Iron Nanoparticle-Incorporated Laser-Induced Graphene Filters for Environmental Remediation via an In Situ Electro-Fenton Process

Abstract

Laser-induced graphene (LIG) has garnered much attention due to its facile and chemically free fabrication technique. Metal nanoparticle incorporation into the LIG matrix can improve its electrical and catalytical properties for environmental application. Here, we demonstrate the fabrication of nanoscale zerovalent iron (nZVI) nanoparticle-incorporated LIG (Fe-LIG) and sulfidized-nanoscale zerovalent iron (S-nZVI) nanoparticle-incorporated LIG (SFe-LIG) surfaces. The sheets were first fabricated to investigate nanoparticle loading, successful incorporation in the LIG matrix, and electrochemical performance as electrodes. Fe-LIG and SFe-LIG sheets showed ∼3-3.5 times more charge density as compared with the control LIG sheet. The XPS and its deconvolution confirmed the presence of nZVI and S-nZVI in the Fe-LIG and SFe-LIG surfaces, which can generate in situ hydroxyl radical (•OH) via iron activation of electrogenerated hydrogen peroxide (H2O2) in short in situ electro-Fenton process. After confirmation of the successful incorporation of iron-based nanoparticles in the LIG matrix, filters were fabricated to demonstrate the application in the flow-through filtration. The Fe-LIG and SFe-LIG filters showed ∼10-30% enhanced methylene blue removal under the application of 2.5 V at ∼1000 LMH flux. The Fe-LIG and SFe-LIG filters also showed complete 6-log bacteria and virus removal at 2.5 and 5 V, respectively, while the LIG filters showed only ∼4-log removal. Such enhanced removal by the Fe-LIG and SFe-LIG filters as compared to LIG filters is attributed to the improved charge density, electrochemical activity, and in situ electro-Fenton process. The study shows the potential to develop catalytic LIG-based surfaces for various applications, including contaminant removal and microbial inactivation.