Electrosynthesis of chlorine from seawater-like solution through single-atom catalysts

Yangyang Liu, Can Li, Chunhui Tan, Zengxia Pei, Tao Yang, Shuzhen Zhang, Qianwei Huang, Yihan Wang, Zheng Zhou, Xiaozhou Liao, Juncai Dong, Hao Tan (), Wensheng Yan, Huajie Yin, Zhao-Qing Liu, Jun Huang () and Shenlong Zhao ()
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Yangyang Liu: National Center for Nanoscience and Technology
Can Li: China Jiliang University
Chunhui Tan: The University of Sydney
Zengxia Pei: The University of Sydney
Tao Yang: University of Aveiro
Shuzhen Zhang: The University of Sydney
Qianwei Huang: The University of Sydney
Yihan Wang: National Center for Nanoscience and Technology
Zheng Zhou: The University of Sydney
Xiaozhou Liao: The University of Sydney
Juncai Dong: Institute of High Energy Physics, Chinese Academy of Sciences
Hao Tan: University of Science and Technology of China
Wensheng Yan: University of Science and Technology of China
Huajie Yin: Chinese Academy of Sciences
Zhao-Qing Liu: Guangzhou University
Jun Huang: The University of Sydney
Shenlong Zhao: National Center for Nanoscience and Technology

Nature Communications, 2023, vol. 14, issue 1, 1-13

Abstract: 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.

Date: 2023
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DOI: 10.1038/s41467-023-38129-w

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