Atomically Asymmetrical Ir-O-Co Sites Enable Efficient Chloride-Mediated Ethylene Electrooxidation in Neutral Seawater.

Autor: Cai L; Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction, Ministry of Education, College of Chemistry, Central China Normal University (CCNU), Wuhan, 430079, China., Liu Y; College of Materials Science and Engineering, Fuzhou University, Fuzhou, 350108, China., Gao Y; Department of Chemistry, School of Science, Institute of Molecular Plus, Tianjin University, Tianjin, 300072, China., Zhao BH; Department of Chemistry, School of Science, Institute of Molecular Plus, Tianjin University, Tianjin, 300072, China., Guan J; Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction, Ministry of Education, College of Chemistry, Central China Normal University (CCNU), Wuhan, 430079, China., Liu X; Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction, Ministry of Education, College of Chemistry, Central China Normal University (CCNU), Wuhan, 430079, China., Zhang B; Department of Chemistry, School of Science, Institute of Molecular Plus, Tianjin University, Tianjin, 300072, China., Huang Y; Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction, Ministry of Education, College of Chemistry, Central China Normal University (CCNU), Wuhan, 430079, China.
Jazyk: angličtina
Zdroj: Angewandte Chemie (International ed. in English) [Angew Chem Int Ed Engl] 2024 Oct 25, pp. e202417092. Date of Electronic Publication: 2024 Oct 25.
DOI: 10.1002/anie.202417092
Abstrakt: The chloride-mediated ethylene oxidation reaction (EOR) of ethylene chlorohydrin (ECH) via electrocatalysis is practically attractive because of its sustainability and mild reaction conditions. However, the chlorine oxidation reaction (COR), which is essential for the above process, is commonly catalyzed by dimensionally stable anodes (DSAs) with high contents of precious Ru and/or Ir. The development of highly efficient COR electrocatalysts composed of nonprecious metals or decreased amounts of precious metals is highly desirable. Herein, we report a modified Co 3 O 4 with a single-atom Ir substitution (Ir 1 /Co 3 O 4 ) as a highly efficient COR electrocatalyst for chloride-mediated EOR to ECH in neutral seawater. Ir 1 /Co 3 O 4 achieves a Faradaic efficiency (FE) of up to 94.8 % for ECH generation and remarkable stability. Combining experimental results and density functional theory (DFT) calculations, the unique atomically asymmetrical Ir-O-Co configuration with a strong electron coupling effect in Ir1/Co 3 O 4 can accelerate electron transfer to increase the reaction kinetics and maintain the structural stability of Co 3 O 4 during COR. Moreover, a coupling reaction system integrating the anodic chloride-mediated and cathodic H 2 O 2 -mediated EOR show a total FE of ~170 % for paired electrosynthesis of ECH and ethylene glycol (EG) using ethylene as the raw material. The technoeconomic analysis highlights the promising application prospects of this system.
(© 2024 Wiley-VCH GmbH.)
Databáze: MEDLINE
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