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Electrocatalytic nitrogen reduction (eNRR) offers a green pathway for NH3 production from N2 and H2O under ambient conditions. Transition metal oxynitrides (TMOxNy) are among the most promising catalysts but face challenges in achieving high yield and faradaic efficiency (FE). This work develops a hybrid WOxNy/WO3 catalyst with a unique heterogeneous interfacial complexion (HIC) structure. This design enables in situ generation and delivery of highly active hydrogen atoms (H*) in acidic electrolytes, promoting nitrogen hydrogenation and formation of nitrogen vacancies (Nv) on the WOxNy surface. This significantly enhances the selectivity of eNRR for NH3 synthesis while suppressing hydrogen evolution reaction (HER). A simple two-step fabrication process—microwave hydrothermal growth followed by plasma-assisted surface nitridation—was developed to fabricate the designed catalyst electrode, achieving an NH3 yield of 3.2 × 10-10 mol·cm-2·s-1 with 40.1% FE, outperforming most TMN/TMOxNy electrocatalysts. Multiple control experiments confirm that the eNRR follows a HIC-enhanced Mars-van Krevelen (MvK) mechanism. 

Non-equilibrium plasma has been found to have a synergistic effect on catalytic synthesis of NH₃. 

In plasma discharges, the acceleration of electrons by a fast varying electric field and the subsequent collisional electron energy transfer determines the plasma dynamics, chemical reactivity, and breakdown. Current in situ electric field measurements require reconstruction of the temporal profile over many observations. However, such methods are unsuitable for non-repetitive and unstable plasmas. Here, we present a method for creating “movies” of dynamic electric fields in a single acquisition at sample rates of 500 × 106 fps. This ultrafast diagnostic was demonstrated in radio frequency electric fields between two parallel plates in air, as well as in Ar nanosecond-pulsed single-sided dielectric barrier discharges. 

Abstract Manipulating surface charge, electric field, and plasma afterglow in a non-equilibrium plasma is critical to control plasma-surface interaction for plasma catalysis and manufacturing. Here, we show enhancements of surface charge, electric field during breakdown, and afterglow by ferroelectric barrier discharge. The results show that the ferroelectrics manifest spontaneous electric polarization to increase the surface charge by two orders of magnitude compared to discharge with an alumina barrier. Time-resolved in-situ electric field measurements reveal that the fast polarization of ferroelectrics enhances the electric field during the breakdown in streamer discharge and doubles the electric field compared to the dielectric barrier discharge. Moreover, due to the existence of surface charge, the ferroelectric electrode extends the afterglow time and makes discharge sustained longer when alternating the external electric field polarity. The present results show that ferroelectric barrier discharge offers a promising technique to tune plasma properties for efficient plasma catalysis and electrified manufacturing. 

This study examines low-temperature chemistry (LTC) enhancement by nanosecond dielectric barrier discharge (ns-DBD) plasma on a dimethyl ether (DME)/oxygen [Formula: see text] (Ar) premixture for deflagration-to-detonation transition (DDT) in a microchannel. It is found that non-equilibrium plasma generates active species and kinetically accelerates LTC of DME and DDT. In situ laser diagnostics and computational modeling examine the influence of the ns-DBDs on the LTC of DME and DDT using formaldehyde ([Formula: see text]) laser-induced fluorescence (LIF) and high-speed imaging. Firstly, high-speed imaging in combination with LIF is used to trace the presence of LTC throughout the flame front propagation and DDT. Then, competition between plasma-enhanced LTC of ignition and reduced heat release rate of combustion due to plasma-assisted partial fuel oxidation is studied with LIF. Observations of plasma-enhanced LTC effects on DDT are interpreted with the aid of detailed kinetic simulations. The results show that an appropriate number of ns-DBDs enhances LTC of DME and increases [Formula: see text] formation and low-temperature ignition, accelerating DDT. Moreover, it is found that, with many ns-DBDs, [Formula: see text] concentration decreases, indicating that excessive discharges may accelerate fuel oxidation in the premixture, reducing heat release and weakening shock–ignition coupling, inhibiting DDT.