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Low-Coordinate Step Atoms via Plasma-Assisted Calcinations to Enhance Electrochemical Reduction of Nitrogen to Ammonia

Journal Article


Abstract


  • © 2020 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim The electrochemical N2 reduction reaction (NRR) is emerging as a promising alternative to the industrial Haber–Bosch process for distributed and modular production of NH3. Nevertheless, developing high-efficiency catalysts to simultaneously realize both high activity and selectivity for the development of a sustainable NRR is very critical but extremely challenging. Here, a unique plasma-assisted strategy is developed to synthesize iridium diphosphide nanocrystals with abundant surface step atoms anchored in P,N-codoped porous carbon nanofilms (IrP2@PNPC-NF), where the edges of the IrP2 nanocrystals are extremely irregular, and the ultrathin PNPC-NF possesses a honeycomb-like macroporous structure. These characteristics ensure that IrP2@PNPC-NF delivers superior NRR performance with an NH3 yield rate of 94.0 µg h−1 mg−1cat. and a faradaic efficiency (FE) of 17.8%. Density functional theory calculations reveal that the unique NRR performance originates from the low-coordinate step atoms on the edges of IrP2 nanocrystals, which can lower the reaction barrier to improve the NRR activity and simultaneously inhibit hydrogen evolution to achieve a high FE for NH3 formation. More importantly, such a plasma-assisted strategy is general and can be extended to the synthesis of other high-melting-point noble-metal phosphides (OsP2@PNPC-NF, Re3P4@PNPC-NF, etc.) with abundant step atoms at lower temperatures.

Authors


  •   Yang, Xiaohui (external author)
  •   Ling, Faling (external author)
  •   Zi, Xiangrong (external author)
  •   Zhang, Han (external author)
  •   Zhang, Huijuan (external author)
  •   Zhou, Miao (external author)
  •   Guo, Zaiping
  •   Wang, Yu (external author)

Publication Date


  • 2020

Published In


Citation


  • Yang, X., Ling, F., Zi, X., Wang, Y., Zhang, H., Zhang, H., Zhou, M., Guo, Z. & Wang, Y. (2020). Low-Coordinate Step Atoms via Plasma-Assisted Calcinations to Enhance Electrochemical Reduction of Nitrogen to Ammonia. Small,

Scopus Eid


  • 2-s2.0-85082478652

Ro Metadata Url


  • http://ro.uow.edu.au/eispapers1/3911

Place Of Publication


  • Germany

Abstract


  • © 2020 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim The electrochemical N2 reduction reaction (NRR) is emerging as a promising alternative to the industrial Haber–Bosch process for distributed and modular production of NH3. Nevertheless, developing high-efficiency catalysts to simultaneously realize both high activity and selectivity for the development of a sustainable NRR is very critical but extremely challenging. Here, a unique plasma-assisted strategy is developed to synthesize iridium diphosphide nanocrystals with abundant surface step atoms anchored in P,N-codoped porous carbon nanofilms (IrP2@PNPC-NF), where the edges of the IrP2 nanocrystals are extremely irregular, and the ultrathin PNPC-NF possesses a honeycomb-like macroporous structure. These characteristics ensure that IrP2@PNPC-NF delivers superior NRR performance with an NH3 yield rate of 94.0 µg h−1 mg−1cat. and a faradaic efficiency (FE) of 17.8%. Density functional theory calculations reveal that the unique NRR performance originates from the low-coordinate step atoms on the edges of IrP2 nanocrystals, which can lower the reaction barrier to improve the NRR activity and simultaneously inhibit hydrogen evolution to achieve a high FE for NH3 formation. More importantly, such a plasma-assisted strategy is general and can be extended to the synthesis of other high-melting-point noble-metal phosphides (OsP2@PNPC-NF, Re3P4@PNPC-NF, etc.) with abundant step atoms at lower temperatures.

Authors


  •   Yang, Xiaohui (external author)
  •   Ling, Faling (external author)
  •   Zi, Xiangrong (external author)
  •   Zhang, Han (external author)
  •   Zhang, Huijuan (external author)
  •   Zhou, Miao (external author)
  •   Guo, Zaiping
  •   Wang, Yu (external author)

Publication Date


  • 2020

Published In


Citation


  • Yang, X., Ling, F., Zi, X., Wang, Y., Zhang, H., Zhang, H., Zhou, M., Guo, Z. & Wang, Y. (2020). Low-Coordinate Step Atoms via Plasma-Assisted Calcinations to Enhance Electrochemical Reduction of Nitrogen to Ammonia. Small,

Scopus Eid


  • 2-s2.0-85082478652

Ro Metadata Url


  • http://ro.uow.edu.au/eispapers1/3911

Place Of Publication


  • Germany