One-pot synthesis of array-like sulfur-doped carbon nitride with covalently crosslinked ultrathin MoS2 cocatalyst for drastically enhanced photocatalytic hydrogen evolution

doi:10.1016/j.jmst.2020.10.030

Abstract

Abstract:

Constructing noble-metal-free loaded catalyst with high-efficiency photocatalytic activity by a simple and scalable method is of profound significance for fundamental research and practical application. Herein, a simple one-pot method was used to synthesize novel samples of array-like sulfur-doped graphitic carbon nitride (SCN) nanosheets with ultrathin MoS₂ loading (MS/SCN-x%). The ultrathin MoS₂ cocatalyst was evenly distributed on the surface of SCN and was linked to the main catalyst by covalent chemical bonds. Benefited from the multiple advantages of the array-like porous nanosheets structure with rich exposed surface, covalent cross-linking structure, and enhanced visible light absorption, the MS/SCN-2.5 % composites drastically improve hydrogen evolution performance, which is superior to original MoS₂ nanosheet modified by two-step mixing method, and also rivals with Pt/SCN. The designing strategy of photocatalyst modified by noble-metal-free cocatalyst with covalent bond structure provides fascinating insights into enhanced photocatalytic hydrogen evolution.

Key words: Carbon nitride, Noble-metal-free cocatalyst, Covalent cross-linking, Photocatalytic hydrogen evolution

Shumin Zhang, Hu Dong, Changsheng An, Zhongfu Li, Difa Xu, Kaiqiang Xu, Zhaohui Wu, Jie Shen, Xiaohua Chen, Shiying Zhang. One-pot synthesis of array-like sulfur-doped carbon nitride with covalently crosslinked ultrathin MoS₂ cocatalyst for drastically enhanced photocatalytic hydrogen evolution[J]. J. Mater. Sci. Technol., 2021, 75: 59-67.

Figures/Tables 12

Fig. 1. Scheme illustration of the formation of MS/SCN-x% composites.

Fig. 2. SEM images of SCN (a), MoS2 (b), MS/SCN-0.5 % (c), MS/SCN-1.5 % (d), MS/SCN-2.5 % (e) and MS/SCN-5.0 % (f).

Fig. 3. TEM (a, b), HRTEM (c) images and elemental mapping of MS/SCN-2.5 % composite.

Fig. 4. N2 adsorption-desorption isotherms (a) the corresponding BJH pore size distribution and pore volume (b) of SCN and MS/SCN-2.5 %.

Fig. 5. Physical characterizations of MS/SCN-2.5 %, together with g-C3N4 and SCN as reference samples. (a) XRD patterns. (b) FT-IR spectra.

Fig. 6. XPS spectra of MS/SCN-2.5 %, SCN and MoS2: (a) C 1s (b) N 1s (c) Mo 3d (d) S 2p.

Fig. 7. N1 s high-resolution spectra of MS/SCN-20 % prepared by one-step calcining.

Fig. 8. UV-vis diffuse reflection spectra of g-C3N4, MoS2 and MS/SCN-x% composites (MS/SCN-0.5 %, MS/SCN-1.5 %, MS/SCN-2.5 %, MS/SCN-5.0 %).

Fig. 9. (a) Time course of H2 evolution over SCN and MS/SCN-x% composite (MS/SCN-0.5 %, MS/SCN-1.5 %, MS/SCN-2.5 %, MS/SCN-5.0 %); (b) Recycling test of MS/SCN-2.5 % composite; (c) The effect of MoS2 cocatalyst on the hydrogen evolution activity; (d) Comparison of photocatalyst hydrogen evolution activity of the SCN, MoS2, MS/SCN-2.5 %, SCN/Pt and MoS2/SCN-R.

Fig. 10. (a) Fluorescence emission spectra of SCN and MS/SCN-2.5 %; (b) Time-resolved PL delay spectra of SCN and MS/SCN-2.5 %; (c) Transient photocurrent curves; (d) EIS Nyquist plots of SCN and MS/SCN-x% composites.

Fig. 11. Tauc plots (a) and XPS valence band (b) of g-C3N4 and SCN.

Fig. 12. Schematic illustration of the photocatalytic hydrogen evolution process in MS/SCN-x% composites under visible light irradiation.

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One-pot synthesis of array-like sulfur-doped carbon nitride with covalently crosslinked ultrathin MoS₂ cocatalyst for drastically enhanced photocatalytic hydrogen evolution

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