Yang Guo-Li, Che Xue-Jing, Hou Sheng-Li, Cao Chun-Shuai, Zhao Bin
Department of Chemistry, Key Laboratory of Advanced Energy Material Chemistry, MOE Nankai University, Tianjin 300071, China.
Shenyang National Laboratory for Materials Science (SYNL), Institute of Metal Research (IMR), Chinese Academy of Sciences (CAS), No. 72 Wenhua Road, Shenyang 110016, China.
Inorg Chem. 2021 Feb 1;60(3):1922-1929. doi: 10.1021/acs.inorgchem.0c03397. Epub 2021 Jan 15.
Photocatalytic hydrogen evolution is desired to effectively alleviate the serious crisis of energy and the environment, and the utilization of low-cost photocatalysts, especially cobalt-based MOF catalysts, is meaningful, but rarely investigated. Herein, through a self-assembly strategy, we synthesized a Co clusters-based MOF () by the ligand ,'-bicyclo[2.2.2]oct-7-ene-2,3,5,6-tetracarboxdiimide bi(1,2,4-triazole), containing abundant carbonyl O atoms in the channels of the 3D skeleton, and a large porosity of 50.7%. The as-synthesized MOF can be stable in the pH range of 3-10 and shows a narrow band gap of 1.82 eV. Furthermore, its maximum amount of water absorption can reach 192 cm/g. Under irradiation of simulated solar light, the rate of hydrogen evolution is 23.05 μmol·h·g among 12 h with the presence of co-catalyst Pt and photosensitizer RhB. The reaction mechanism has been probed by the transient photocurrent response and steady-state photoluminescence spectra. Therefore, as a narrow band gap photocatalyst, the cobalt clusters-based MOF () has potential applications for hydrogen evolution from water.
光催化析氢有望有效缓解严重的能源和环境危机,利用低成本的光催化剂,尤其是钴基金属有机框架催化剂,具有重要意义,但很少有人对此进行研究。在此,我们通过自组装策略,使用配体,'-双环[2.2.2]辛-7-烯-2,3,5,6-四羧酸二亚胺双(1,2,4-三唑)合成了一种基于钴簇的金属有机框架(),其三维骨架通道中含有丰富的羰基氧原子,孔隙率高达50.7%。所合成的金属有机框架在pH值为3至10的范围内稳定,带隙窄至1.82 eV。此外,其最大吸水量可达192 cm/g。在模拟太阳光照射下,在助催化剂Pt和光敏剂RhB存在的情况下,12小时内析氢速率为23.05 μmol·h·g。通过瞬态光电流响应和稳态光致发光光谱对反应机理进行了探究。因此,作为一种窄带隙光催化剂,基于钴簇的金属有机框架()在水分解制氢方面具有潜在的应用前景。