A tube-like Pd@coordination polymer with enhanced solar light harvesting for boosting photocatalytic H2 production in a wide pH range and seawater

• Published in: Nanoscale advances 2023-06, Vol.5 (13), p.3527-3535
• Main Authors: Li, Jieling, Sun, Shihao, Gao, Ningshuang, Li, Hua, Liang, Kun, Hai, Jun, He, Suisui, Mu, Xijiao, Wang, Baodui
• Format: Article
• Language: English
• Subjects: Chemistry
• ISSN: 2516-0230
• DOI: 10.1039/d3na00252g

Coordination polymers (CPs) have emerged as promising candidates for photocatalytic H 2 production owing to their structural tailorability and functional diversity. However, the development of CPs with high energy transfer efficiency for highly efficient photocatalytic H 2 production in a wide pH range still faces many challenges. Here we constructed a novel tube-like Pd( ii ) coordination polymer with well-distributed Pd nanoparticles (denoted as Pd/Pd( ii )CPs) based on the coordination assembly of rhodamine 6G and Pd( ii ) ions and further photo-reduction under visible light irradiation. Both the Br − ion and double solvent play a key role in forming the hollow superstructures. The resulting tube-like Pd/Pd( ii )CPs exhibit high stability in aqueous solution with the pH range from 3 to 14 due to the high Gibbs free energies of protonation and deprotonation, which provides the feasibility of photocatalytic hydrogen generation in a wide pH range. Electromagnetic field calculations showed that the tube-like Pd/Pd( ii )CPs have a good confinement effect on light. Therefore, the H 2 evolution rate could reach 112.3 mmol h −1 g −1 at pH 13 under visible light irradiation, which is far superior to those of reported coordination polymer-based photocatalysts. Moreover, such Pd/Pd( ii )CPs could also reach a H 2 production rate of 37.8 mmol h −1 g −1 in seawater under visible light with low optical density (40 mW cm −2 ) close to morning or cloudy sunlight. The above unique characteristics make the Pd/Pd( ii )CPs possess great potential for practical applications. Photocatalytic hydrogen generation by EY-sensitized tube-like Pd/Pd( ii )CPs in seawater and under different pH conditions.