Although ammonia (NH3) synthesis efficiency
from the
NO reduction reaction (NORR) is significantly promoted in recent years,
one should note that NO is one of the major air pollutants in the
flue gas. The limited NO conversion ratio is still the key challenge
for the sustainable development of the NORR route, which potentially
contributes more to contaminant emissions rather than its upcycling.
Herein, we provide a simple but effective approach for continuous
NO reduction into NH3, promoted by coexisting SO2 poison as a gift in the flue gas. It is significant to discover
that SO2 plays a decisive role in elevating the capacity
of NO absorption and reduction. A unique redox pair of SO2–NO is constructed, which contributes to the exceptionally
high conversion ratio for both NO (97.59 ± 1.42%) and SO2 (99.24 ± 0.49%) in a continuous flow. The ultrahigh
selectivity for both NO-to-NH3 upcycling (97.14 ±
0.55%) and SO2-to-SO4
2– purification
(92.44 ± 0.71%) is achieved synchronously, demonstrating strong
practicability for the value-added conversion of air contaminants.
The molecular mechanism is revealed by comprehensive in situ technologies to identify the essential contribution of SO2 to NO upcycling. Besides, realistic practicality is realized by
the efficient product recovery and resistance ability against various
poisoning effects. The proposed strategy in this work not only achieves
a milestone efficiency for NH3 synthesis from the NORR
but also raises great concerns about contaminant resourcing in realistic
conditions.