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

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.

Unveiling the Oxygen Evolution Mechanism with FeNi (Hydr)oxide under Neutral Conditions

“…The anodization strategy of FeNi foam, similar to other new strategies, – with a Ni:Fe ratio of 1:1, in phosphate buffer for OER, presents a promising avenue for scientific exploration. This approach offers numerous advantages, including the prepared electrode’s stability and efficiency toward OER and the cost-effectiveness and abundance of Ni and Fe.…”

Reaction between Nickel Hydroxide and Cerium(IV) Ammonium Nitrate in Aqueous Solution

“…Knowledge of the WOR mechanism can inform the development of sustainable energy technologies by providing insight into efficient methods for converting solar energy into chemical energy. − Additionally, the WOR mechanism is crucial for understanding the process of photosynthesis in plants, which is responsible for generating oxygen and reducing carbon dioxide in the atmosphere …”

Insight into the Dynamic Evolution of Supported Metal Catalysts by In Situ/Operando Techniques and Theoretical Simulations

“…The methods to improve the internal triggers mainly occur in the synthesis stage of catalysts, such as doping atoms, construction defects and so on. The external conditions induce the catalysts evolving real active sites during reaction, which is the focus of this paper. , Reactants, intermediates and products, as substances that interact directly with the catalysts, can provide the driving force for dynamic evolution of the catalyst surface. CO as a kind of reducing gas can induce the reconstruction of active metal species in the Rh-, Pt-, Au-, and Cu-based supported catalysts .…”