Sustainable,
renewable-energy-powered, and low-carbon-emission
alternatives for the energy-intensive and extreme-process-conditions-demanding
industrial Haber–Bosch ammonia synthesis are urgently needed
to meet global net-zero emission targets. Plasma catalysis enables
renewable-electricity-driven ammonia synthesis under mild conditions.
To reveal unknown energy-efficient pathways for ammonia synthesis,
here, we specify energy loss pathways and maximize the energy efficiency
of the ammonia synthesis in atmospheric-pressure and low-temperature
pulsed plasmas. The ammonia yield, energy efficiency, and process
temperature are obtained under variable process parameters (i.e.,
the pulse voltage, pulse width, and gap distance) in a nanosecond
pulse dielectric barrier discharge reactor. The ways to reduce energy
losses for “power-to-chemical (= ammonia)” production
including N2 vibrational excitation and relaxation are
revealed by combining plasma optical emission spectroscopy with chemical
reaction kinetics modeling. Multiparameter process optimization based
on the Bayesian neural network model allows us to select the pulse
waveforms, voltages, and discharge gaps to achieve high ammonia yields
with a high energy efficiency and a low emission footprint.