木质素基碳量子点与氧空位协同调控的S型LCQDs/Bi2WO6异质结用于光催化H2O2生产

引用本文: 王其申, 陈昌兆, 李孟卿, 吴玲敏, 代凯. 木质素基碳量子点与氧空位协同调控的S型LCQDs/Bi₂WO₆异质结用于光催化H₂O₂生产[J]. 物理化学学报, 2025, 41(11): 100147. doi: 10.1016/j.actphy.2025.100147 shu

Citation: Qishen Wang, Changzhao Chen, Mengqing Li, Lingmin Wu, Kai Dai. Lignin derived carbon quantum dots and oxygen vacancies coregulated S-scheme LCQDs/Bi₂WO₆ heterojunction for photocatalytic H₂O₂ production[J]. Acta Physico-Chimica Sinica, 2025, 41(11): 100147. doi: 10.1016/j.actphy.2025.100147 shu

木质素基碳量子点与氧空位协同调控的S型LCQDs/Bi₂WO₆异质结用于光催化H₂O₂生产

王其申 ^1, ,
陈昌兆 ^{1,
,} ,
李孟卿 ^1, ,
吴玲敏 ^{2,
,} ,
代凯 ^{3,
,}

1.
安徽理工大学力学与光电物理学院, 安徽淮南 232001
2.
华南理工大学化学与化工学院燃料电池技术广东省重点实验室, 广东广州 510640
3.
淮北师范大学污染物敏感材料与环境修复安徽省重点实验室, 绿色和精准合成化学及应用教育部重点实验室, 安徽淮北 235000

通讯作者: 陈昌兆, chzhchen@aust.edu.cn; 吴玲敏, 202110184982@mail.scut.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 12304134

安徽省教育厅优秀科研创新团队 2022AH010028

安徽省自然科学基金 2108085ME148

摘要: 光催化制备H₂O₂与高值木质素技术创新了绿色化学合成和废弃生物质转化的相关途径。本研究通过水热法合成了木质素基碳量子点(LCQDs)，并构建了S型异质结光催化剂LCQDs/Bi₂WO₆以高效生产H₂O₂，其在模拟可见光下展现出优异的H₂O₂产率(3.776 mmol·h⁻¹·g⁻¹)，较BWO−A样品提升5.97倍，在五轮循环后仍可保持89.72%的性能。这一突破源于LCQDs与氧空位缺陷的协同调控：LCQDs独特的上转换发光特性结合S型电荷转移路径，有效增强了光吸收能力和载流子分离效率，而氧空位作为电子陷阱则延长了载流子寿命。结合原位电子顺磁共振分析和能带结构表征，我们证实了反应途中•O₂⁻和•OH自由基的大量存在，复合材料主要通过连续单电子反应优化H₂O₂合成路径，经过导带与价带位置的同步调整，增强了氧还原反应(ORR)与水氧化反应(WOR)能力。鉴于木质素的主要来源为农林废弃物，该研究不仅为高性能光催化体系的设计提供了新策略，还显著推动了废弃生物质资源的高值化利用。

关键词:

English

Lignin derived carbon quantum dots and oxygen vacancies coregulated S-scheme LCQDs/Bi₂WO₆ heterojunction for photocatalytic H₂O₂ production

Qishen Wang ^1, ,
Changzhao Chen ^{1,
,} ,
Mengqing Li ^1, ,
Lingmin Wu ^{2,
,} ,
Kai Dai ^{3,
,}

1.
School of Mechanics and Photoelectric Physics, Anhui University of Science and Technology, Huainan 232001, Anhui Province, China
2.
Guangdong Provincial Key Laboratory of Fuel Cell Technology School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510640, Guangdong Province, China
3.
Key Laboratory of Green and Precise Synthetic Chemistry and Applications, Ministry of Education, Anhui Province Key Laboratory of Pollutant Sensitive Materials and Environmental Remediation, Huaibei Normal University, Huaibei 235000, Anhui Province, China

Corresponding author: Email: chzhchen@aust.edu.cn (C. Chen); Email: 202110184982@mail.scut.edu.cn (L. Wu); Email: daikai940@chnu.edu.cn (K. Dai)

Received Date: 06 July 2025
Accepted Date: 03 August 2025
Revised Date: 30 July 2025
Available Online: 15 November 2025
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 Natural Science Foundation of Anhui Province

Abstract: This study presents an innovative photocatalytic system utilizing waste biomass resources for sustainable synthesis of hydrogen peroxide (H₂O₂) and high-value lignin derivatives. A lignin derived carbon quantum dots (LCQDs) loaded S-scheme heterojunction photocatalyst LCQDs/Bi₂WO₆ (LCD/BWO) was synthesized via hydrothermal method. The LCD/BWO composite demonstrates exceptional H₂O₂ production rate (3.776 mmol·h⁻¹·g⁻¹) and maintains 89.72% activity retention after 5 cycles under visible light irradiation, representing a 5.97-fold enhancement over catalyst BWO−A. The performance leap stems from synergistic effects between LCQDs and oxygen vacancies (OVs) defects: the unique up-conversion luminescence of LCQDs combined with S-scheme charge transfer mechanism enhances light absorption and carrier separation efficiency, while interfacial OVs act as electron traps to prolong carrier lifetime. In situ electron paramagnetic resonance (In situ EPR) analysis revealed substantial generation of •O₂⁻ and •OH radicals on catalyst surfaces. Band structure characterization confirms optimized H₂O₂ synthesis through consecutive single-electron reactions. Synergistic regulation of band positions significantly enhances oxygen reduction reaction (ORR) and water oxidation reaction (WOR) capabilities. As lignin primarily originates from agricultural/forestry waste, this work not only provides new design strategies for efficient photocatalytic systems but also advances high−value utilization of waste biomass resources.

Key words:

Lignin-derived carbon quantum dots (LCQDs)
/ Oxygen vacancies (OVs)
/ S-scheme heterojunction
/ In situ EPR
/ H₂O₂ production

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通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

木质素基碳量子点与氧空位协同调控的S型LCQDs/Bi₂WO₆异质结用于光催化H₂O₂生产

通讯作者: 陈昌兆, chzhchen@aust.edu.cn; 吴玲敏, 202110184982@mail.scut.edu.cn; 代凯, daikai940@chnu.edu.cn

English

Lignin derived carbon quantum dots and oxygen vacancies coregulated S-scheme LCQDs/Bi₂WO₆ heterojunction for photocatalytic H₂O₂ production

Corresponding author: Email: chzhchen@aust.edu.cn (C. Chen); Email: 202110184982@mail.scut.edu.cn (L. Wu); Email: daikai940@chnu.edu.cn (K. Dai)

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