Citation: Xiutao Xu, Chunfeng Shao, Jinfeng Zhang, Zhongliao Wang, Kai Dai. Rational Design of S-Scheme CeO₂/Bi₂MoO₆ Microsphere Heterojunction for Efficient Photocatalytic CO₂ Reduction[J]. Acta Physico-Chimica Sinica, ;2024, 40(10): 230903. doi: 10.3866/PKU.WHXB202309031 shu

Rational Design of S-Scheme CeO₂/Bi₂MoO₆ Microsphere Heterojunction for Efficient Photocatalytic CO₂ Reduction

Laboratory of Green and Precise Synthetic Chemistry and Applications, Ministry of Education, Anhui Province Key Laboratory of Pollutant Sensitive Materials and Environmental Remediation, Anhui Province Key Laboratory of Intelligent Computing and Applications, Anhui Province Industrial Generic Technology Research Center for Alumics Materials, Huaibei Normal University, Huaibei 235000, Anhui Province, China

Corresponding author: Jinfeng Zhang, jfzhang@chnu.edu.cn Zhongliao Wang, wangzl@chnu.edu.cn Kai Dai, daikai940@chnu.edu.cn

^†

Received Date: 18 September 2023
Revised Date: 26 October 2023
Accepted Date: 26 October 2023
Available Online: 20 December 2023
Fund Project: the National Natural Science Foundation of China 22278169the National Natural Science Foundation of China 51973078the Excellent Scientific Research and Innovation Team of Education Department of Anhui Province 2022AH010028the Major Projects of Education Department of Anhui Province 2022AH040068the Key Foundation of Educational Commission of Anhui Province 2022AH050396the Key Foundation of Educational Commission of Anhui Province 2022AH050376Anhui Provincial Quality Engineering Project 2022sx134

In the pursuit of efficient photocatalytic carbon dioxide (CO₂) conversion, the use of artificial semiconductors powered by solar energy offers great potential for simulating natural carbon cycling. However, the efficiency of photocatalytic CO₂ conversion remains suboptimal, primarily due to inadequate separation of photogenerated charges, which hinders the performance of semiconductor-based CO₂ reduction. Consequently, recent research efforts have focused on identifying ideal materials for CO₂ photocatalytic conversion. Among the candidate materials, the structure of Bi₂MoO₆ consists of alternating layers of (Bi₂O₂)²⁺ and perovskite-like (MoO₄)²⁻ layers with shared oxygen atoms between them. This inherent charge distribution within Bi₂MoO₆ creates an inhomogeneous electric field, facilitating the efficient separation of photogenerated charge carriers. The morphology and structure of a catalyst significantly influence the rate of recombination of photogenerated charge carriers. Research has shown that ultrathin Bi₂MoO₆ nanosheets, compared to other 2D and 3D structures of Bi₂MoO₆ materials, possess longer fluorescence lifetimes, providing more opportunities for the separation of photogenerated charge carriers. However, Bi₂MoO₆ still exhibits relatively low catalytic efficiency due to its insufficiently negative conduction band position (ranging between −0.2 and −0.4 V). To address this limitation, a viable strategy is to load a semiconductor with a more negatively positioned conduction band onto Bi₂MoO₆, creating an S-scheme heterojunction. In this study, Bi₂MoO₆ nanosheets were synthesized through a hydrothermal method, and simultaneously, CeO₂ nanoparticles were grown on their surfaces, forming an S-scheme heterojunction modified with Ce³⁺/Ce⁴⁺ ion bridges. Time-resolved photoluminescence (TRPL) and photoelectrochemical tests demonstrated the enhanced charge separation effect of this heterojunction. In situ X-ray photoelectron spectroscopy (In situ XPS) analysis and theoretical calculations further confirmed that photogenerated electrons follow an S-scheme mechanism, transferring from Bi₂MoO₆ to CeO₂. Experimental results revealed that the photocatalytic CO₂ reduction efficiencies of CeO₂/Bi₂MoO₆, Bi₂MoO₆, and CeO₂ were 65.3, 14.8, and 1.2 μmol∙g⁻¹∙h⁻¹, respectively. Compared to pure Bi₂MoO₆, the catalytic efficiency of the CeO₂/Bi₂MoO₆ composite catalyst for CO₂ photocatalytic reduction to CO improved by a factor of 3.12. This enhancement in photocatalytic CO₂ conversion performance can be attributed to the synergistic interaction between the S-scheme heterojunction and Ce³⁺/Ce⁴⁺ ion bridging, resulting in enhanced light absorption, efficient charge separation, and redox capabilities of the composite catalyst. This study offers valuable insights into the rational design and construction of novel S-scheme heterojunction photocatalysts.
- Photocatalytic CO₂ conversion,
- CeO₂,
- Bi₂MoO₆,
- S-scheme heterojunction,
- Charge transfer
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通讯作者: 陈斌, bchen63@163.com

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沈阳化工大学材料科学与工程学院沈阳 110142

Rational Design of S-Scheme CeO2/Bi2MoO6 Microsphere Heterojunction for Efficient Photocatalytic CO2 Reduction

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通讯作者: 陈斌, bchen63@163.com

Rational Design of S-Scheme CeO₂/Bi₂MoO₆ Microsphere Heterojunction for Efficient Photocatalytic CO₂ Reduction