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Vacancy Engineering of Iron-Doped W18O49 Nanoreactors for Low-Barrier Electrochemical Nitrogen Reduction

Journal Article


Abstract


  • © 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim The electrochemical nitrogen reduction reaction (NRR) is a promising energy-efficient and low-emission alternative to the traditional Haber–Bosch process. Usually, the competing hydrogen evolution reaction (HER) and the reaction barrier of ambient electrochemical NRR are significant challenges, making a simultaneous high NH3 formation rate and high Faradic efficiency (FE) difficult. To give effective NRR electrocatalysis and suppressed HER, the surface atomic structure of W18O49, which has exposed active W sites and weak binding for H2, is doped with Fe. A high NH3 formation rate of 24.7 μg h−1 mgcat−1 and a high FE of 20.0 % are achieved at an overpotential of only −0.15 V versus the reversible hydrogen electrode. Ab initio calculations reveal an intercalation-type doping of Fe atoms in the tunnels of the W18O49 crystal structure, which increases the oxygen vacancies and exposes more W active sites, optimizes the nitrogen adsorption energy, and facilitates the electrocatalytic NRR.

Authors


  •   Tong, Yueyu (external author)
  •   Guo, Haipeng (external author)
  •   Liu, Daolan (external author)
  •   Yan, Xiao (external author)
  •   Su, Panpan (external author)
  •   Liang, Ji
  •   Zhou, Si
  •   Liu, Jian (external author)
  •   Lu, Gao (external author)
  •   Dou, Shi Xue

Publication Date


  • 2020

Citation


  • Tong, Y., Guo, H., Liu, D., Yan, X., Su, P., Liang, J., Zhou, S., Liu, J., Lu, G. & Dou, S. (2020). Vacancy Engineering of Iron-Doped W18O49 Nanoreactors for Low-Barrier Electrochemical Nitrogen Reduction. Angewandte Chemie - International Edition,

Scopus Eid


  • 2-s2.0-85082178466

Ro Metadata Url


  • http://ro.uow.edu.au/eispapers1/3851

Has Global Citation Frequency


Place Of Publication


  • Germany

Abstract


  • © 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim The electrochemical nitrogen reduction reaction (NRR) is a promising energy-efficient and low-emission alternative to the traditional Haber–Bosch process. Usually, the competing hydrogen evolution reaction (HER) and the reaction barrier of ambient electrochemical NRR are significant challenges, making a simultaneous high NH3 formation rate and high Faradic efficiency (FE) difficult. To give effective NRR electrocatalysis and suppressed HER, the surface atomic structure of W18O49, which has exposed active W sites and weak binding for H2, is doped with Fe. A high NH3 formation rate of 24.7 μg h−1 mgcat−1 and a high FE of 20.0 % are achieved at an overpotential of only −0.15 V versus the reversible hydrogen electrode. Ab initio calculations reveal an intercalation-type doping of Fe atoms in the tunnels of the W18O49 crystal structure, which increases the oxygen vacancies and exposes more W active sites, optimizes the nitrogen adsorption energy, and facilitates the electrocatalytic NRR.

Authors


  •   Tong, Yueyu (external author)
  •   Guo, Haipeng (external author)
  •   Liu, Daolan (external author)
  •   Yan, Xiao (external author)
  •   Su, Panpan (external author)
  •   Liang, Ji
  •   Zhou, Si
  •   Liu, Jian (external author)
  •   Lu, Gao (external author)
  •   Dou, Shi Xue

Publication Date


  • 2020

Citation


  • Tong, Y., Guo, H., Liu, D., Yan, X., Su, P., Liang, J., Zhou, S., Liu, J., Lu, G. & Dou, S. (2020). Vacancy Engineering of Iron-Doped W18O49 Nanoreactors for Low-Barrier Electrochemical Nitrogen Reduction. Angewandte Chemie - International Edition,

Scopus Eid


  • 2-s2.0-85082178466

Ro Metadata Url


  • http://ro.uow.edu.au/eispapers1/3851

Has Global Citation Frequency


Place Of Publication


  • Germany