构建共价三嗪框架/氮掺杂碳包覆氧化亚铜S型异质结促进光催化析氢

引用本文: 黄凯辉, 陈德俊, 张欣, 沈荣晨, 张鹏, 许第发, 李鑫. 构建共价三嗪框架/氮掺杂碳包覆氧化亚铜S型异质结促进光催化析氢[J]. 物理化学学报, 2024, 40(12): 240702. doi: 10.3866/PKU.WHXB202407020 shu

Citation: Kaihui Huang, Dejun Chen, Xin Zhang, Rongchen Shen, Peng Zhang, Difa Xu, Xin Li. Constructing Covalent Triazine Frameworks/N-Doped Carbon-Coated Cu₂O S-Scheme Heterojunctions for Boosting Photocatalytic Hydrogen Production[J]. Acta Physico-Chimica Sinica, 2024, 40(12): 240702. doi: 10.3866/PKU.WHXB202407020 shu

构建共价三嗪框架/氮掺杂碳包覆氧化亚铜S型异质结促进光催化析氢

黄凯辉 ^{1, 2, †,} ,
陈德俊 ^{2, †,} ,
张欣 ^{3,
,} ,
沈荣晨 ^{1, 2,
,} ,
张鹏 ^{4,
,} ,
许第发 ^5, ,
李鑫 ^{1, 2,
,}

1.
华南农业大学, 生物质工程研究院, 农业农村部能源植物资源与利用重点实验室, 广州 510642
2.
华南农业大学, 材料与能源学院, 生物基材料与能源教育部重点实验室, 广州 510642
3.
湖北文理学院, 低维光电材料与器件湖北省重点实验室, 湖北襄阳 441053
4.
郑州大学, 材料科学与工程学院, 低碳环保材料国际合作中心(CDLCEM), 郑州 450001
5.
长沙学院, 应用环境光催化湖南省重点实验室, 长沙 410022

通讯作者: 张欣, xinzhang@hbuas.edu.cn; 沈荣晨, shenrongchenscau@163.com; 张鹏, zhangp@zzu.edu.cn; 李鑫, xinli@scau.edu.cn

基金项目:
国家自然科学基金 22378148

国家自然科学基金 21975084

国家自然科学基金 2230082074

广东省自然科学基金 2024A1515012433
^†These authors contributed equally to this work.

摘要: 开发用于制氢的高效光催化剂在可持续能源研究中至关重要。本研究设计并制备了一种具有S型异质结结构的共价三嗪框架(CTF)-Cu₂O@NC复合材料，旨在提高光催化析氢的效率。由于氮掺杂碳(NC)层和S型异质结的协同效应，复合物的光吸收能力、电子-空穴分离效率和产氢活性显著增强。该系统的结构和光电化学表征表明，S型异质结不仅提高了光生载流子的分离效率，而且还保持了很强的氧化还原能力，从而进一步促进了光催化反应。此外，NC层可以同时减少Cu₂O的光腐蚀并促进电子转移。实验结果表明，CTF-7% Cu₂O@NC复合材料在可见光照射下表现出优异的制氢性能，达到15645 μmol∙g⁻¹∙h⁻¹，大大超过了纯CTF的光催化活性(2673 μmol∙g⁻¹∙h⁻¹)。这项研究为开发高效、创新的光催化材料提供了一种新方法，有力地支持了可持续氢能源的发展。

关键词:

English

Constructing Covalent Triazine Frameworks/N-Doped Carbon-Coated Cu₂O S-Scheme Heterojunctions for Boosting Photocatalytic Hydrogen Production

Kaihui Huang ^{1, 2, †,} ,
Dejun Chen ^{2, †,} ,
Xin Zhang ^{3,
,} ,
Rongchen Shen ^{1, 2,
,} ,
Peng Zhang ^{4,
,} ,
Difa Xu ^5, ,
Xin Li ^{1, 2,
,}

