Journal
SMALL
Volume 16, Issue 25, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.202000955
Keywords
CO2 reduction; ethylene production; immobilization; mesoporous carbon; molecular copper complex
Categories
Funding
- Creative Materials Discovery Program through the National Research Foundation of Korea (NRF) - Ministry of Science and ICT [NRF-2017M3D1A1039377]
- Global Frontier R&D Program of the Center for Multiscale Energy System - National Research Foundation under the Ministry of Science and ICT, Korea [2012M3A6A7054855]
- National Research Foundation of Korea (NRF) - Korea government (MSIT) [NRF-2017R1A2B3012003]
- KIST-SNU Joint Research Lab project under the KIST Institutional Program by the Korea government (Ministry of Science and ICT) [2V06170]
- BK21PLUS SNU Materials Division for Educating Creative Global Leaders [21A20131912052]
- Research Institute of Advanced Materials (RIAM) and Soft Foundry at Seoul National University
- Institute of Engineering Research
- National Research Council of Science & Technology (NST), Republic of Korea [C030370] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
- National Research Foundation of Korea [2012M3A6A7054855] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
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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.
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