A ClO-mediated photoelectrochemical filtration system for highly-efficient and complete ammonia conversion.

Abstract

The ability to convert excess ammonia in water into harmless N2 is highly desirable for environmental remediation. We present a chlorine-oxygen radical (ClO)-mediated photoelectrochemical filtration system for highly efficient and complete ammonia removal from water. The customized photochemical device comprised a Ag-functionalized TiO2nanotube array mesh photoanode and a Pd-Cu co-modified nickel foam (Pd-Cu/NF) cathode. Under illumination, holes generated at the anode catalyzed the conversion of H2O and Cl- to HOand Cl, respectively. In turn, these radicals then reacted further, yielding ClO, which selectively decomposed ammonia. The cathode enabled further reduction of anodic byproducts such as NO3- to N2. The complete oxidation of all dissolved ammonia was achieved within 15 min reaction under neutral conditions, where N2 was the dominant product. The impact of key parameters was assessed, which enabled the discovery of optimal reaction conditions and the proposal of the underlying working mechanism. The flow-through configuration demonstrated a 5-fold increase of ammonia oxidation rate compared to the conventional batch reactor. The role of ClO in the oxidation of ammonia was verified with electron paramagnetic resonance and scavenger studies. This study provided greater mechanistic insights into photoelectrochemical filtration technology and demonstrated the potential of future nanotechnology for removing ammonia.