Electrosynthesis of chlorine from seawater-like solution through single-atom catalysts
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Li, C
Tan, C
Pei, Z
Yang, T
Zhang, S
Huang, Q
Wang, Y
Zhou, Z
Liao, X
Dong, J
Tan, H
Yan, W
Yin, H
Liu, ZQ
et al.
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Abstract
The chlor-alkali process plays an essential and irreplaceable role in the modern chemical industry due to the wide-ranging applications of chlorine gas. However, the large overpotential and low selectivity of current chlorine evolution reaction (CER) electrocatalysts result in significant energy consumption during chlorine production. Herein, we report a highly active oxygen-coordinated ruthenium single-atom catalyst for the electrosynthesis of chlorine in seawater-like solutions. As a result, the as-prepared single-atom catalyst with Ru-O4 moiety (Ru-O4 SAM) exhibits an overpotential of only ~30 mV to achieve a current density of 10 mA cm−2 in an acidic medium (pH = 1) containing 1 M NaCl. Impressively, the flow cell equipped with Ru-O4 SAM electrode displays excellent stability and Cl2 selectivity over 1000 h continuous electrocatalysis at a high current density of 1000 mA cm−2. Operando characterizations and computational analysis reveal that compared with the benchmark RuO2 electrode, chloride ions preferentially adsorb directly onto the surface of Ru atoms on Ru-O4 SAM, thereby leading to a reduction in Gibbs free-energy barrier and an improvement in Cl2 selectivity during CER. This finding not only offers fundamental insights into the mechanisms of electrocatalysis but also provides a promising avenue for the electrochemical synthesis of chlorine from seawater electrocatalysis.
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Nature Communications
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14
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© The Author(s) 2023. Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.
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Analytical chemistry
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Liu, Y; Li, C; Tan, C; Pei, Z; Yang, T; Zhang, S; Huang, Q; Wang, Y; Zhou, Z; Liao, X; Dong, J; Tan, H; Yan, W; Yin, H; Liu, ZQ; Huang, J; Zhao, S, Electrosynthesis of chlorine from seawater-like solution through single-atom catalysts, Nature Communications, 2023, 14, pp. 2475