Synergistic effect of Pt single atoms, clusters and nanoparticles on carbon doping with nitrogen for highly efficient and selective hydrogenation of nitroaromatics

Abstract

This work constructs a series of Pt/NC catalysts with various Pt contents (0.22 wt%, 0.42 wt%, and 1.08 wt%) via the liquid-phase reduction method and their catalytic behaviors are systematically evaluated for heterogeneous catalytic hydrogenation of nitroarenes. The results show that 1.08% Pt/NC exhibits excellent catalytic performance: under quite mild conditions (30 °C, 1.0 MPa H2), it can efficiently convert nitrophenol within just 3 min (90.2% conversion), with nitro-group hydrogenation selectivity >99% and a TOF of 5298.6 h−1; moreover, it has an extremely ultra-high TOF of 74 191.8 h−1 in the hydrogenation reaction of nitrobenzene to aniline, showing ultra-high intrinsic activity. Additionally, using nitrobenzene selective hydrogenation as a model reaction, the proposed reaction pathways are provided. Combined with spherical Aberration Corrected-Transmission Electron Microscope (AC-STEM) and XPS characterization studies, it can be known that Pt single atoms, clusters and nanoparticles are together loaded on the surface of nitrogen-doped carbon, and there is electron interaction between pyridinic nitrogen and Pt (electrons transferring from Pt to N). Compared with other catalysts, the electronic interaction between Pt and N in 1.08% Pt/NC is stronger, its adsorption capacity for hydrogen at Pt nanoparticles and clusters and the –NO2 group at Pt single atoms via the interaction of “Ptδ+⋯O[double bond, length as m-dash]N” is superior, and it can greatly enhance the activity and selectivity of nitro-group hydrogenation.

Graphical abstract: Synergistic effect of Pt single atoms, clusters and nanoparticles on carbon doping with nitrogen for highly efficient and selective hydrogenation of nitroaromatics

Supplementary files

Article information

Article type
Paper
Submitted
11 Apr 2025
Accepted
27 May 2025
First published
28 May 2025

J. Mater. Chem. A, 2025, Advance Article

Synergistic effect of Pt single atoms, clusters and nanoparticles on carbon doping with nitrogen for highly efficient and selective hydrogenation of nitroaromatics

Y. Fang, Q. Liu, M. Tian, L. Ruan, K. Chen, H. Zhang, Z. Yang, H. Ye and L. Zhu, J. Mater. Chem. A, 2025, Advance Article , DOI: 10.1039/D5TA02865E

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