production rate on a typical TC/CCN-FD sample. (c) CO2RR generation rates on typical samples obtained under different situations. (d) Wavelength-dependent CO2 reduction of TC/CCN-FD under monochromatic light exposure for 1 h. (e,f) In situ DRIFTS of TC/CCN-FD during the adsorption stage (0-1 h) and under irradiation (1-2 h).

Fig. 9. Calculated Fermi levels of CCN (a) and Ti3C2Tx (b) (Insets: optimized structures). The calculated differential charge density distribution and optimized structures of TC/CCN-FD (c,d) and TC/CCN-P (e,f). Charge accumulation and depletion are shown in blue and red, respectively. Gray, pink, green, silver, and white spheres represent C, N, O, Ti, and H atoms, respectively.

Fig. 10. The calculated electrostatic potentials of TC/CCN-FD (a) and TC/CCN-P (b).

Scheme 2. Possible photocatalytic mechanisms for CO2 reduction of TC/CCN-FD.

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Regulating interfacial coupling of 1D crystalline g-C₃N₄ nanorods with 2D Ti₃C₂T_x MXene for boosting photocatalytic CO₂ reduction

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