A variety of carbon materials such as carbon nanotubes and graphene have been widely investigated as conductive substrates to immobilize metal complex-based catalysts for electrocatalytic CO2 reduction. However, highly ordered mesoporous carbons have received scant attention as substrates for CO2 reduction electrocatalysts. The unique porous structure of such carbon provides the opportunity to not only house catalytically active materials but also facilitate reactant transport. In this work, we propose a simple approach for immobilization of the highly active and cost-efficient molecular catalyst iron porphyrin, into a highly ordered mesoporous carbon, CMK-3 having a large surface area of 1345 m2 g-1via a simple vacuum infiltration method. The resulting heterogeneous electrocatalyst (CMK-FeTPP) is utilized for the conversion of aqueous CO2 into CO with 92.1% faradaic efficiency and a high effective turnover frequency of 3.9 s-1 at an overpotential of 680 mV. We believe that this new approach has the potential to be widely used to fabricate efficient electrocatalysts for not only CO2 conversion but also other electrochemical gas conversion systems.
Bibliographical noteFunding Information:
This work was supported by the ARC Centre of Excellence Scheme (Project Number CE 140100012). JC also thanks the University of Wollongong (UOW) for a University Postgraduate Award. The authors thank Dr Patricia Hayes for assistance with Raman spectroscopy, and the Materials Node of the Australian National Fabrication Facility (ANFF) and the UOW Electron Microscopy Centre for their facilities and research support. This study was also supported by a National Research Foundation of Korea (NRF) grant funded by the Korean government (MSIP) (No. 2020R1C1C1004459, 2017M3A7B4041987, and No. 2016R1A5A1012966). We also appreciate Prof. Toru Waki-hara's helpful discussion for this paper. This research work was supported by the Foundation for Australia-Japan Studies (FAJS) and partly performed at the Queensland node of the Australian National Fabrication Facility (ANFF), a company established under the National Collaborative Research Infrastructure Strategy to provide nano-and microfabrication facilities for Australian researchers.
© The Royal Society of Chemistry.
All Science Journal Classification (ASJC) codes
- Renewable Energy, Sustainability and the Environment
- Materials Science(all)