Surface Plasmon Enabling Nitrogen Fixation in Pure Water through a Dissociative Mechanism under Mild Conditions

Canyu Hu, Xing Chen, Jianbo Jin, Yong Han, Shuangming Chen, Huanxin Ju, Jun Cai, Yunrui Qiu, Chao Gao, Chengming Wang, Zeming Qi, Ran Long, Li Song, Zhi Liu, Yujie Xiong

Research output: Contribution to journalArticlepeer-review

75 Scopus citations

Abstract

Nitrogen fixation in a simulated natural environment (i.e., near ambient pressure, room temperature, pure water, and incident light) would provide a desirable approach to future nitrogen conversion. As the NN triple bond has a thermodynamically high cleavage energy, nitrogen reduction under such mild conditions typically undergoes associative alternating or distal pathways rather than following a dissociative mechanism. Here, we report that surface plasmon can supply sufficient energy to activate N2 through a dissociative mechanism in the presence of water and incident light, as evidenced by in situ synchrotron radiation-based infrared spectroscopy and near ambient pressure X-ray photoelectron spectroscopy. Theoretical simulation indicates that the electric field enhanced by surface plasmon, together with plasmonic hot electrons and interfacial hybridization, may play a critical role in NN dissociation. Specifically, AuRu core-antenna nanostructures with broadened light adsorption cross section and active sites achieve an ammonia production rate of 101.4 μmol g-1 h-1 without any sacrificial agent at room temperature and 2 atm pressure. This work highlights the significance of surface plasmon to activation of inert molecules, serving as a promising platform for developing novel catalytic systems.

Original languageEnglish (US)
Pages (from-to)7807-7814
Number of pages8
JournalJournal of the American Chemical Society
Volume141
Issue number19
DOIs
StatePublished - May 15 2019

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

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