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Multiscale Sampling of a Heterogeneous Water/Metal Catalyst Interface using Density Functional Theory and Force-Field Molecular Dynamics

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Published on: April 12, 2019

Covalent Organic Frameworks Anchoring Single-Atom Pt for Three-Phase Interface-Assisted Photocatalytic Overall Water

Ting-Ting Sun¹, Hao Zhang¹, Ya Wang¹

¹Heilongjiang Provincial Key Laboratory of CO2 Resource Utilization and Energy Catalytic Materials, School of Material Science and Chemical Engineering, Harbin University of Science and Technology, Harbin, 150080, P.R. China.

Angewandte Chemie (International Ed. in English)

|September 18, 2025

Summary

Atomically dispersed platinum in covalent organic frameworks (COFs) enhances overall water splitting (OWS). A novel gas-liquid-solid system boosts hydrogen and oxygen production rates and stability, suppressing reverse reactions.

Keywords:

Covalent organic frameworks Overall water splitting Photocatalysis Single‐atom Pt Three‐phase interface strategy

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Area of Science:

Materials Science
Photocatalysis
Renewable Energy

Background:

Covalent organic frameworks (COFs) show potential for overall water splitting (OWS).
Existing COF systems use cocatalysts prone to aggregation and low atomic utilization.
The oxygen reduction reaction (ORR) backward reaction limits catalytic efficiency and stability.

Purpose of the Study:

To develop a COF-based photocatalyst with atomically dispersed platinum for enhanced OWS.
To improve catalytic performance and durability by integrating a gas-liquid-solid three-phase interface.
To investigate the underlying mechanisms of enhanced photocatalysis.

Main Methods:

Synthesis of triazine-based COFs with N/O-coordinated atomically dispersed Pt sites (Pt-TBPyT-COF).
Implementation of a gas-liquid-solid three-phase interface-assisted photocatalytic system.
Characterization using density functional theory (DFT) calculations and in situ experiments.

Main Results:

Pt-TBPyT-COF achieved H2 and O2 evolution rates of 469.8 and 234.9 µmol·g−1·h−1, with an apparent quantum yield of 8.91% at 450 nm.
The gas-liquid-solid system improved H2 and O2 rates to 568.7 and 284.3 µmol·g−1·h−1 over 5 hours, suppressing ORR.
Stable photocatalytic activity was maintained for 30 hours.

Conclusions:

Atomically dispersed Pt sites in COFs accelerate H desorption.
Triazine units in COFs facilitate charge separation and reduce OER energy barriers.
The integrated system significantly enhances OWS performance, efficiency, and durability.