Journal
SCIENCE
Volume 372, Issue 6547, Pages 1187-+Publisher
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.abg2371
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Funding
- Australian Renewable Energy Agency [2018/RND009 DM015]
- Australian Research Council (Centre of Excellence in Electromaterials Science) [CE140100012, DP200101878, FT200100317]
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Ammonia (NH3) is a globally important commodity for fertilizer production, but its synthesis by the Haber-Bosch process causes substantial emissions of carbon dioxide. Alternative methods being explored include the promising electrochemical lithium-mediated nitrogen reduction reaction, which has required sacrificial sources of protons. In this study, a phosphonium salt is introduced as a proton shuttle to help resolve this limitation, resulting in high NH3 production rates and demonstrated continuous operation for more than 3 days.
Ammonia (NH3) is a globally important commodity for fertilizer production, but its synthesis by the Haber-Bosch process causes substantial emissions of carbon dioxide. Alternative, zero-carbon emission NH3 synthesis methods being explored include the promising electrochemical lithium-mediated nitrogen reduction reaction, which has nonetheless required sacrificial sources of protons. In this study, a phosphonium salt is introduced as a proton shuttle to help resolve this limitation. The salt also provides additional ionic conductivity, enabling high NH3 production rates of 53 +/- 1 nanomoles per second per square centimeter at 69 +/- 1% faradaic efficiency in 20-hour experiments under 0.5-bar hydrogen and 19.5-bar nitrogen. Continuous operation for more than 3 days is demonstrated.
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