物理化学学报 >> 2024, Vol. 40 >> Issue (11): 2407002.doi: 10.3866/PKU.WHXB202407002

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具有0D/2D界面的InOOH/ZnIn2S4空心球S型异质结用于增强光催化CO2转化性能

蔡佳星1,†, 徐文迪3,†, 迟浩强4, 刘倩1, 高娃1,*(), 史丽3,*(), 刘敬祥1,5,*(), 邹志刚4, 周勇2,4,*()   

  1. 1 天津工业大学物理科学与技术学院, 天津 300387
    2 安徽工业大学化学与环境工程学院, 安徽 芜湖 241000
    3 南京邮电大学有机电子与信息显示国家重点实验室, 先进材料研究所(IAM), 南京 210023
    4 南京大学物理学院, 江苏省纳米技术重点实验室, 生态材料与可再生能源研究中心, 固态微结构国家实验室, 先进微结构协同创新中心, 南京 210093
    5 Multidisciplinary Platform of Advanced Engineering, Chemical Engineering Discipline, School of Engineering, Monash University Malaysia, Bandar Sunway 47500, Selangor, Malaysia
  • 收稿日期:2024-07-02 修回日期:2024-08-05 录用日期:2024-08-05 发布日期:2024-10-14
  • 通讯作者: Email: gaowa@tiangong.edu.cn (高娃)iamlshi@njupt.edu.cn (史丽)jxlow@tiangong.edu.cn (刘敬祥)zhouyong1999@nju.edu.cn (周勇)
  • 作者简介:

    †These authors contributed equally to this work.

  • 基金资助:
    国家重点研发计划(2022YFE0126500); 国家重点研发计划(2018YFE0208500); 国家自然科学基金委员会项目(21972065); 国家自然科学基金委员会项目(22203046); 国家自然科学基金委员会项目(22202152); 江苏省科学基金会(BK20220006); 合肥微尺度物理科学国家实验室(KF2020006); 广东省创新创业团队引进项目(2019ZL08L101); 中国高校发展基金(UDF01001159); 南京邮电大学有机电子与信息显示国家重点实验室项目(GZR2023010003); 南京邮电大学自然科学研究创业人才招聘基金(NY221128)

Highly Efficient InOOH/ZnIn2S4 Hollow Sphere S-Scheme Heterojunction with 0D/2D Interface for Enhancing Photocatalytic CO2 Conversion

Jiaxing Cai1, Wendi Xu3, Haoqiang Chi4, Qian Liu1, Wa Gao1,*(), Li Shi3,*(), Jingxiang Low1,5,*(), Zhigang Zou4, Yong Zhou2,4,*()   

  1. 1 School of Physical Science and Technology, Tiangong University, Tianjin 300387, China
    2 School of Chemical and Environmental Engineering, Anhui Polytechnic University, Wuhu 241000, Anhui Province, China
    3 State Key Laboratory of Organic Electronics and Information Displays & Institute of Advanced Materials (IAM), Nanjing University of Posts and Telecommunications, Nanjing 210023, China
    4 School of Physics, Jiangsu Key Laboratory of Nanotechnology, Eco-materials and Renewable Energy Research Center (ERERC), National Laboratory of Solid State Microstructures, Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing 210093, China
    5 Multidisciplinary Platform of Advanced Engineering, Chemical Engineering Discipline, School of Engineering, Monash University Malaysia, Bandar Sunway 47500, Selangor, Malaysia
  • Received:2024-07-02 Revised:2024-08-05 Accepted:2024-08-05 Published:2024-10-14
  • Contact: Email: gaowa@tiangong.edu.cn (Wa Gao)iamlshi@njupt.edu.cn (Li Shi)jxlow@tiangong.edu.cn (Jingxiang Low)zhouyong1999@nju.edu.cn (Yong Zhou)
  • Supported by:
    the National Key R & D Program of China(2022YFE0126500); the National Key R & D Program of China(2018YFE0208500); the National Natural Science Foundation of China(21972065); the National Natural Science Foundation of China(22203046); the National Natural Science Foundation of China(22202152); the Natural Science Foundation of Jiangsu Province(BK20220006); the Hefei National Laboratory for Physical Sciences at the Microscale(KF2020006); the Program for Guangdong Introducing Innovative and Entrepreneurial Team(2019ZL08L101); the Chinese University Development Fund(UDF01001159); the Project of State Key Laboratory of Organic Electronics and Information Displays, Nanjing University of Posts and Telecommunications(GZR2023010003); Natural Science Research Start-up Foundation of Recruiting Talents of Nanjing University of Posts and Telecommunications(NY221128)

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摘要：

S型异质结光催化剂因其能够同时促进光生载流子的分离，并优化光催化剂的还原和氧化能力，而被广泛应用于光催化CO2转化中。尽管S型异质结具有巨大的潜力，但其光催化CO2转化性能仍然有限，这主要是由于其界面光生载流子迁移缓慢和光利用效率差。本文报道了一种具有0D/2D接触界面的InOOH/ZnIn2S4空心球S型异质结，以提高光催化CO2转化性能。具体来说，空心球结构可以允许入射光在光催化剂内进行多重反射，以增强光利用效率。此外，0D/2D接触界面可以促进光生载流子在InOOH/ZnIn2S4空心球S型异质结上的迁移速率。结合原位光照X射线光电子能谱表征和自由基捕获实验，确认了InOOH和ZnIn2S4上光生空穴和电子的空间分离，有利于高效利用光生载流子进行光催化CO2转化。因此，优化后的InOOH/ZnIn2S4展示了比原始ZnIn2S4高出25.8倍的光催化CO2转化性能。本工作展示了一种简单而有效的策略，用于提高S型异质结的界面光电荷载流子迁移和光利用效率。

关键词: 光催化CO2转化, S型异质结, ZnIn2S4, 空心球, 接触界面

Abstract:

S-scheme heterojunction system represents a highly efficient strategy for photocatalytic applications as it can simultaneously facilitate photogenerated charge carrier separation and enhance the reduction-oxidation potentials of the photocatalyst. Despite its gigantic potential, the photocatalytic CO2 conversion efficiency of the S-scheme heterojunction remains limited mainly attributed to the sluggish interfacial charge carrier migration and poor light utilization efficiency. Herein, we prepare an InOOH/ZnIn2S4 hollow sphere S-scheme heterojunction with 0D/2D contact interface for enhancing photocatalytic CO2 conversion performance. Specifically, the hollow sphere morphology can cause the multireflection of incident light within the photocatalyst leading to enhanced light absorption of the photocatalyst. In addition, the 0D/2D contact interface can facilitate the photogenerated charge carrier migration transfer over the InOOH/ZnIn2S4 S-scheme heterojunction. Furthermore, combining in situ irradiated X-ray photoelectron spectroscopy (ISI-XPS) characterization and radicals trapping test, it is affirmed the accumulation of photogenerated holes and electrons respectively on InOOH and ZnIn2S4, which is beneficial for the effective utilization of photogenerated charge carriers. As a result, the photocatalytic CO2 conversion performance of the optimized InOOH/ZnIn2S4 is ca. 25.8 times higher than that of pristine ZnIn2S4. Our reported results demonstrate a facile yet effective strategy for enhancing the interfacial photogenerated charge carrier migration and light utilization efficiency of S-scheme heterojunction.

Key words: Photocatalytic CO2 conversion, S-scheme heterojunction, ZnIn2S4, Hollow sphere, Contact interface