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Research Article

Constructing Pd–N interactions in Pd/g-C3N4 to improve the charge dynamics for efficient photocatalytic hydrogen evolution

Xudong Xiao1,§Siying Lin1,§Liping Zhang2( )Huiyuan Meng3Jing Zhou4Qi Li1Jianan Liu1Panzhe Qiao5( )Baojiang Jiang1( )Honggang Fu1( )
Key Laboratory of Functional Inorganic Material Chemistry, Ministry of Education of the People’ s Republic of China, School of Chemistry and Materials Science, Heilongjiang University, Harbin 150080, China
Department of Mechanical and Energy Engineering, Southern University of Science and Technology, Shenzhen 518055, China
School of Safety Engineering, Heilongjiang University of Science and Technology, Harbin 150080, China
Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201800, China
Chinese Acad Sci, Shanghai Synchrotron Radiat Facil, Shanghai Adv Res Inst, Shanghai 201204, China

§ Xudong Xiao and Siying Lin contributed equally to this work.

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Graphical Abstract

A strategy to prepare C3N4 decorated with Pd nanoparticles is demonstrated utilizing amidinothiourea as the precursor of C3N4 that interacts strongly with Pd atoms. In the Pd/C3N4 composite material Pd–N bonds were formed, and they can significantly enhance the charge separation and transport efficiency. As a result, Pd/C3N4 showed excellent performance in photocatalytic hydrogen evolution.

Abstract

The formation of chemical bonds between metal ions and their supports is an effective strategy to achieve good catalytic activity. However, both the synthesis of active metal species on a support and control of their coordination environment are still challenging. Here, we show the use of an organic compound to produce tubular carbon nitride (TCN) as a support for Pd nanoparticles (NPs), creating a composite material (NP-Pd-TCN). It was found that Pd ions preferentially bind with the electron-rich N atoms of TCN, leading to strong metal–support interactions that benefit charge transfer from g-C3N4 to Pd. X-ray absorption spectroscopy further revealed that the metal–support interactions resulted in the formation of Pd–N bonds, which are responsible for the improvement in the charge dynamics as evidenced by the results from various techniques including photoluminescence (PL) spectroscopy, photocurrent measurements, and electrochemical impedance spectroscopy (EIS). Owing to the good dynamical properties, NP-Pd-TCN was used for photocatalytic hydrogen evolution under visible-light irradiation (λ > 420 nm) and an excellent evolution rate of ~ 381 μmol·h −1 (0.02 g of the photocatalyst) was attained. This work aims to promote a strategy to synthesize efficient photocatalysts for hydrogen production by controllably introducing metal nanoparticles on a support and in the meantime forming chemical bonds to achieve intimate metal-support contact.

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Nano Research
Pages 2928-2934
Cite this article:
Xiao X, Lin S, Zhang L, et al. Constructing Pd–N interactions in Pd/g-C3N4 to improve the charge dynamics for efficient photocatalytic hydrogen evolution. Nano Research, 2022, 15(4): 2928-2934. https://doi.org/10.1007/s12274-021-3905-y
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Received: 27 August 2021
Revised: 25 September 2021
Accepted: 26 September 2021
Published: 04 December 2021
© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2021
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