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

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Electrosynthesis of chlorine from seawater-like solution through single-atom catalysts
Nature Communications ( IF 14.7 ) Pub Date : 2023-04-29 , DOI: 10.1038/s41467-023-38129-w
Yangyang Liu _{1,

2} , Can Li ₃ , Chunhui Tan ₂ , Zengxia Pei ₂ , Tao Yang ₄ , Shuzhen Zhang ₂ , Qianwei Huang ₅ , Yihan Wang _{1,

2} , Zheng Zhou ₂ , Xiaozhou Liao ₅ , Juncai Dong ₆ , Hao Tan ₇ , Wensheng Yan ₇ , Huajie Yin ₈ , Zhao-Qing Liu ₉ , Jun Huang ₂ , Shenlong Zhao _{1,

2}

Affiliation

CAS Key Laboratory of Nanosystem and Hierarchical Fabrication, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology, Beijing, 100190, China.
School of Chemical and Biomolecular Engineering, The University of Sydney, Sydney, NSW, 2006, Australia.
Key Laboratory of Rare Earth Optoelectronic Materials and Devices of Zhejiang Province, College of Optical and Electronic Technology, China Jiliang University, Hangzhou, 310018, China.
Department of Mechanical Engineering, University of Aveiro, Aveiro, 3810-93, Portugal.
School of Aerospace, Mechanical and Mechatronic Engineering, The University of Sydney, Sydney, NSW, 2006, Australia.
Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, 100049, China.
National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230029, China.
Institute of Solid-State Physics, Chinese Academy of Sciences, Hefei, 230031, China.
School of Chemistry and Chemical Engineering/Guangzhou Key Laboratory for Clean Energy and Materials/Key Laboratory for Water Quality and Conservation of the Pearl River Delta, Ministry of Education, Guangzhou University, Guangzhou, 510006, China.

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.

中文翻译：

通过单原子催化剂从类海水溶液中电合成氯

由于氯气的广泛应用，氯碱工艺在现代化学工业中起着不可替代的重要作用。然而，目前的析氯反应 (CER) 电催化剂存在较大的过电位和较低的选择性，导致氯气生产过程中大量的能源消耗。在此，我们报道了一种高活性氧配位钌单原子催化剂，用于在类似海水的溶液中电合成氯。因此，所制备的具有 Ru-O ₄部分的单原子催化剂 (Ru-O ₄ SAM)在酸性介质 ( ^pH = 1) 含有 1 M NaCl。令人印象深刻的是，配备 Ru-O _{4 的流通池}SAM 电极在 1000 mA cm ^-2的高电流密度下，在 1000 小时的连续电催化中表现出优异的稳定性和 Cl ₂选择性。Operando 表征和计算分析表明，与基准 RuO _{2电极相比，氯离子优先吸附在 Ru-O}₄ SAM上的 Ru 原子表面，从而导致吉布斯自由能垒的降低和 Cl ₂的改善CER 期间的选择性。这一发现不仅提供了对电催化机制的基本见解，而且为从海水电催化中电化学合成氯提供了一条有前途的途径。

更新日期：2023-04-29

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