Green pathway of Urea Synthesis through Plasma-Ice Interaction Optimization and Mechanistic Insights with N2 + CO2 and NH3 + CO2 Gas Mixtures

Abstract

This study explores a green pathway for urea synthesis using plasma-ice interaction with gas mixtures of N2 + CO2 and NH3 + CO2. Electrical and optical emission spectroscopy were employed to characterize the plasmas, revealing that urea formation involves complex reactions driven by high-energy species, producing reactive nitrogen and carbon intermediates that further react to form urea. Physicochemical analyses of plasma-treated ice showed increased pH, electrical conductivity (EC), and reduced oxidation-reduction potential (ORP). Optimization of plasma process parameters (gas pressure, applied voltage, and treatment time) was performed to enhance urea formation. Among these parameters, plasma treatment time had the most substantial influence. Increasing treatment time from 20 to 60 minutes significantly impacted physicochemical properties: for N2 + CO2 plasma, pH increased by 21.05%, EC by 184.7%, and ORP decreased by 27.48%; for NH3 + CO2 plasma, pH increased by 27.37%, EC by 239.05%, and ORP decreased by 72.67%, respectively. The study shows that NH3 + CO2 plasma produces a significantly higher concentration of urea (7.7 mg L-1) compared to N2 + CO2 plasma (0.55 mg L-1). This is attributed to the direct availability and reactivity of ammonia, which simplifies reaction pathways and enhances intermediate formation. These findings highlight the potential of plasma-ice interaction as an energy-efficient and environmentally friendly method for urea synthesis, offering a sustainable alternative to conventional processes.