Step-scheme CdS/TiO2 nanocomposite hollow microsphere with enhanced photocatalytic CO2 reduction activity

doi:10.1016/j.jmst.2020.02.062

Abstract

Abstract:

Converting solar energy into chemical energy by artificial photosynthesis is promising in addressing the issues of the greenhouse effect and fossil fuel crisis. Herein, a novel photocatalyst, i.e. CdS/TiO₂ hollow microspheres (HS), were dedicatedly designed to boost overall photocatalytic efficiency. TiO₂ nanoparticles were in-situ decorated on the inside and outside the shell of CdS HS, ensuring close contact between TiO₂ and CdS. The CdS/TiO₂ HS with abundant mesopores inside of the shell boost the light absorption via multiscattering effect as well as accessible to reactions in all directions. The heterojunction was scrutinized and the charge transfer across it was revealed by in-situ irradiated X-ray photoelectron spectroscopy (ISI-XPS). Ultimately, the charge transfer in this composite was determined to follow step-scheme mechanism, which not only facilitates the separation of charge carriers but also preserves strong redox ability. Benefited from the intimate linkage between CdS and TiO₂ and the favorable step-scheme heterojunction, enhanced photocatalytic CO₂ reduction activity was accomplished. The CH₄ yield rate of CdS/TiO₂ reaches 27.85 μmol g^-1 h^-1, which is 145.6 and 3.8 times higher than those of pristine CdS and TiO₂, respectively. This work presents a novel insight into constructing step-scheme photocatalytic system with desirable performance.

Key words: Step-scheme heterojunction, CdS, TiO₂, Hollow microspheres, Photocatalytic CO₂ reduction

Zhongliao Wang, Yifan Chen, Liuyang Zhang, Bei Cheng, Jiaguo Yu, Jiajie Fan. Step-scheme CdS/TiO₂ nanocomposite hollow microsphere with enhanced photocatalytic CO₂ reduction activity[J]. J. Mater. Sci. Technol., 2020, 56: 143-150.

Figures/Tables 6

Fig. 1. (a) The formation procedures of CdS/TiO2 HS. FESEM images of CdS HS (b) and CdS/TiO2 HS (c, d); TEM (e, f), HRTEM image (g) and its corresponding EDS elemental mapping images of CdS/TiO2 HS (h). Note that CdS/TiO2 refers to CdS/TiO2 1:1 in this paper unless otherwise stated.

Fig. 2. (a) Photocatalytic CO2 reduction activity tests under full-spectrum irradiation of CdS HS, TiO2 and CdS/TiO2 HS with various molar ratios. (b) Stability tests for CdS/TiO2 HS 1:1. (c, d) Gas chromatography-mass spectrometry (GC-MS) analysis of the resultant CH4 and CO for CdS/TiO2 composite, respectively.

Fig. 3. In-situ DRIFTS spectra of (a) the surface adsorbed carbonate species and (b) intermediates in photocatalytic CO2 reduction for CdS/TiO2 HS (0-60 min under dark conditions and 60-120 min under full-spectrum irradiation).

Fig. 4. High-resolution XPS for (a) Cd 3d, (b) S 2p, (c) Ti 2p, and (d) O 2p of CdS/TiO2 without or with 365 nm LED irradiation (CdS/TiO2 UV).

Fig. 5. Electrostatic potentials of (a) CdS (100) and (b) TiO2 (101) surface.

Fig. 6. (a) The work functions of CdS and TiO2 before contact. (b) Thermodynamic electron transfer after contact with the formation of a balanced Fermi level and IEF. (c) The step-scheme electrons transfer diagram between CdS and TiO2 under the full spectrum.

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Step-scheme CdS/TiO₂ nanocomposite hollow microsphere with enhanced photocatalytic CO₂ reduction activity

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