Enhanced Nitrate-to-Ammonia Activity on Fe/ZnO Nanoparticles via Tuning Intermediate Adsorption in Alkaline Electrolyte
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Date
2024
Authors
Bui, T.S.
Ma, Z.
Yuwono, J.A.
Kumar, P.V.
O'Connell, G.E.P.
Peng, L.
Yang, Y.
Lim, M.
Daiyan, R.
Lovell, E.C.
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Journal article
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Advanced Functional Materials, 2024; 34(48):2408704-1-2408704-11
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Thanh Son Bui, Zhipeng Ma, Jodie A. Yuwono, Priyank V. Kumar, George E.P. O, Connell, Lingyi Peng, Yuwei Yang, Maggie Lim, Rahman Daiyan, Emma C. Lovell, and Rose Amal
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Abstract
The electrocatalytic recycling of waste nitrate (NO3RR) is a promising decentralized route for green ammonia synthesis. Nonetheless, it suffers from the competing hydrogen evolution reaction and the insufficient proton supply in high pH conditions. Herein, iron oxide nanoparticles anchored on ZnO is introduced as a strategy to enhance the water dissociation ability and proton transfer rate, advancing NH4 + production from alkaline NO3RR. Supported by a set of ex situ and in situ characterization, the findings reveal the reduction of iron oxides, along with improvements in charge transfer properties and proton generation from H2O. Theoretical calculations show that iron oxides reduce the kinetic barrier of the rate-limiting step (*NO2-to-*NO2H) and result in a thermodynamically favorable process to hydrogenation steps, which in turn reduce the overall energy barrier of alkaline NO3RR. Optimal catalytic activity is realized with a Fe loading of 0.5 wt.%, delivering a Faradaic efficiency of ≈83% for ammonium with a NH4 + yield rate of 31 nmol s−1 cm−2 at −0.7 V versus RHE. The results pave the way for the utilization of bi-metal interaction to tune the reaction pathway for achieving sustainable ammonium synthesis in alkaline, contributing to ongoing efforts to achieve a sustainable nitrogen cycle via N-based electrochemistry.
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© 2024 The Author(s). Advanced Functional Materials published by Wiley-VCH GmbH. This is an open access article under the terms of the Creative Commons Attribution-NonCommercial License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited and is not used for commercial purposes.