Concurrent Mechanisms of Hot Electrons and Interfacial Water Molecule Ordering in Plasmon-Enhanced Nitrogen Fixation

Shaoce ZHANG, Dong CHEN, Peigang CHEN, Rong ZHANG, Yue HOU, Ying GUO, Pei LI, Xiu LIANG, Tingyang XING, Jie CHEN, Yuwei ZHAO, Zhaodong HUANG, Dangyuan LEI, Chunyi ZHI

Research output: Journal PublicationsJournal Article (refereed)peer-review

3 Citations (Scopus)

Abstract

The participation of high-energy hot electrons generated from the non-radiative decay of localized surface plasmons is an important mechanism for promoting catalytic processes. Herein, another vital mechanism associated with the localized surface plasmon resonance (LSPR) effect, significantly contributing to the nitrogen reduction reaction (NRR), is found. That is to say, the LSPR-induced strong localized electric fields can weaken the intermolecular hydrogen bonds and regulate the arrangement of water molecules at the solid–liquid interface. The AuCu pentacle nanoparticles with excellent light absorption ability and the capability to generate strong localized electric fields are chosen to demonstrate this effect. The in situ Raman spectra and theoretical calculations are employed to verify the mechanism at the molecular scale in a nitrogen fixation process. Meanwhile, due to the promoted electron transfer at the interface by the well-ordered interfacial water, as well as the participation of high-energy hot electrons, the optimal catalyst exhibits excellent performance with an NH3 yield of 52.09 µg h−1 cm−2 and Faradaic efficiency (FE) of 45.82% at ─0.20 V versus RHE. The results are significant for understanding the LSPR effect in catalysis and provide a new approach for regulating the reaction process.

Original languageEnglish
Article number2310776
JournalAdvanced Materials
Volume36
Issue number15
Early online date17 Jan 2024
DOIs
Publication statusPublished - 11 Apr 2024
Externally publishedYes

Bibliographical note

This work was supported by a grant from the Research Grants Council of the Hong Kong Special Administrative Region, China [Project No. T23‐713/22‐R]. D.L. is thankful for the funding support from the National Natural Science Foundation of China through the Excellent Young Scientists Fund (Hong Kong and Macau) (62022001) and the Hong Kong Branch of National Precious Metals Material Engineering Research Center (ITC Fund).

Publisher Copyright:
© 2024 The Authors. Advanced Materials published by Wiley-VCH GmbH.

Keywords

  • AuCu pentacle nanoparticle
  • localized surface plasmon resonance
  • nitrogen fixation
  • well-ordered water molecules

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