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Title: Turning water from a hindrance to the promotor of preferential electrochemical nitrogen reduction
Authors: Koh, Charlynn Sher Lin
Lee, Hiang Kwee
Sim, Howard Yi Fan
Han, Xuemei
Phan-Quang, Gia Chuong
Ling, Xing Yi
Keywords: Science::Chemistry
Issue Date: 2020
Source: Koh, C. S. L., Lee, H. K., Sim, H. Y. F., Han, X., Phan-Quang, G. C. & Ling, X. Y. (2020). Turning water from a hindrance to the promotor of preferential electrochemical nitrogen reduction. Chemistry of Materials, 32(4), 1674-1683.
Project: RG11/18
Journal: Chemistry of Materials
Abstract: Electrochemical nitrogen reduction reaction (NRR) offers sustainable ammonia production but suffers from poor performance owing to favorable water electrolysis. Recent designs achieve better efficiency by eradicating water but do not leverage on water as a readily available NRR proton source. Herein, we design a hydrophobic oleylamine-functionalized zeolitic-imidazolate framework coated over the electrocatalyst to achieve >18% NRR efficiency in the presence of water, an approximately fourfold boost compared to that without water. Our strategy kinetically regulates water availability at the electrocatalyst surface, suppresses direct water adsorption/electrolysis, and promotes preferential nitrogen adsorption to achieve water-assisted NRR. Conversely, control systems without hydrophobic modification experience a drastic decrease in efficiencies (<3%) upon water addition. In situ surface-enhanced Raman scattering investigation reveals that our hydrophobic system's ability in suppressing water accessibility to the electrocatalyst is the key to transform water from a hindrance to an NRR promotor. Our universal design is a paradigm shift from current approaches to achieve sustainable air-to-ammonia electrosynthesis.
ISSN: 0897-4756
DOI: 10.1021/acs.chemmater.9b05313
Rights: © 2020 American Chemical Society. All rights reserved.
Fulltext Permission: none
Fulltext Availability: No Fulltext
Appears in Collections:SPMS Journal Articles

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