Multiphase Porous Electrochemical Catalysts Derived from Iron-Based Metal-Organic Framework Compounds

Herbicide use has attracted attention recently due to potential damage to human health and lethality to the honey bees and other pollinators. Fenton reagent treatment processes can be applied for the degradation of herbicidal contaminants from water. However, the need to carry out the normal Fenton reactions under acidic conditions often hinders their practical application for pollution control. Herein, we report on the synthesis and application of multiphasic porous electro-Fenton catalysts prepared from calcinated metal-organic framework compounds, CMOF@PCM, and their application for the mineralization of herbicides in aqueous solution at circum-neutral pH. CMOF nanoparticles (NPs) are anchored on porous carbon monolithic (PCM) substrates, which allow for binder-free application. H₂O₂ is electrochemically generated on the PCM substrate which serves as a cathode, while ·OH is generated by the CMOF NPs at low applied potentials (-0.14 V). Results show that the structure and reactivity of the CMOF@PCM electro-Fenton catalysts are dependent on the specific MOF precursor used during synthesis. For example, CMIL-88-NH₂, which is prepared from MIL-88(Fe)-NH₂, is a porous core-shell structured NP comprised of a cementite (Fe₃C) intermediate layer that is sandwiched between a graphitic shell and a magnetite (Fe₃O₄) core. The electro-Fenton production of hydroxyl radical on the CMOF@PCM composite material is shown to effectively degrade an array of herbicides.