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Type: Journal article
Title: Efficient nitrogen fixation to ammonia through integration of plasma oxidation with electrocatalytic reduction
Author: Li, L.
Tang, C.
Cui, X.
Zheng, Y.
Wang, X.
Xu, H.
Zhang, S.
Shao, T.
Davey, K.
Qiao, S.
Citation: Angewandte Chemie International Edition, 2021; 60(25):14131-14137
Publisher: Wiley
Issue Date: 2021
ISSN: 1433-7851
Statement of
Laiquan Li, Cheng Tang, Xiaoyang Cui, Yao Zheng, Xuesi Wang, Haolan Xu ... et al.
Abstract: Transformation of atmospheric nitrogen (N2) to ammonia (NH3) is a long-sought goal for human being. However, present one-step N2 fixation is impeded by tough activation of the N≡N bond and low selectivity to NH3. Here we report fixation of N2-to-NH3 can be advantageously decoupled to a two-step process with one problem solved independently and effectively in each step, including: 1) facile activation of N2 to NOx- by a non-thermal plasma technique, and; 2) highly selective conversion of NOx- to NH3 by electrocatalytic reduction. Importantly, this process uses air and water as low-cost raw materials for scalable ammonia production under ambient conditions. For NOx- reduction to NH3 we present a novel surface boron-rich core-shell nickel boride electrocatalyst. Combining a series of physical characterizations and in situ spectrometric measurements, we reveal that the surface boron-rich feature is the key to boosting activity, selectivity, and stability via enhanced NOx- adsorption, and suppression of hydrogen evolution and surface Ni oxidation. Consequently, a highly significant ammonia production of 198.3 µmol h-1 cm-2 was achieved, together with nearly 100% Faradaic efficiency.
Keywords: Boron-rich surface
Electrocatalytic nitrate reduction
Nitrogen fixation
ammonia production
Description: First published: 14 April 2021
Rights: © 2021 Wiley-VCH GmbH.
DOI: 10.1002/anie.202104394
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