(Press-News.org) Photocatalytic hydrogen evolution is a key technology for clean energy conversion, in which platinum (Pt) is widely used as an effective cocatalyst. The anchoring and dispersion of Pt play a decisive role in catalytic performance. However, achieving precise control over metal-support interactions at the atomic level remains challenging due to the chemical heterogeneity of catalyst surfaces.
In a study published in Angewandte Chemie International Edition, Prof. ZHOU Xukai and his colleagues from the Dalian Institute of Chemical Physics (DICP) of the Chinese Academy of Sciences introduced a conformational isomer strategy to precisely tune the nitrogen atom positions, enhancing the photocatalytic hydrogen evolution performance of covalent organic frameworks (COFs).
COFs is ideal for studying metal-support interactions at the atomic level due to their programmable topology and well-defined pore environments. Combining trisubstituted aldehydes with trisubstituted aromatic amines or aromatic methyl compounds, researchers designed four COFs: two olefin-linked COFs (COF-A1/A2) and two imine-linked COFs (COF-I1/I2).
These COFs shared the same hexagonal pore topology, and the positions of nitrogen anchoring sites could be precisely tuned at the angstrom-level. After in situ photodeposition of Pt, the spatial arrangement of nitrogen atoms was found to play a decisive role in determining the dispersion and coordination environment of Pt species.
Multiple characterizations revealed that the imine-linked COF-I2 could simultaneously stabilize both Pt2+ single atoms and metallic Pt clusters, forming dual active sites, while the olefin-linked COF-A2 primarily anchored Pt single atoms. This structural difference directly led to a great disparity in photocatalytic performance: the hydrogen evolution rate of COF-I2-Pt was 6.1 times higher than that of COF-A2-Pt. Under monochromatic light irradiation at 420 nm, COF-I2-Pt achieved an apparent quantum efficiency of 12.1%.
Mechanistic investigations showed that the superior performance of COF-I2-Pt was because of the synergistic effect between Pt clusters and single atoms. The charge redistribution between them effectively promoted the separation of photogenerated electron-hole pairs and optimized the kinetics of proton adsorption and reduction. Femtosecond transient absorption spectroscopy confirmed that a prolonged lifetime of the key charge-separated state in COF-I2-Pt was the primary reason for efficient hydrogen evolution.
"Our study provides a new way for the rational design of atomically precise photocatalysts," said Prof. ZHOU. "And the concept of 'nitrogen-shift engineering' can be extended to the design of other porous framework materials, providing guidance for developing efficient energy conversion materials."
END
Researchers enhance photocatalytic hydrogen evolution performance of covalent organic frameworks by constitutional isomer strategy
2026-03-06
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