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

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• Valence electron structure and cohesive energy of OH cleavage process were obtained. • Transition metals are robust electron donors for OH yield implying its ratio pivotal. • Excellent mineralization of AMTH was observed at all pH values after 8 h treatment. • Degradation pathways and intermediates of Amitriptyline were elaborated. 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.