This review underlines the strategies to suppress HER for selective NRR in view of proton-/electron-transfer kinetics, thermodynamics, and electrocatalyst design on the basis of deep understanding for NRR mechanisms.
With the increasingly prominent energy issues and environment problems, the electrocatalytic production of value-added fine chemicals by hybrid water electrolysis has posed much hope for replacing the conventionally energy-intensive chemical...
Integrated/cascade plasma-enabled
N2 oxidation and electrocatalytic
NO
x
– (where x = 2, 3) reduction reaction (pNOR-eNO
x
–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 eNO
x
–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 eNO
x
–RR at a microscopic level is also decoupled using copper (Cu) nanoparticles
as a representative electrocatalyst. The concentration of produced
NO
x
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 NO
x
– and the key N-containing intermediates (e.g., −NH2) of eNO
x
–RR are detected
with in situ infrared spectroscopy. Besides, in situ Raman spectroscopy further reveals the dynamic reconstruction
process of Cu nanoparticles during the eNO
x
–RR process. The Cu nanoparticle-driven pNOR-eNO
x
–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-eNO
x
–RR
system for the green electrosynthesis of NH3 directly from
air and water under ambient conditions.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.