Selective electrochemical reduction of nitric oxide to hydroxylamine by atomically dispersed iron catalyst

Dong Hyun Kim, Stefan Ringe, Haesol Kim, Sejun Kim, Bupmo Kim, Geunsu Bae, Hyung-Suk Oh, Frédéric Jaouen, Wooyul Kim (), Hyungjun Kim () and Chang Hyuck Choi ()
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Dong Hyun Kim: Gwangju Institute of Science and Technology
Stefan Ringe: Daegu Gyeongbuk Institute of Science and Technology
Haesol Kim: Gwangju Institute of Science and Technology
Sejun Kim: Korea Advanced Institute of Science and Technology
Bupmo Kim: Pohang University of Science and Technology
Geunsu Bae: Gwangju Institute of Science and Technology
Hyung-Suk Oh: Clean Energy Research Center, Korea Institute of Science and Technology
Frédéric Jaouen: ICGM, Université de Montpellier, CNRS, ENSCM
Wooyul Kim: Sookmyung Women’s University
Hyungjun Kim: Korea Advanced Institute of Science and Technology
Chang Hyuck Choi: Gwangju Institute of Science and Technology

Nature Communications, 2021, vol. 12, issue 1, 1-11

Abstract: Abstract Electrocatalytic conversion of nitrogen oxides to value-added chemicals is a promising strategy for mitigating the human-caused unbalance of the global nitrogen-cycle, but controlling product selectivity remains a great challenge. Here we show iron–nitrogen-doped carbon as an efficient and durable electrocatalyst for selective nitric oxide reduction into hydroxylamine. Using in operando spectroscopic techniques, the catalytic site is identified as isolated ferrous moieties, at which the rate for hydroxylamine production increases in a super-Nernstian way upon pH decrease. Computational multiscale modelling attributes the origin of unconventional pH dependence to the redox active (non-innocent) property of NO. This makes the rate-limiting NO adsorbate state more sensitive to surface charge which varies with the pH-dependent overpotential. Guided by these fundamental insights, we achieve a Faradaic efficiency of 71% and an unprecedented production rate of 215 μmol cm−2 h−1 at a short-circuit mode in a flow-type fuel cell without significant catalytic deactivation over 50 h operation.

Date: 2021
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Persistent link: https://EconPapers.repec.org/RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-22147-7

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DOI: 10.1038/s41467-021-22147-7

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