Proceedings of Catalyst Design Strategies for Photo- and Electrochemical Fuel Synthesis (ECAT25)
Publication date: 19th December 2024
Graphdiyne (GDY) is an emerging two-dimensional (2D) carbon material composed of sp² and sp-hybridized carbon atoms, resulting in a regular and porous structure. GDY, rich in π-conjugated electrons, exhibits remarkable properties such as low weight, high mechanical strength, excellent conductivity, and tunable electronic and optical characteristics [1]. These outstanding features make GDY appealing for various applications, including electronic devices, catalysis and photocatalysis, purification membranes, and energy harvesting [2]. Notably, GDY’s intrinsic band gap (0.7–1.4 eV) plays a critical role in charge carrier mobility, making it particularly attractive for solar-to-chemical energy conversion [3]. Despite its exceptional properties, GDY faces challenges such as low processability and a narrow energy band arrangement, which limit its practical application in photocatalysis. To address these limitations, GDY needs structural modification, such as molecular functionalization, hybridization with metals and metal oxides, and heteroatom doping [4].
Here we present strategies for structural modifications of the GDY configuration, aiming to tailor its photophysical properties. In the first approach, pristine GDY was oxidized to generate oxygen defects, followed by size reduction to form quantum dots (QDs). In a complementary strategy, we synthesized nitrogen-doped GDY to tune its band gap and optical characteristics. The structural properties of GDY, both before and after modification, were characterized using techniques such as high-resolution transmission electron microscopy (HRTEM), Raman spectroscopy, and X-ray photoelectron spectroscopy (XPS). The experimental and theoretical results demonstrated that introducing oxygen defects or heteroatom doping induces significant changes in the electronic and optical properties of GDY. The engineered materials exhibited exceptional photosensitization when combined with commercial TiO₂-P25 for photocatalytic hydrogen generation. Notably, a hybrid material containing 1 wt% defect-rich GDY-QDs achieved a hydrogen evolution rate of 1322 μmol g⁻¹ h⁻¹, five times higher than TiO₂-P25 alone.
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