Light-Driven Chemical Looping for Ammonia Synthesis

Dayne F. Swearer, Nicola R. Knowles, Henry O. Everitt, Naomi J. Halas*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

84 Scopus citations

Abstract

Synthetic ammonia has been the primary worldwide source of agricultural fertilizer over the last century and is a promising carbon-free energy carrier for sustainable transportation. Despite its global importance, synthetic ammonia produced with the Haber-Bosch process is extremely energy- and resource-intensive. Here we demonstrate a three-step chemical looping strategy to produce ammonia using only light, natural gas, nitrogen, and water. Titanium nitride nanoparticles were utilized as plasmonic antennas to assist the transformation of magnesium-based nanomaterials through oxide, metallic, and nitride phases under optical illumination. All reactions were performed and monitored in situ using frequency-modulated rotational spectroscopy, which allowed the experiments to take advantage of the rotational spectra's unique sensitivity to isotopic labeling to monitor and verify key reaction intermediates. This validation of a light-driven process for the synthesis of ammonia demonstrates an innovative route toward photosynthetic production of essential chemical commodities.

Original languageEnglish (US)
Pages (from-to)1505-1512
Number of pages8
JournalACS Energy Letters
Volume4
Issue number7
DOIs
StatePublished - May 31 2019

ASJC Scopus subject areas

  • Chemistry (miscellaneous)
  • Renewable Energy, Sustainability and the Environment
  • Fuel Technology
  • Energy Engineering and Power Technology
  • Materials Chemistry

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