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Title: Enabling electrochemical N2 reduction to NH3 in the low overpotential region using non-noble metal Bi electrodes via surface composition modification

Abstract

The electrochemical N2 reduction reaction (ENRR) that can produce NH3 using water as the hydrogen source at ambient temperature and pressure can be an exciting alternative to the Haber–Bosch process. The major challenge for electrochemical NH3 production is the competing hydrogen evolution reaction (HER), which seriously limits the faradaic efficiency (FE) for NH3 production. To date, noble metal electrocatalysts that are inactive for the HER have mainly been investigated for the ENRR. Studies reporting a FE greater than 10% for NH3 production using non-noble metal catalysts in the low overpotential region (E ≤ 0.2 V vs. RHE) are very rare. This study reports effective electrochemical surface modification strategies that drastically increase the ENRR activity of a non-noble Bi electrode in the low overpotential region and achieve a FE for NH3 production as high as 13.2% at -0.2 V vs. RHE in pH 7.5 phosphate buffer. Finally, the effect of each of the surface modifications on the activity for the ENRR and the electrode stability during the ENRR were systematically elucidated, which may be used to develop general strategies to enhance the ENRR activities of other non-noble metal electrodes in the low overpotential region.

Authors:
ORCiD logo [1]; ORCiD logo [2]
  1. Univ. of Wisconsin, Madison, WI (United States); Univ. of Hanyang, Seoul (Korea, Republic of)
  2. Univ. of Wisconsin, Madison, WI (United States)
Publication Date:
Research Org.:
Univ. of Wisconsin, Madison, WI (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; USDOE
OSTI Identifier:
1801875
Alternate Identifier(s):
OSTI ID: 1637379
Grant/Contract Number:  
SC0008707
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Materials Chemistry. A
Additional Journal Information:
Journal Volume: 8; Journal Issue: 27; Journal ID: ISSN 2050-7488
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Chemistry; Energy & Fuels; Materials Science

Citation Formats

Jang, Youn Jeong, and Choi, Kyoung-Shin. Enabling electrochemical N2 reduction to NH3 in the low overpotential region using non-noble metal Bi electrodes via surface composition modification. United States: N. p., 2020. Web. doi:10.1039/d0ta02550j.
Jang, Youn Jeong, & Choi, Kyoung-Shin. Enabling electrochemical N2 reduction to NH3 in the low overpotential region using non-noble metal Bi electrodes via surface composition modification. United States. https://doi.org/10.1039/d0ta02550j
Jang, Youn Jeong, and Choi, Kyoung-Shin. Mon . "Enabling electrochemical N2 reduction to NH3 in the low overpotential region using non-noble metal Bi electrodes via surface composition modification". United States. https://doi.org/10.1039/d0ta02550j. https://www.osti.gov/servlets/purl/1801875.
@article{osti_1801875,
title = {Enabling electrochemical N2 reduction to NH3 in the low overpotential region using non-noble metal Bi electrodes via surface composition modification},
author = {Jang, Youn Jeong and Choi, Kyoung-Shin},
abstractNote = {The electrochemical N2 reduction reaction (ENRR) that can produce NH3 using water as the hydrogen source at ambient temperature and pressure can be an exciting alternative to the Haber–Bosch process. The major challenge for electrochemical NH3 production is the competing hydrogen evolution reaction (HER), which seriously limits the faradaic efficiency (FE) for NH3 production. To date, noble metal electrocatalysts that are inactive for the HER have mainly been investigated for the ENRR. Studies reporting a FE greater than 10% for NH3 production using non-noble metal catalysts in the low overpotential region (E ≤ 0.2 V vs. RHE) are very rare. This study reports effective electrochemical surface modification strategies that drastically increase the ENRR activity of a non-noble Bi electrode in the low overpotential region and achieve a FE for NH3 production as high as 13.2% at -0.2 V vs. RHE in pH 7.5 phosphate buffer. Finally, the effect of each of the surface modifications on the activity for the ENRR and the electrode stability during the ENRR were systematically elucidated, which may be used to develop general strategies to enhance the ENRR activities of other non-noble metal electrodes in the low overpotential region.},
doi = {10.1039/d0ta02550j},
journal = {Journal of Materials Chemistry. A},
number = 27,
volume = 8,
place = {United States},
year = {Mon Jul 06 00:00:00 EDT 2020},
month = {Mon Jul 06 00:00:00 EDT 2020}
}

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