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Internal Electric Field Enhances B Refilling and Carbon Vacancy Double Modulation to Promote Photocatalytic Hydrogen Evolution

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Abstract

Defect engineering is an effective mean to improve the photocatalytic evolution of H2, but the increase of activity caused by a single modification method is often limited. Although the carbon vacancy plays a very important role in promoting the hydrogen evolution activity, it is easy to inactivate due to the instability of the vacancy. Precise B refilling induced by surface carbon defects can not only stabilize the carbon vacancy but also adjust the energy band structure of g-C3N4 (CN), so that B refilling carbon vacancies CN (BRf-VC-CN) shows the highest electron reduction ability. The electrochemical results show that BRf-VC-CN represent the strongest ability of carrier separation and transfer, and the large internal electric field also indicates that the enhanced interlayer electron transfer. At the same time, surface heteroatom refilling can also improve the H2O adsorption. As a result, the hydrogen evolution of the sample after B refilling is greatly increased to 18,100 μL g−1 h−1, which is 27.2 times higher than that of CN. This work will provide reliable and clear insights for the controlled defect engineering of photocatalysts, and provide general modification strategies for conventional typical heteroatoms used in H2 production.

Graphical Abstract

A defect-induced heteroatom refilling strategy is used here to synthesize B introduced in carbon nitride by precisely controlling the “introduction” sites on C1 sites. The interaction between vacancy and refilled heteroatoms makes B-refilled samples show high internal electric field strength and greatly improve the photocatalytic activity.

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Acknowledgements

This work was supported by National Key Research and Development Program of China (2022YFB3803600), the National Natural Science Foundation of China (21972040), the Innovation Program of Shanghai Municipal Education Commission (2021-01-07-00-02-E00106), the Science and Technology Commission of Shanghai Municipality (20DZ2250400, 22230780200), and the Program of Introducing Talents of Discipline to Universities (B20031), the National Natural Science Foundation of China (22006038).

Funding

National Natural Science Foundation of China, 21972040, 22006038, Program of Introducing Talents of Discipline to Universities, B20031, Innovation Program of Shanghai Municipal Education Commission, 2021-01-07-00-02-E00106, National Key Research and Development Program of China, 2022YFB3803600, Science and Technology Commission of Shanghai Municipality, 20DZ2250400,22230780200

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Authors and Affiliations

  1. National Engineering Research Center of Industrial Wastewater Detoxication and Resource Recovery, State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process, School of Resources and Environmental Engineering, East China University of Science & Technology, Shanghai, 200237, People’s Republic of China

    Liang Zhou & Juying Lei

  2. Key Laboratory for Advanced Materials, Shanghai Engineering Research Center for Multimedia Environmental Catalysis and Resource Utilization, Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, School of Chemistry and Molecular Engineering, East China University of Science & Technology, Shanghai, 200237, People’s Republic of China

    Yujie Liu, Yifan Zheng, Muhammad Tayyab, Summan Aman & Jinlong Zhang

  3. Shanghai Institute of Pollution Control and Ecological Security, Tongji University, Shanghai, 200092, People’s Republic of China

    Liang Zhou & Juying Lei

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  1. Yujie Liu
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Correspondence to Jinlong Zhang.

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Liu, Y., Zheng, Y., Tayyab, M. et al. Internal Electric Field Enhances B Refilling and Carbon Vacancy Double Modulation to Promote Photocatalytic Hydrogen Evolution. Catal Lett 154, 798–807 (2024). https://doi.org/10.1007/s10562-023-04346-7

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