Tailored p-Orbital Delocalization by Diatomic Pt-Ce Induced Interlayer Spacing Engineering for Highly-Efficient Ammonia Electrosynthesis

Dong Chen, Shaoce Zhang, Di Yin, Wanpeng Li, Xiuming Bu, Quan Quan, Zhengxun Lai, Wei Wang, You Meng, Chuntai Liu, Sen Po Yip, Fu Rong Chen, Chunyi Zhi, Johnny C. Ho

Research output: Contribution to journalArticlepeer-review

21 Citations (Scopus)

Abstract

Electrochemical nitrate reduction to ammonia (eNO3RR) is a green and appealing method for ammonia synthesis, but is hindered by the multistep chemical reaction and competitive hydrogen generation. Herein, the synthesis of 2D SnS nanosheets with tailored interlayer spacing is reported, including both expansion and compression, through the active diatomic Pt-Ce pairs. Taking together the experimental results, in situ Raman spectra, and DFT calculations, it is found that the compressed interlayer spacing can tune the electron density of localized p-orbital in Sn into its delocalized states, thus enhancing the chemical affinity towards NO3 and NO2 but inhibiting hydrogen generation simultaneously. This phenomenon significantly facilitates the rate-determining step (*NO3→*NO2) in eNO3RR, and realizes an excellent Faradaic efficiency (94.12%) and yield rate (0.3056 mmol cm−2 h−1) for NH3 at −0.5 V versus RHE. This work provides a powerful strategy for tailoring flexible interlayer spacing of 2D materials and opens a new avenue for constructing high-performance catalysts for ammonia synthesis.

Original languageEnglish
Article number2203201
JournalAdvanced Energy Materials
Volume13
Issue number6
DOIs
Publication statusPublished - Feb 10 2023

All Science Journal Classification (ASJC) codes

  • Renewable Energy, Sustainability and the Environment
  • General Materials Science

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