Title : Integrated dual-GDE system for high-efficiency ammonia synthesis from dilute no and energy-saving direct gaseous recovery
Abstract:
Electrochemical upcycling of nitrogenous air pollutants into green energy carriers offers a sustainable alternative to the energy-intensive Haber-Bosch process. However, conventional aqueous-phase nitric oxide reduction reaction (NORR) is strictly limited by low NO solubility and the complex post-separation of aqueous ammonium ions NH4+. Here, we present an integrated, highly energy-efficient dual-gas diffusion electrode (GDE) platform that couples high-rate NORR with continuous gaseous ammonia NH3 recovery from dilute NO (1–10% in Ar). In Stage 1, a GDE loaded with carbon-supported nanoscale zero-valent iron (Fe/C) successfully bypasses mass transport limitations, achieving a high NH3 Faradaic efficiency of 96% at 1% NO feed and a maximum production rate of 1239 umol/cm2h at 10% NO in 0.5M H2SO4. Density functional theory (DFT) calculations confirm that Fe/C selectively lowers the energy barrier for N–O bond cleavage in the H2NO intermediate. In Stage 2, the generated NH4+stream is directly routed into a GDE-based electrochemical stripping (GDE-ES) cell. Taking advantage of a highly alkaline cathodic microenvironment and an air sweep gas (20mL/min) functioning simultaneously as an oxygen reduction reaction (ORR) reactant and stripping carrier, the system achieves a superior nitrogen flux of 770 gN/m2/d at 10mA cm2. Benefit from cathodic ORR voltage compensation, the net energy demand was constrained to 9.44 kWh/ kg N, representing a 43–66% energy saving compared to conventional air stripping. This work establishes a closed-loop electrochemical route for converting industrial off-gases into high-purity chemical resources

