N 2 Electroreduction to NH 3 by Selenium Vacancy‐Rich ReSe 2 Catalysis at an Abrupt Interface

Lai, Feili, Zong, Wei, He, Guanjie , Xu, Yang, Huang, Haowei, Weng, Bo, Rao, Dewei, Martens, Johan A., Hofkens, Johan, Parkin, Ivan P. and Liu, Tianxi (2020) N 2 Electroreduction to NH 3 by Selenium Vacancy‐Rich ReSe 2 Catalysis at an Abrupt Interface. Angewandte Chemie, 132 (32). pp. 13422-13429. ISSN 0044-8249

Full content URL: https://doi.org/10.1002/ange.202003129

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Item Type:Article
Item Status:Live Archive

Abstract

Vacancy engineering has been proved repeatedly as an adoptable strategy to boost electrocatalysis, while its poor selectivity restricts the usage in nitrogen reduction reaction (NRR) as overwhelming competition from hydrogen evolution reaction (HER). Revealed by density functional theory calculations, the selenium vacancy in ReSe2 crystal can enhance its electroactivity for both NRR and HER by shifting the d‐band from −4.42 to −4.19 eV. To restrict the HER, we report a novel method by burying selenium vacancy‐rich ReSe2@carbonized bacterial cellulose (Vr‐ReSe2@CBC) nanofibers between two CBC layers, leading to boosted Faradaic efficiency of 42.5 % and ammonia yield of 28.3 μg h−1 cm−2 at a potential of −0.25 V on an abrupt interface. As demonstrated by the nitrogen bubble adhesive force, superhydrophilic measurements, and COMSOL Multiphysics simulations, the hydrophobic and porous CBC layers can keep the internal Vr‐ReSe2@CBC nanofibers away from water coverage, leaving more unoccupied active sites for the N2 reduction (especially for the potential determining step of proton‐electron coupling and transferring processes as *NN → *NNH).

Keywords:carbon nanofibers, COLSOM simulation, DFT calculations, nitrogen reduction reaction, ReSe2
Subjects:F Physical Sciences > F200 Materials Science
F Physical Sciences > F100 Chemistry
Divisions:College of Science > School of Chemistry
ID Code:43118
Deposited On:25 Nov 2020 14:13

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