posted on 2024-01-08, 05:47authored byKai Chen, Jiaqi Xiang, Yali Guo, Xijun Liu, Xingang Li, Ke Chu
Electrochemical
reduction of NO to NH3 (NORR)
offers
a prospective method for efficient NH3 electrosynthesis.
Herein, we first design single-atom Pd-alloyed Cu (Pd1Cu)
as an efficient and robust NORR catalyst at industrial-level current
densities (>0.2 A cm–2). Operando spectroscopic
characterizations and theoretical computations unveil that Pd1 strongly electronically couples its adjacent two Cu atoms
(Pd1Cu2) to enhance the NO activation while
promoting the NO-to-NH3 protonation energetics and suppressing
the competitive hydrogen evolution. Consequently, the flow cell assembled
with Pd1Cu exhibits an unprecedented NH3 yield
rate of 1341.3 μmol h–1 cm–2 and NH3–Faradaic efficiency of 85.5% at an industrial-level
current density of 210.3 mA cm–2, together with
an excellent long-term durability for 200 h of electrolysis, representing
one of the highest NORR performances on record.