Microscopic-Level
Insights into the Mechanism of Enhanced
NH3 Synthesis in Plasma-Enabled Cascade N2 Oxidation–Electroreduction
System
Posted on 2022-05-19 - 07:04
Integrated/cascade plasma-enabled
N2 oxidation and electrocatalytic
NOx– (where x = 2, 3) reduction reaction (pNOR-eNOx–RR) holds great promise for the renewable
synthesis of ammonia (NH3). However, the corresponding
activated effects and process of plasma toward N2 and O2 molecules and the mechanism of eNOx–RR to NH3 are unclear and need
to be further uncovered, which largely limits the large-scale deployment
of this process integration technology. Herein, we systematically
investigate the plasma-enabled activation and recombination processes
of N2 and O2 molecules, and more meaningfully,
the mechanism of eNOx–RR at a microscopic level is also decoupled using copper (Cu) nanoparticles
as a representative electrocatalyst. The concentration of produced
NOx in the pNOR system is confirmed as
a function of the length for spark discharge as well as the volumetric
ratio for N2 and O2 feeding gas. The successive
protonation process of NOx– and the key N-containing intermediates (e.g., −NH2) of eNOx–RR are detected
with in situ infrared spectroscopy. Besides, in situ Raman spectroscopy further reveals the dynamic reconstruction
process of Cu nanoparticles during the eNOx–RR process. The Cu nanoparticle-driven pNOR-eNOx–RR system can finally
achieve a high NH3 yield rate of ∼40 nmol s–1 cm–2 and Faradaic efficiency of
nearly 90%, overperforming the benchmarks reported in the literature.
It is anticipated that this work will stimulate the practical development
of the pNOR-eNOx–RR
system for the green electrosynthesis of NH3 directly from
air and water under ambient conditions.
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Ren, Yongwen; Yu, Chang; Wang, Linshan; Tan, Xinyi; Wang, Zhao; Wei, Qianbing; et al. (1753). Microscopic-Level
Insights into the Mechanism of Enhanced
NH3 Synthesis in Plasma-Enabled Cascade N2 Oxidation–Electroreduction
System. ACS Publications. Collection. https://doi.org/10.1021/jacs.2c00089