Electrocatalytic Reduction of CO2 to Ethylene by Molecular Cu‐Complex Immobilized on Graphitized Mesoporous Carbon. Issue 25 (28th May 2020)

• Record Type: Journal Article
• Authors: Balamurugan, Mani; Jeong, Hui‐Yun; Choutipalli, Venkata Surya Kumar; Hong, Jung Sug; Seo, Hongmin; Saravanan, Natarajan; Jang, Jun Ho; Lee, Kang‐Gyu; Lee, Yoon Ho; Im, Sang Won; Subramanian, Venkatesan; Kim, Sun Hee; Nam, Ki Tae
• Is Part Of: Small. Volume 16:Issue 25(2020)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2020-05-28
• Subjects: CO2 reduction -- ethylene production -- immobilization -- mesoporous carbon -- molecular copper complex; Nanotechnology -- Periodicals; Nanoparticles -- Periodicals; Microtechnology -- Periodicals; 620.5
• DOI: 10.1002/smll.202000955
• Languages: English
• ISSNs: 1613-6810

Abstract

Abstract: The electrochemical reduction of carbon dioxide (CO2 ) to hydrocarbons is a challenging task because of the issues in controlling the efficiency and selectivity of the products. Among the various transition metals, copper has attracted attention as it yields more reduced and C2 products even while using mononuclear copper center as catalysts. In addition, it is found that reversible formation of copper nanoparticle acts as the real catalytically active site for the conversion of CO2 to reduced products. Here, it is demonstrated that the dinuclear molecular copper complex immobilized over graphitized mesoporous carbon can act as catalysts for the conversion of CO2 to hydrocarbons (methane and ethylene) up to 60%. Interestingly, high selectivity toward C2 product (40% faradaic efficiency) is achieved by a molecular complex based hybrid material from CO2 in 0.1 m KCl. In addition, the role of local pH, porous structure, and carbon support in limiting the mass transport to achieve the highly reduced products is demonstrated. Although the spectroscopic analysis of the catalysts exhibits molecular nature of the complex after 2 h bulk electrolysis, morphological study reveals that the newly generated copper cluster is the real active site during the catalytic reactions. Abstract : Dinuclear copper complex immobilized on graphitized mesoporous carbon exhibits more efficient CO2 reduction activity than that of the mononuclear composite material. Although postcatalytic analysis of the material displays the existence of molecular nature, morphological study shows copper clustering as the real active site. The importance of porous structure, substrate, and controlling the local pH in C2 product selectivity is demonstrated.