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N₂ Electroreduction to NH₃ by Selenium Vacancy-Rich ReSe₂ Catalysis at an Abrupt Interface

Lai, F; Zong, W; He, G; Xu, Y; Huang, H; Weng, B; Rao, D; ... Parkin, IP; + view all (2020) N₂ Electroreduction to NH₃ by Selenium Vacancy-Rich ReSe₂ Catalysis at an Abrupt Interface. Angewandte Chemie International Edition , 59 (32) pp. 13320-13327. 10.1002/anie.202003129. Green open access

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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 ReSe 2 crystal can enhance its electroactivity for both NRR and HER by shifting the d -band from -2.91 to -2.33 eV. To restrict the HER, we report a novel method by burying selenium vacancy-rich ReSe 2 @carbonized bacterial cellulose (V r -ReSe 2 @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 at 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 V r -ReSe 2 @CBC nanofibers away from water coverage, leaving more unoccupied active sites for the N 2 reduction (especially for the potential determining step of proton-electron coupling and transferring processes as *HNNH 2 → *H 2 NNH 2 ).

Type: Article
Title: N₂ Electroreduction to NH₃ by Selenium Vacancy-Rich ReSe₂ Catalysis at an Abrupt Interface
Location: Germany
Open access status: An open access version is available from UCL Discovery
DOI: 10.1002/anie.202003129
Publisher version: https://doi.org/10.1002/anie.202003129
Language: English
Additional information: This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions.
Keywords: COLSOM simulation, DFT calculation, ReSe2, carbon nanofiber, nitrogen reduction reaction
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
URI: https://discovery.ucl.ac.uk/id/eprint/10098293
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