Chu Xiaoyu, Wang Xinrui, Tian Shuo, Zhao Yongkuo, Liu Shikai, Yan Hong, Shang Yan
Heilongjiang 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.
Dalton Trans. 2024 Aug 27;53(34):14325-14332. doi: 10.1039/d4dt01271b.
Modulating the photogenerated electrons of CeO to activate O and efficiently photocatalytic degradation of chlorophenols is a highly desired goal. Herein, we have successfully fabricated an FePc/CeO heterojunction through H-bond induced assembly. The photocatalytic degradation of 2,4-DCP by the amount-optimized FePc/CeO nanocomposite was improved by 3 times compared with that by pure CeO. By means of electron paramagnetic resonance (EPR) and single wavelength photocurrent spectroscopy, it is confirmed that the excellent photocatalytic performance is mainly attributed to the formation of the Z-scheme heterojunction, which promotes charge separation and transfer, and the introduction of FePc broadens the visible light absorption range of the heterojunction. Moreover, O temperature-programmed-desorbed curves and electrochemical O reduction measurement results demonstrate that the single Fe-N(II) site in FePc is more conducive to promoting O activation than that of other metal phthalocyanines. Based on FT-IR and liquid chromatography-tandem mass spectrometry (LC-MS/MS), a possible reaction pathway of 2,4-DCP degradation was proposed. This study provides a novel strategy for preparing CeO based Z-scheme heterojunctions with abundant monoatomic sites for pollutant degradation.
调控CeO的光生电子以活化O并高效光催化降解氯酚是一个非常理想的目标。在此，我们通过氢键诱导组装成功制备了FePc/CeO异质结。与纯CeO相比，经量优化的FePc/CeO纳米复合材料对2,4-二氯酚的光催化降解性能提高了3倍。通过电子顺磁共振（EPR）和单波长光电流光谱证实，优异的光催化性能主要归因于Z型异质结的形成，其促进了电荷分离和转移，并且FePc的引入拓宽了异质结的可见光吸收范围。此外，O程序升温脱附曲线和电化学O还原测量结果表明，FePc中的单个Fe-N(II)位点比其他金属酞菁更有利于促进O活化。基于傅里叶变换红外光谱（FT-IR）和液相色谱-串联质谱（LC-MS/MS），提出了2,4-二氯酚降解的可能反应途径。本研究为制备具有丰富单原子位点的CeO基Z型异质结用于污染物降解提供了一种新策略。
