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Abstract
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-SO42- 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.
[1
]Research Center for Carbon-Neutral Environmental & Energy Technology, Institute of
Fundamental and Frontier Sciences, University of Electronic Science and Technology
of China, Chengdu, Sichuan 611731, People’s Republic of China