A physical catalyst for the electrolysis of nitrogen to ammonia

Song, Yang; Johnson, Daniel A.; Peng, Rui; Hensley, Dale K.; Bonnesen, Peter V.; Liang, Liangbo; Huang, Jingsong; Yang, Fengchang; Zhang, Fei; Qiao, Rui; Baddorf, Arthur P.; Tschaplinski, Timothy J.; Engle, Nancy L.; Hatzell, Marta C.; Wu, Zili; Cullen, David A.; Meyer, III, Harry M.; Sumpter, Bobby G.; Rondinone, Adam Justin

doi:10.1126/sciadv.1700336

Title: A physical catalyst for the electrolysis of nitrogen to ammonia

Journal Article · Fri Apr 27 00:00:00 EDT 2018 · Science Advances

DOI:https://doi.org/10.1126/sciadv.1700336· OSTI ID:1468286

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^[1]; Peng, Rui ^[1];

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^[1]; Yang, Fengchang ^[2]; Zhang, Fei ^[2];

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^[1]; Engle, Nancy L. ^[1];

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Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
Georgia Inst. of Technology, Atlanta, GA (United States)

Ammonia synthesis consumes 3 to 5% of the world’s natural gas, making it a significant contributor to greenhouse gas emissions. Strategies for synthesizing ammonia that are not dependent on the energy-intensive and methane-based Haber-Bosch process are critically important for reducing global energy consumption and minimizing climate change. Motivated by a need to investigate novel nitrogen fixation mechanisms, we herein describe a highly textured physical catalyst, composed of N-doped carbon nanospikes, that electrochemically reduces dissolved N₂ gas to ammonia in an aqueous electrolyte under ambient conditions. The Faradaic efficiency (FE) achieves 11.56 ± 0.85% at –1.19 V versus the reversible hydrogen electrode, and the maximum production rate is 97.18 ± 7.13 μg hour^–1 cm^–2. The catalyst contains no noble or rare metals but rather has a surface composed of sharp spikes, which concentrates the electric field at the tips, thereby promoting the electroreduction of dissolved N₂ molecules near the electrode. The choice of electrolyte is also critically important because the reaction rate is dependent on the counterion type, suggesting a role in enhancing the electric field at the sharp spikes and increasing N₂ concentration within the Stern layer. In conclusion, the energy efficiency of the reaction is estimated to be 5.25% at the current FE of 11.56%.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725; AC02-05CH11231

OSTI ID:: 1468286

Journal Information:: Science Advances, Vol. 4, Issue 4; ISSN 2375-2548

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 245 works

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