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

Murphy, Eamonn; Liu, Yuanchao; Matanovic, Ivana; Rüscher, Martina; Huang, Ying; Ly, Alvin; Guo, Shengyuan; Zang, Wenjie; Yan, Xingxu; Martini, Andrea; Timoshenko, Janis; Cuenya, Beatriz Roldán; Zenyuk, Iryna V.; Pan, Xiaoqing; Spoerke, Erik D.; Atanassov, Plamen

doi:10.1038/s41467-023-40174-4

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

Journal Article · 27 July 2023 · Nature Communications

DOI: https://doi.org/10.1038/s41467-023-40174-4 · OSTI ID:1992949

Murphy, Eamonn;

; Matanovic, Ivana; Rüscher, Martina;

; Ly, Alvin;

;

; Martini, Andrea;

;

Abstract Electrocatalytic reduction of waste nitrates (NO ₃ ⁻ ) enables the synthesis of ammonia (NH ₃ ) 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; 3 d -, 4 d -, 5 d - and f -block M-N-C catalysts. The selectivity and activity of NO ₃ ⁻ reduction to NH ₃ in neutral media, with a specific focus on deciphering the role of the NO ₂ ⁻ intermediate in the reaction cascade, reveals strong correlations (R=0.9) between the NO ₂ ⁻ reduction activity and NO ₃ ⁻ reduction selectivity for NH ₃ . Moreover, theoretical computations reveal the associative/dissociative adsorption pathways for NO ₂ ⁻ evolution, over the normal M-N ₄ sites and their oxo-form (O-M-N ₄ ) for oxyphilic metals. This work provides a platform for designing multi-element NO ₃ RR cascades with single-atom sites or their hybridization with extended catalytic surfaces.

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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: European Research Council (ERC); National Science Foundation (NSF); USDOE; USDOE National Nuclear Security Administration (NNSA); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Energy Efficiency Office. Advanced Materials & Manufacturing Technologies Office (AMMTO); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: 89233218CNA000001; AC02-05CH11231; AC02-06CH11357; NA0003525

OSTI ID:: 1992949

Report Number(s):: LA-UR--22-29040; 4554; PII: 40174

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 14; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

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