Efficient nitrogen fixation to ammonia through integration of plasma oxidation with electrocatalytic reduction
Date
2021
Authors
Li, L.
Tang, C.
Cui, X.
Zheng, Y.
Wang, X.
Xu, H.
Zhang, S.
Shao, T.
Davey, K.
Qiao, S.
Editors
Advisors
Journal Title
Journal ISSN
Volume Title
Type:
Journal article
Citation
Angewandte Chemie International Edition, 2021; 60(25):14131-14137
Statement of Responsibility
Laiquan Li, Cheng Tang, Xiaoyang Cui, Yao Zheng, Xuesi Wang, Haolan Xu ... et al.
Conference Name
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.
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Dissertation Note
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Description
First published: 14 April 2021
Data source: Supporting information, 10.1002/anie.202104394
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© 2021 Wiley-VCH GmbH.