1.
Institute of Biomass Engineering, Key Laboratory of Energy Plants Resource and Utilization, Ministry of Agriculture and Rural Affairs, South China Agricultural University, Guangzhou 510642, China
2.
Key Laboratory for Biobased Materials and Energy of Ministry of Education, College of Materials and Energy, South China Agricultural University, Guangzhou 510642, China
3.
Hubei Key Lab Low Dimens Optoelect Mat ₂ Devices, Hubei University of Arts and Science, Xiangyang 441053, Hubei Province, China
4.
State Centre for International Cooperation on Designer Low-Carbon ₂ Environmental Materials (CDLCEM), School of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450001, China
5.
Hunan Key Laboratory of Applied Environmental Photocatalysis, Changsha University, Changsha 410022, China

Corresponding author: Email: xinzhang@hbuas.edu.cn (X.Z.); Email: shenrongchenscau@163.com (R.S.); Email: zhangp@zzu.edu.cn (P.Z.); Email: xinli@scau.edu.cn (X.L.)

Received Date: 21 July 2024
Accepted Date: 19 September 2024
Revised Date: 18 September 2024
Available Online: 15 December 2024
Fund Project:
The project was supported from the National Natural Science Foundation of China

The project was supported from the National Natural Science Foundation of China

The project was supported from the National Natural Science Foundation of China

Natural Science Foundation of Guangdong Province

Abstract: The development of efficient photocatalysts for hydrogen production is crucial in sustainable energy research. In this study, we designed and prepared a Covalent Triazine Framework (CTF)-Cu₂O@NC composite featuring an S-scheme heterojunction structure aimed at enhancing the photocatalytic hydrogen production. The light absorption capacity, electron-hole separation efficiency and H₂-evolution activity of the composite were significantly enhanced due to the synergistic effects of the nitrogen-doped carbon (NC) layer and the S-scheme heterojunction. Structural and photoelectrochemical characterization of the system reveal that the S-scheme heterojunctions not only enhance the separation efficiency of photogenerated carriers but also maintain the strong redox capabilities to further promote the photocatalytic reactions. Moreover, the NC layer could simultaneously reduce the photocorrosion of Cu₂O and promote the electron transfer. Experimental results demonstrate that the CTF-7% Cu₂O@NC composite shows outstanding hydrogen-production performance under visible light, achieving 15645 μmol∙g⁻¹∙h⁻¹, significantly surpassing the photocatalytic activity of pure CTF (2673 μmol∙g⁻¹∙h⁻¹). This study introduces a novel approach to the development of efficient and innovative photocatalytic materials, strongly supporting the advancement of sustainable hydrogen energy.

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

构建共价三嗪框架/氮掺杂碳包覆氧化亚铜S型异质结促进光催化析氢

通讯作者: 张欣, xinzhang@hbuas.edu.cn; 沈荣晨, shenrongchenscau@163.com; 张鹏, zhangp@zzu.edu.cn; 李鑫, xinli@scau.edu.cn

English

Constructing Covalent Triazine Frameworks/N-Doped Carbon-Coated Cu₂O S-Scheme Heterojunctions for Boosting Photocatalytic Hydrogen Production

Corresponding author: Email: xinzhang@hbuas.edu.cn (X.Z.); Email: shenrongchenscau@163.com (R.S.); Email: zhangp@zzu.edu.cn (P.Z.); Email: xinli@scau.edu.cn (X.L.)

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CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

构建共价三嗪框架/氮掺杂碳包覆氧化亚铜S型异质结促进光催化析氢

通讯作者: 张欣, xinzhang@hbuas.edu.cn; 沈荣晨, shenrongchenscau@163.com; 张鹏, zhangp@zzu.edu.cn; 李鑫, xinli@scau.edu.cn

English

Constructing Covalent Triazine Frameworks/N-Doped Carbon-Coated Cu2O S-Scheme Heterojunctions for Boosting Photocatalytic Hydrogen Production

Corresponding author: Email: xinzhang@hbuas.edu.cn (X.Z.); Email: shenrongchenscau@163.com (R.S.); Email: zhangp@zzu.edu.cn (P.Z.); Email: xinli@scau.edu.cn (X.L.)

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

Constructing Covalent Triazine Frameworks/N-Doped Carbon-Coated Cu₂O S-Scheme Heterojunctions for Boosting Photocatalytic Hydrogen Production

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs