Metal-organic framework-derived nitrogen-doped highly disordered carbon for electrochemical ammonia synthesis using N2 and H2O in alkaline electrolytes

Mukherjee, Shreya; Cullen, David A.; Karakalos, Stavros; Liu, Kexi; Zhang, Hao; Zhao, Shuai; Xu, Hui; More, Karren Leslie; Wang, Guofeng; Wu, Gang

doi:10.1016/j.nanoen.2018.03.059

Title: Metal-organic framework-derived nitrogen-doped highly disordered carbon for electrochemical ammonia synthesis using N₂ and H₂O in alkaline electrolytes

Journal Article · Fri Mar 23 00:00:00 EDT 2018 · Nano Energy

DOI:https://doi.org/10.1016/j.nanoen.2018.03.059· OSTI ID:1440813

Mukherjee, Shreya ^[1];

^[2]; Karakalos, Stavros ^[3]; Liu, Kexi ^[4]; Zhang, Hao ^[1]; Zhao, Shuai ^[5]; Xu, Hui ^[5];

^[2]; Wang, Guofeng ^[4]; Wu, Gang ^[1]

Univ. at Buffalo, The State Univ. of New York, Buffalo, NY (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Univ. of South Carolina, Columbia, SC (United States)
Univ. of Pittsburgh, Pittsburgh, PA (United States)
Giner Inc., Newton, MA (United States)

Ammonia (NH₃) is considered an important chemical for both agriculture fertilizer and renewable energy. The conventional Haber-Bosh process to produce NH₃ is energy intensive and leads to significant CO₂ emission. Alternatively, electrochemical synthesis of ammonia (ESA) through the nitrogen reduction reaction (NRR) by using renewable electricity has recently attracted significant attention. Herein, we report a metal-organic framework-derived nitrogen-doped nanoporous carbon as an electrocatalyst for the NRR. It exhibits a remarkable production rate of NH₃ up to 3.4 ×10^–6 mol cm^–2 h^–1 with a Faradaic efficiency (FE) of 10.2% at –0.3 V vs. RHE under room temperature and ambient pressure using aqueous 0.1 M KOH electrolyte. Increasing the temperature to 60 °C further improves production rates to 7.3 × 10^–6 mol cm^–2 h^–1. The stability of the nitrogen-doped carbon electrocatalyst was demonstrated during an 18-h continuous test with constant production rates. First principles calculations were used to elucidate the possible active sites and reaction pathway. The moiety, which consists of three pyridinic N atoms (N₃) adjacent with one carbon vacancy embedded in a carbon layer, is able to strongly adsorb N₂ and further realize N≡N triple bond dissociation for the subsequent protonation process. The rate-determining step of the NRR is predicted to be the adsorption and bond activation of N₂ molecule. Increasing overpotentials is favorable for the protonation process during NH₃ generation. Further doping Fe into the nitrogen-doped carbon likely blocks the N₃ active sites and facilitates the hydrogen evolution reaction, a strong competitor to the NRR, thus yielding negative effect on ammonia production. Furthermore, this work provides a new insight into the rational design and synthesis of nitrogen-doped and defect-rich carbon as efficient NRR catalysts for NH₃ synthesis at ambient conditions.

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

Sponsoring Organization:: USDOE Advanced Research Projects Agency - Energy (ARPA-E)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1440813

Alternate ID(s):: OSTI ID: 1496459

Journal Information:: Nano Energy, Vol. 48, Issue C; ISSN 2211-2855

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 316 works

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