S型CeO2/Bi2MoO6微球异质结的理性设计及其高效光催化CO2还原

引用本文: 许修涛, 邵春风, 张金锋, 王中辽, 代凯. S型CeO₂/Bi₂MoO₆微球异质结的理性设计及其高效光催化CO₂还原[J]. 物理化学学报, 2024, 40(10): 230903. doi: 10.3866/PKU.WHXB202309031 shu

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

S型CeO₂/Bi₂MoO₆微球异质结的理性设计及其高效光催化CO₂还原

淮北师范大学, 绿色和精准合成化学及应用教育部重点实验室、污染物敏感材料与环境修复安徽省重点实验室、智能计算及应用安徽省重点实验室和安徽省陶铝新材料产业共性技术研究中心, 安徽淮北 235000

通讯作者: 张金锋, jfzhang@chnu.edu.cn; 王中辽, wangzl@chnu.edu.cn; 代凯, daikai940@chnu.edu.cn

基金项目:
国家自然科学基金 22278169

国家自然科学基金 51973078

安徽省高校优秀科研创新团队 2022AH010028

安徽省教育厅重大项目 2022AH040068

安徽省教育厅重点项目 2022AH050396

安徽省教育厅重点项目 2022AH050376

安徽省质量工程项目 2022sx134

摘要: 人工半导体光催化CO₂转化被广泛认为是模拟自然碳循环的最有前途的策略之一。其中，Bi₂MoO₆具有光催化CO₂转化的潜力。然而，由于其光生电荷载体的快速复合，其催化性能仍然不足。因此，改善Bi₂MoO₆的催化效率是一个紧迫的问题。在这项研究中，我们通过水热法合成了Bi₂MoO₆纳米片，并在其表面同时生长了CeO₂纳米颗粒，形成了Ce³⁺/Ce⁴⁺离子桥接修饰的S型异质结。时间分辨光致发光光谱和光电化学测试揭示了这种异质结的增强电荷分离效应。此外，原位X射线光电子能谱分析和理论计算进一步证实，光生电子转移路径遵循S型机制，从氧化型半导体Bi₂MoO₆的导带转移到还原型半导体CeO₂的价带。实验结果表明，CeO₂/Bi₂MoO₆、Bi₂MoO₆和CeO₂的光催化CO₂还原为CO的效率分别为65.3、14.8和1.2 μmol∙g⁻¹∙h⁻¹。与纯Bi₂MoO₆相比，CeO₂/Bi₂MoO₆复合催化剂将CO₂光催化还原为CO的催化效率提高了3.12倍。这项工作为设计和构建新型S型异质结光催化剂提供了独特的见解。

关键词:

English

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: Email: jfzhang@chnu.edu.cn (J.Z.); Fax: +86-561-3803256; Email: wangzl@chnu.edu.cn (Z.W.); Email: daikai940@chnu.edu.cn (K.D.)

Received Date: 18 September 2023
Accepted Date: 26 October 2023
Revised Date: 26 October 2023
Available Online: 15 October 2024
Fund Project:
the National Natural Science Foundation of China

the National Natural Science Foundation of China

the Excellent Scientific Research and Innovation Team of Education Department of Anhui Province

the Major Projects of Education Department of Anhui Province

the Key Foundation of Educational Commission of Anhui Province

the Key Foundation of Educational Commission of Anhui Province

Anhui Provincial Quality Engineering Project
^†These authors contributed equally to this work.

Abstract: 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.

Key words:

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

S型CeO₂/Bi₂MoO₆微球异质结的理性设计及其高效光催化CO₂还原

通讯作者: 张金锋, jfzhang@chnu.edu.cn; 王中辽, wangzl@chnu.edu.cn; 代凯, daikai940@chnu.edu.cn

English

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

Corresponding author: Email: jfzhang@chnu.edu.cn (J.Z.); Fax: +86-561-3803256; Email: wangzl@chnu.edu.cn (Z.W.); Email: daikai940@chnu.edu.cn (K.D.)

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