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Updated: Jun 19, 2025
Synthesis of Metal Nanoparticles Supported on Carbon Nanotube with Doped Co and N Atoms and its Catalytic Applications in Hydrogen Production
Published on: December 6, 2021
Engineering single-atom rhodium-C3N sites on covalent organic frameworks for boosting photocatalytic hydrogen
Delu Zhang1, Chao Zhang1, Xiaoning Lai1
1State Key Laboratory Base for Eco-chemical Engineering, College of Chemical Engineering, Qingdao University of Science and Technology, Qingdao 266042, China.
Abstract:
Developing efficient and stable photocatalysts for solar hydrogen (H2) energy conversion is meaningful but challenging. Herein, a novel photocatalyst with Rh single atoms (Rh SAs) anchoring in β-ketoimine-linked covalent organic frameworks (TpPa-1) via RhC3N sites is proposed for achieving highly efficient H2 production in phosphate buffer saline (PBS) solution with sodium ascorbate (SA) as sacrificial agent under visible light. TpPa-1 with abundant N and C-chelate sites provides a reliable basis for anchoring Rh single atoms. The optimized Rh SAs/TpPa-1 exhibits an outstanding hydrogen evolution activity (1836.81μmol h-1 g-1), 9.34 and 2.27 folds enhancement than that of pristine TpPa-1 and Rh NPs/TpPa-1. X-ray absorption fine structure (XAFS) combined with density functional theory (DFT) calculations reveal that the significant improvement in H2 evolution performance on Rh SAs/TpPa-1 originates from the unique RhC3N coordination environment, promoting the charge separation and migration at the atomic interface, and thus decreasing the energy barrier for H* formation. Notably, in situ Raman technique confirmed Rh SAs was the main active sites (RhH) for proton reduction.
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