Elucidating electrochemical nitrate and nitrite reduction over atomically-dispersed transition metal sites

Eamonn Murphy, Yuanchao Liu, Ivana Matanovic, Martina Rüscher, Ying Huang, Alvin Ly, Shengyuan Guo, Wenjie Zang, Xingxu Yan, Andrea Martini, Janis Timoshenko, Beatriz Roldán Cuenya, Iryna V. Zenyuk, Xiaoqing Pan, Erik D. Spoerke and Plamen Atanassov ()
Additional contact information
Eamonn Murphy: University of California
Yuanchao Liu: University of California
Ivana Matanovic: University of New Mexico
Martina Rüscher: Fritz Haber Institute of the Max Planck Society
Ying Huang: University of California
Alvin Ly: University of California
Shengyuan Guo: University of California
Wenjie Zang: University of California
Xingxu Yan: University of California
Andrea Martini: Fritz Haber Institute of the Max Planck Society
Janis Timoshenko: Fritz Haber Institute of the Max Planck Society
Beatriz Roldán Cuenya: Fritz Haber Institute of the Max Planck Society
Iryna V. Zenyuk: University of California
Xiaoqing Pan: University of California
Erik D. Spoerke: Sandia National Laboratories
Plamen Atanassov: University of California

Nature Communications, 2023, vol. 14, issue 1, 1-15

Abstract: Abstract Electrocatalytic reduction of waste nitrates (NO3−) enables the synthesis of ammonia (NH3) in a carbon neutral and decentralized manner. Atomically dispersed metal-nitrogen-carbon (M-N-C) catalysts demonstrate a high catalytic activity and uniquely favor mono-nitrogen products. However, the reaction fundamentals remain largely underexplored. Herein, we report a set of 14; 3d-, 4d-, 5d- and f-block M-N-C catalysts. The selectivity and activity of NO3− reduction to NH3 in neutral media, with a specific focus on deciphering the role of the NO2− intermediate in the reaction cascade, reveals strong correlations (R=0.9) between the NO2− reduction activity and NO3− reduction selectivity for NH3. Moreover, theoretical computations reveal the associative/dissociative adsorption pathways for NO2− evolution, over the normal M-N4 sites and their oxo-form (O-M-N4) for oxyphilic metals. This work provides a platform for designing multi-element NO3RR cascades with single-atom sites or their hybridization with extended catalytic surfaces.

Date: 2023
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DOI: 10.1038/s41467-023-40174-4

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