Accelerating directional charge separation via built-in interfacial electric fields originating from work-function differences

doi:10.1016/S1872-2067(20)63649-X

Abstract

Abstract:

In this work, a hierarchical porous SnS₂/rGO/TiO₂ hollow sphere heterojunction that allows highly-efficient light utilization and shortening distance of charge transformation is rationally designed and synthesized. More importantly, an rGO interlayer is successfully embedded between the TiO₂hollow sphere shells and outermost SnS₂ nanosheets. This interlayer functions as a bridge to connect the two light-harvesting semiconductors and acts as a hole injection layer in the tandem heterojunction. The induced built-in electric fields on both sides of the interface precisely regulate the spatial separation and directional migration of the photo-generated holes from the light-harvesting semiconductor to the rGO hole injection interlayer. These synergistic effects greatly prolong the lifetime of the photo-induced charge carriers. The optimized tandem heterojunction with a 2 wt% rGO loading demonstrate enhanced visible-light-driven photocatalytic activity for Rhodamine B (RhB) dye degradation (removal rate: 97.3%) and Cr(VI) reduction (removal rate: 97.09%). This work reveals a new strategy for the rational design and assembly of hollow-structured photocatalytic materials with spatially separated reduction and oxidation surfaces to achieve excellent photocatalytic performance.

Key words: SnS₂/rGO/TiO₂, Hollow sphere, Photocatalyst, Hole injection layer, Cr(VI) reduction

Chao Xue, Hua An, Guosheng Shao, Guidong Yang. Accelerating directional charge separation via built-in interfacial electric fields originating from work-function differences[J]. Chinese Journal of Catalysis, 2021, 42(4): 583-594.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(20)63649-X

https://www.cjcatal.com/EN/Y2021/V42/I4/583

Figures/Tables 8

Scheme 1. Schematic illustration of the synthetic procedure of the hierarchical porous SnS2/rGO/TiO2 hollow spheres.

Fig. 1. SEM (a), TEM (b), and HRTEM (c) images of TiO2 hollow spheres; SEM (d), TEM (e), and HRTEM (f) images (inset of (e) is the corresponding SAED pattern) of GO/TiO2 composite (TG-4; 2 wt% GO loading).

Fig. 2. SnS2/rGO/TiO2 composite with 2 wt% GO loading (TGS-4 composite): (a,d) SEM and (b,c) TEM images. EDS elemental mapping images of a selected area: (e) Ti, (f) O, (g) C, (h) Sn, and (i) S. (j) Corresponding SAED pattern and (k) HRTEM image.

Fig. 3. XRD patterns (a) and Raman spectra (b) of the as-prepared samples obtained using an excitation wavelength of 633 nm; XPS survey spectrum (c) and high-resolution XPS spectra of the C 1s (d), O 1s (e), Ti 2p (f), S 2p (g), and Sn 3d (h) core levels of the different samples.

Fig. 4. Plots of RhB degradation (a) and Cr(VI) reduction (c); Cycling experiment results for the degradation of RhB (b) and reduction of Cr(VI) (d) over the TGS-4 composite; Plots of RhB degradation (e) and Cr(VI) reduction (f) over the TGS-4 composite in the presence of different scavengers. (CRhB = 20 mg L-1; CK2Cr2O7 = 100 mg·L-1).

Fig. 5. N2 adsorption-desorption isotherms of TiO2 (a) and the TGS-4 composite (b); (c) UV-vis DRS spectra; (d) PL spectra excited at 325 nm; Transient photocurrent responses (e) and Nyquist plots (f) for the as-synthesized samples. The insets in (a) and (b) are the corresponding pore-size distribution curves.

Fig. 6. (a-d) UPS spectra of the different samples; Mott-Schottky plots of TiO2 (e) and SnS2 (f) in 2 moL L-1 Na2SO4 electrolytes.

Fig. 7. Schematic of the energy level alignment and corresponding charge transfer process in the TS-2 (a) and TGS-4 (b) composites during the photoredox reactions.

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