S-Scheme 2D/2D Bi2MoO6/BiOI van der Waals heterojunction for CO2 photoreduction

doi:10.1016/S1872-2067(21)64010-X

Abstract

Abstract:

Reducing CO₂ to hydrocarbon fuels by solar irradiation provides a feasible channel for mitigating excessive CO₂ emissions and addressing resource depletion. Nevertheless, severe charge recombination and the high energy barrier for CO₂ photoreduction on the surface of photocatalysts compromise the catalytic performance. Herein, a 2D/2D Bi₂MoO₆/BiOI composite was fabricated to achieve improved CO₂ photoreduction efficiency. Charge transfer in the composite was facilitated by the van der Waals heterojunction with a large-area interface. Work function calculation demonstrated that S-scheme charge transfer is operative in the composite, and effective charge separation and strong redox capability were revealed by time-resolved photoluminescence and electron paramagnetic resonance spectroscopy. Moreover, the intermediates of CO₂ photoreduction were identified based on the in situ diffuse reflectance infrared Fourier-transform spectra. Density functional theory calculations showed that CO₂ hydrogenation is the rate-determining step for yielding CH₄ and CO. Introducing Bi₂MoO₆ into the composite further decreased the energy barrier for CO₂ photoreduction on BiOI by 0.35 eV. This study verifies the synergistic effect of the S-scheme heterojunction and van der Waals heterojunction in the 2D/2D composite.

Key words: 2D/2D, S-scheme heterojunction, van der Waals heterojunction, CO₂ photoreduction

Zhongliao Wang, Bei Cheng, Liuyang Zhang, Jiaguo Yu, Youji Li, S. Wageh, Ahmed A. Al-Ghamdi. S-Scheme 2D/2D Bi₂MoO₆/BiOI van der Waals heterojunction for CO₂ photoreduction[J]. Chinese Journal of Catalysis, 2022, 43(7): 1657-1666.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)64010-X

https://www.cjcatal.com/EN/Y2022/V43/I7/1657

Figures/Tables 9

Fig. 1. XRD curves (a), FT-IR curves (b), UV-vis DRS and Tauc spectra (inset) (c), and N2 adsorption-desorption isotherms (inset shows pore-size distribution plots) (d) of Bi2MoO6, BiOI, and Bi2MoO6/BiOI composite.

Fig. 2. TEM images of Bi2MoO6 NSs (a,b), BiOI NSs (c,d), and Bi2MoO6/BiOI composite (e,f). HRTEM image (g), HAADF-STEM scan areas and corresponding elemental distributions (h) of Bi2MoO6/BiOI composite.

Fig. 3. (a) Survey spectra; high-resolution XPS spectra of Bi 4f (b), Mo 3d (c), O 1s (d), and I 3d (e) orbitals of various samples.

Fig. 4. Work function profiles of Bi2MoO6 (a) and BiOI (b). (c) Charge density difference of Bi2MoO6/BiOI composite with an isosurface of 3 × 10-4 e/Å3.

Fig. 5. Photocurrent response signals (a), Nyquist spectra (b), steady-state (c), and time-resolved PL spectra (d) of Bi2MoO6, BiOI, and Bi2MoO6/BiOI.

Table 1 Data from time-resolved PL decay curves fitted by the multi-exponential Eq. (1).

Sample	Decay time (ns)			Relative intensity			Average lifetime (ns)
Sample	τ₁	τ₂	τ₃	A₁	A₂	A₃	Average lifetime (ns)
Bi₂MoO₆	1.40	7.15	—	10171	1383	—	3.76
BiOI	1.34	6.76	—	10496	1413	—	3.53
Bi₂MoO₆/BiOI	0.99	6.63	2.31	9910	1023	1596	3.12

Fig. 6. Mott-Schottky curves (a), band configuration (b) of Bi2MoO6 and BiOI; EPR signals of DMPO-•O2- (c), DMPO-•OH (d) for Bi2MoO6, BiOI, and Bi2MoO6/BiOI.

Fig. 7. CO2 adsorption curves (a) and CO2 photoreduction activity (b) of Bi2MoO6, BiOI, and Bi2MoO6/BiOI composite under full-spectrum irradiation. CO2 photoreduction stability (c) and in situ DRIFTS profiles (d) of Bi2MoO6/BiOI composite. (e) Diagram showing evolution of CH4 and CO.

Fig. 8. (a) Band configuration of Bi2MoO6 and BiOI. (b) Establishment of IEF of Bi2MoO6/BiOI interface. (c) Photoexcited charge transfer of Bi2MoO6/BiOI heterojunction. (d,e) Free energy variation for CO2 reduction over BiOI and Bi2MoO6/BiOI.

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S-Scheme 2D/2D Bi₂MoO₆/BiOI van der Waals heterojunction for CO₂ photoreduction

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