Issue 9, 2024

Insight into mechanism for remarkable photocatalytic hydrogen evolution of Cu/Pr dual atom co-modified TiO2

Abstract

The development of high-activity photocatalysts is crucial for the current large-scale development of photocatalytic hydrogen applications. Herein, we have developed a strategy to significantly enhance the hydrogen photocatalytic activity of Cu/Pr di-atom co-modified TiO2 architectures by selectively anchoring Cu single atoms on the oxygen vacancies of the TiO2 surface and replacing a trace of Ti atoms in the bulk with rare earth Pr atoms. Calculation results demonstrated that the synergistic effect between Cu single atoms and Pr atoms regulates the electronic structure of Cu/Pr–TiO2, thus promoting the separation of photogenerated carriers and their directional migration to Cu single atoms for the photocatalytic reaction. Furthermore, the d-band center of Cu/Pr–TiO2, which is located at −4.70 eV, optimizes the adsorption and desorption behavior of H*. Compared to TiO2, Pr–TiO2, and Cu/TiO2, Cu/Pr–TiO2 displays the best H* adsorption Gibbs free energy (−0.047 eV). Furthermore, experimental results confirmed that the photogenerated carrier lifetime of Cu/Pr–TiO2 is not only the longest (2.45 ns), but its hydrogen production rate (34.90 mmol g−1 h−1) also significantly surpasses those of Cu/TiO2 (13.39 mmol g−1 h−1) and Pr–TiO2 (0.89 mmol g−1 h−1). These findings open up a novel atomic perspective for the development of optimal hydrogen activity in dual-atom-modified TiO2 photocatalysts.

Graphical abstract: Insight into mechanism for remarkable photocatalytic hydrogen evolution of Cu/Pr dual atom co-modified TiO2

Supplementary files

Article information

Article type
Communication
Submitted
08 May 2024
Accepted
24 Jun 2024
First published
08 Jul 2024

Nanoscale Horiz., 2024,9, 1532-1542

Insight into mechanism for remarkable photocatalytic hydrogen evolution of Cu/Pr dual atom co-modified TiO2

H. Zheng, B. Zi, T. Zhou, G. Qiu, Z. Luo, Q. Lu, A. R. P. Santiago, Y. Zhang, J. Zhao, J. Zhang, T. He and Q. Liu, Nanoscale Horiz., 2024, 9, 1532 DOI: 10.1039/D4NH00196F

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