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Title: Favoring the unfavored : selective electrochemical nitrogen fixation using a reticular chemistry approach
Authors: Lee, Hiang Kwee
Koh, Charlynn Sher Lin
Lee, Yih Hong
Liu, Chong
Phang, In Yee
Han, Xuemei
Tsung, Chia-Kuang
Ling, Xing Yi
Keywords: Nitrogen Reduction Reaction (NRR)
Hydrogen Evolution Reaction (HER)
Issue Date: 2018
Source: Lee, H. K., Koh, C. S. L., Lee, Y. H., Liu, C., Phang, I. Y., Han, X., et al. (2018). Favoring the unfavored : selective electrochemical nitrogen fixation using a reticular chemistry approach. Science Advances, 4(3), eaar3208-.
Series/Report no.: Science Advances
Abstract: Electrochemical nitrogen-to-ammonia fixation is emerging as a sustainable strategy to tackle the hydrogen- and energy-intensive operations by Haber-Bosch process for ammonia production. However, current electrochemical nitrogen reduction reaction (NRR) progress is impeded by overwhelming competition from the hydrogen evolution reaction (HER) across all traditional NRR catalysts and the requirement for elevated temperature/pressure. We achieve both excellent NRR selectivity (~90%) and a significant boost to Faradic efficiency by 10 percentage points even at ambient operations by coating a superhydrophobic metal-organic framework (MOF) layer over the NRR electrocatalyst. Our reticular chemistry approach exploits MOF’s water-repelling and molecular-concentrating effects to overcome HER-imposed bottlenecks, uncovering the unprecedented electrochemical features of NRR critical for future theoretical studies. By favoring the originally unfavored NRR, we envisage our electrocatalytic design as a starting point for high-performance nitrogen-to-ammonia electroconversion directly from water vapor–abundant air to address increasing global demand of ammonia in (bio)chemical and energy industries.
DOI: 10.1126/sciadv.aar3208
Rights: © 2018 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC). This is an open-access article distributed under the terms of the Creative Commons Attribution-NonCommercial license, which permits use, distribution, and reproduction in any medium, so long as the resultant use is not for commercial advantage and provided the original work is properly cited.
Fulltext Permission: open
Fulltext Availability: With Fulltext
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