Degradation intermediates of Amitriptyline and fundamental importance of transition metal elements in LDH-based catalysts in Heterogeneous Electro-Fenton system

This study proposes an efficient Layered Double Hydroxide-based (LDH-based) Heterogenous Electro Fenton (Hetero-EF) strategy that ensures the stable operation for representative antidepressants Amitriptyline Hydrochloride removal in a wide pH tolerance. The extra brilliant mineralization ability was over ~ 90% after 5 cycles. Moreover, the detailed degradation pathways and intermediates of Amitriptyline Hydrochloride were firstly elucidated and probed using ultra performance liquid chromatography quadrupole-time-of-flight mass spectrometry (UPLC-QTOF-MS). According to the Density Functional Theory and D-Band Center Theory, the subsequent computational simulation shed new light on the ability of LDH catalyzing for hydroxyl radical formation, the relevant role of transition metal atoms in LDH catalysts, and the electrons transfer process in the Hetero-EF reaction, i.e., LDH's metal atoms are robust electron donor sites for the generation of hydroxyl radical and charges transformation for the redox reaction, which highlights the importance of the transition metal elements in catalysts and exerts feasibility for enhancing the performance of Heterogeneous Electro-Fenton (Hetero-EF). Thereby, this research proposes a reliable strategy for building efficient Hetero-EF systems and gives a global contribution to developing the high-performance LDH EF-catalysts through the optimization of the metal atom ratio modification, synthesis parameters, and computational modeling.

Automated summary

This study proposes an efficient Heterogeneous Electro Fenton (Hetero-EF) strategy based on Layered Double Hydroxide (LDH) for stable removal of the antidepressant Amitriptyline Hydrochloride in a wide pH tolerance. The study also elucidates the detailed degradation pathways and intermediates of Amitriptyline Hydrochloride, and sheds new light on the ability of LDH to catalyze hydroxyl radical formation and the role of transition metal atoms in LDH catalysts through computational simulation.