Photocatalytic syngas synthesis from CO2 and H2O using ultrafine CeO2-decorated layered double hydroxide nanosheets under visible-light up to 600 nm

doi:10.1007/s11705-020-1947-4

Front. Chem. Sci. Eng.

2021, Vol. 15

Issue (1) : 99-108 https://doi.org/10.1007/s11705-020-1947-4

RESEARCH ARTICLE

Photocatalytic syngas synthesis from CO₂ and H₂O using ultrafine CeO₂-decorated layered double hydroxide nanosheets under visible-light up to 600 nm

Ling Tan, Kipkorir Peter, Jing Ren, Baoyang Du, Xiaojie Hao, Yufei Zhao(

), Yu-Fei Song(

)

State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China

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Abstract

The rational design of photocatalyst that can effectively reduce CO₂ under visible light (l>400 nm), and simultaneously precise control of the products syngas (CO/H₂) ratio is highly desirable for the Fischer-Tropsch reaction. In this work, we synthesized a series of CeO₂-decorated layered double hydroxides (LDHs, Ce-x) samples for photocatalytic CO₂ reduction. It was found that the selectivity and productivity of CO and H₂ from photoreduction of CO₂ in conjunction with Ru-complex as photosensitizer performed an obvious “volcano-like” trend, with the highest point at Ce-0.15 and the CO/H₂ ratio can be widely tunable from 1/7.7 to 1/1.3. Furthermore, compared with LDH, Ce-0.15 also drove photocatalytic CO₂ to syngas under 600 nm irradiation. It implied that an optimum amount of CeO₂ modifying LDH promoted the photoreduction of CO₂ to syngas. This report gives the way to fully utilize the rare earth elements and provides a promising route to enhance the photo-response ability and charge injection efficiency of LDH-based photocatalysts in the synthesis of syngas with a tunable ratio under visible light irradiation.

Keywords visible light catalysis CO₂ conversion layered double hydroxide rare earth elements

Corresponding Author(s): Yufei Zhao,Yu-Fei Song

Just Accepted Date: 04 June 2020 Online First Date: 30 July 2020 Issue Date: 12 January 2021

Cite this article:

Ling Tan,Kipkorir Peter,Jing Ren, et al. Photocatalytic syngas synthesis from CO₂ and H₂O using ultrafine CeO₂-decorated layered double hydroxide nanosheets under visible-light up to 600 nm[J]. Front. Chem. Sci. Eng., 2021, 15(1): 99-108.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-020-1947-4
https://academic.hep.com.cn/fcse/EN/Y2021/V15/I1/99

Fig.1 Scheme 1 Scheme of the tunable selectivity of syngas from photocatalytic CO₂ reduction by LDH, Ce-x (x = 0.05, 0.10, 0.15, 0.20, 0.30 and 0.40) and CeO₂ in conjunction with Ru-complex photosensitizer.

Fig.2 (a) XRD patterns and (b) FTIR spectra of LDH and Ce-x (x = 0.05, 0.10, 0.15, 0.20, 0.30 and 0.40), respectively; (c) BET of the as-synthesized LDH, Ce-x (x = 0.15, 0.20 and 0.40) and (d) the corresponding pore size distribution.

Fig.3 TEM images of (a) LDH, (b) Ce-0.05, (c) Ce-0.15, and the corresponding particle size distribution of CeO₂ (the insert picture of Fig. 2(c)), (d) HRTEM image of Ce-0.15; TEM images of (e) Ce-0.20 and (f) Ce-0.40.

Fig.4 The (a) selectivity, (b) productivity of LDH and Ce-x (x = 0.05, 0.10, 0.15, 0.20, 0.30 and 0.40, respectively) and CeO₂ in CO₂PR under visible light irradiation; (c) isotope trace analysis GC-MS spectra using Ce-0.15 photocatalysts; (d) the selectivity of catalyst under control experimental reaction conditions (1. Ar atmosphere; 2. Without Ce-0.15; 3. Without Ru(bpy)₃Cl₂; 4. In dark); (e) selectivity and (f) productivity of recycle Ce-0.15.

Fig.5 The UV-vis spectra of (a) LDH, Ce-x and CeO₂, (b) the photosensitizer Ru(bpy)₃Cl₂·6H₂O as our previous report [³⁹] and the selectivity of (c) LDH and (d) Ce-0.15 in CO₂PR under different cut-off filter light irradiation.

Fig.6 (a) PL spectra of as-synthesized catalyst in a solution containing 4 × 10^?⁶ mol Ru(bpy)₃Cl₂·6H₂O; (b) EIS spectra of the as-synthesized LDH and Ce-x.

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