A strong-alkali resistant zinc-organic framework with 1,3,6,8-tetra(pyridin-4-yl)pyrene for efficient photocatalytic hydrogen evolution

• Published in: Journal of materials chemistry. A, Materials for energy and sustainability Materials for energy and sustainability, 2023-08, Vol.11 (3), p.16255-16262
• Main Authors: Yang, Guo-Li, Xie, Yao, Jiao, Zhuo-Hao, Zhao, Jian, Hou, Sheng-Li, Shi, Ying, Han, Jie, Zhao, Bin
• Format: Article
• Language: English
• Subjects: Absorption; Aqueous solutions; Catalytic activity; Density functional theory; Electromagnetic absorption; Energy gap; Evolution; Exploitation; Hydrogen evolution; Hydrogen production; Metal-organic frameworks; Photocatalysis; Photoelectric effect; Pyrene; Sodium hydroxide; Zinc
• ISSN: 2050-7488; 2050-7496
• DOI: 10.1039/d3ta02520a

Photocatalytic hydrogen evolution using metal-organic frameworks (MOFs) has tremendous potential for relieving the environmental and energy crises. Herein, a three dimensional zinc-organic framework ( 1 ) was successfully synthesized based on 1,3,6,8-tetra(pyridin-4-yl)pyrene (TTPy). Compound 1 exhibited a good light absorption with an absorption edge at approximately 600 nm. Importantly, 1 can maintain the crystalline state in TEOA solution, and even remain stable in a 5 M NaOH aqueous solution, suggesting 1 has high alkali resistance. Photocatalytic results indicate that 1 as a photocatalyst has high activity for H 2 production with TEOA as a sacrificial agent, and the H 2 evolution rate is 315.06 μmol g −1 h −1 even under long reaction time (35 h) without the addition of photosensitizers. Mechanism explorations suggest that the π-π interaction between parallel ligands, high alkali-stability and light-absorbing ability, good photocurrent response, and suitable band gap of compound 1 are responsible for the high photocatalytic activity. Density functional theory (DFT) calculations further reveal that the experimental energy gap of 1 is well consistent with the theoretical bandgap. This work provides a new strategy for the exploitation of alkali-stable MOFs in the photocatalysis field. A 3D Zn-MOF was for the first time synthesized from TTPy, and it exhibited excellent alkali-stability and high H 2 production rate (315.06 μmol g −1 h −1 ) in photocatalytic experiments.