S型CeO2/Bi2MoO6微球异质结的理性设计及其高效光催化CO2还原

doi:10.3866/PKU.WHXB202309031

物理化学学报 >> 2024, Vol. 40 >> Issue (10): 2309031.doi: 10.3866/PKU.WHXB202309031

所属专题：太阳燃料光催化剂

S型CeO₂/Bi₂MoO₆微球异质结的理性设计及其高效光催化CO₂还原

许修涛†, 邵春风†, 张金锋*(), 王中辽*(), 代凯*()

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

收稿日期:2023-09-18 修回日期:2023-10-26 录用日期:2023-10-26 发布日期:2024-03-13
通讯作者: Email: daikai940@chnu.edu.cn (代凯)wangzl@chnu.edu.cn (王中辽)jfzhang@chnu.edu.cn; Fax: +86-561-3803256 (张金锋)
作者简介:
^†These authors contributed equally to this work.
基金资助:
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)

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

Xiutao Xu, Chunfeng Shao, Jinfeng Zhang*(), Zhongliao Wang*(), Kai Dai*()

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

Received:2023-09-18 Revised:2023-10-26 Accepted:2023-10-26 Published:2024-03-13
Contact: Email: daikai940@chnu.edu.cn (Kai Dai)wangzl@chnu.edu.cn (Zhongliao Wang)jfzhang@chnu.edu.cn; Fax: +86-561-3803256 (Jinfeng Zhang)
Supported by:
the National Natural Science Foundation of China(22278169); the National Natural Science Foundation of China(51973078); the Excellent Scientific Research and Innovation Team of Education Department of Anhui Province(2022AH010028); the Major Projects of Education Department of Anhui Province(2022AH040068); the Key Foundation of Educational Commission of Anhui Province(2022AH050396); the Key Foundation of Educational Commission of Anhui Province(2022AH050376); Anhui Provincial Quality Engineering Project(2022sx134)

摘要/Abstract

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: 光催化CO₂转化, CeO₂, Bi₂MoO₆, S型异质结, 电荷转移

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: Photocatalytic CO₂ conversion, CeO₂, Bi₂MoO₆, S-scheme heterojunction, Charge transfer

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), 2309031. doi: 10.3866/PKU.WHXB202309031

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 Phys. -Chim. Sin. 2024, 40(10), 2309031. doi: 10.3866/PKU.WHXB202309031

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB202309031

https://www.whxb.pku.edu.cn/CN/Y2024/V40/I10/2309031

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Sample	Life time (ns)	Pre-exponential factors (%)	<τ> (ns)
CeO₂/Bi₂MoO₆	τ₁ = 7.331	A₁ = 18.23	7.33
CeO₂/Bi₂MoO₆	τ₂ = 0.031	A₂ = 81.77	7.33
CeO₂	τ₁ = 9.025	A₁ = 28.03	9.02
CeO₂	τ₂ = 0.029	A₂ = 71.97	9.02
Bi₂MoO₆	τ₁ = 8.708	A₁ = 56.22	8.71
Bi₂MoO₆	τ₂ = 0.018	A₂ = 43.78	8.71

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S型CeO₂/Bi₂MoO₆微球异质结的理性设计及其高效光催化CO₂还原

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

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