Journal Article

PUBDB-2024-06370

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Synergizing Fe$_2$O$_3$ Nanoparticles on Single Atom Fe‐N‐C for Nitrate Reduction to Ammonia at Industrial Current Densities

Murphy, E. ; Sun, B. ; Rüscher, M.Extern* ; Liu, Y. ; Zang, W. ; Guo, S. ; Chen, Y.-H. ; Hejral, U.Extern* ; Huang, Y. ; Ly, A. ; Zenyuk, I. V. ; Pan, X. ; Timoshenko, J.Extern* ; Cuenya, B. R. ; Spoerke, E. D. ; Atanassov, P. (Corresponding author)

2024
Wiley-VCH Weinheim

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Please use a persistent id in citations: doi:10.1002/adma.202401133  doi:10.3204/PUBDB-2024-06370

Abstract: The electrochemical reduction of nitrates (NO3−) enables a pathway for the carbon neutral synthesis of ammonia (NH3), via the nitrate reduction reaction (NO3RR), which has been demonstrated at high selectivity. However, to make NH3 synthesis cost-competitive with current technologies, high NH3 partial current densities (jNH3) must be achieved to reduce the levelized cost of NH3. Here, the high NO3RR activity of Fe-based materials is leveraged to synthesize a novel active particle-active support system with Fe$_2$O$_3$ nanoparticles supported on atomically dispersed Fe–N–C. The optimized 3×Fe$_2$O$_3$/Fe–N–C catalyst demonstrates an ultrahigh NO3RR activity, reaching a maximum jNH3 of 1.95 A cm−2 at a Faradaic efficiency (FE) for NH3 of 100% and an NH3 yield rate over 9 mmol hr−1 cm−2. Operando XANES and post-mortem XPS reveal the importance of a pre-reduction activation step, reducing the surface Fe$_2$O$_3$ (Fe3+) to highly active Fe0 sites, which are maintained during electrolysis. Durability studies demonstrate the robustness of both the Fe$_2$O$_3$ particles and Fe–Nx sites at highly cathodic potentials, maintaining a current of −1.3 A cm−2 over 24 hours. This work exhibits an effective and durable active particle-active support system enhancing the performance of the NO3RR, enabling industrially relevant current densities and near 100% selectivity.

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Contributing Institute(s):

1. DOOR-User (DOOR ; HAS-User)

Research Program(s):

1. 6G3 - PETRA III (DESY) (POF4-6G3) (POF4-6G3)
2. SWEDEN-DESY - SWEDEN-DESY Collaboration (2020_Join2-SWEDEN-DESY) (2020_Join2-SWEDEN-DESY)

Experiment(s):

1. PETRA Beamline P64 (PETRA III)

Appears in the scientific report 2024

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Database coverage:
; ; ; Clarivate Analytics Master Journal List ; Current Contents - Engineering, Computing and Technology ; Current Contents - Physical, Chemical and Earth Sciences ; DEAL Wiley ; Essential Science Indicators ; IF >= 25 ; JCR ; Nationallizenz ; SCOPUS ; Science Citation Index Expanded ; Web of Science Core Collection

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