Abstract
Single-atom electrocatalysts (SACs), which comprise singly isolated metal sites supported on heterogeneous substrates, have attracted considerable recent attention as next-generation electrocatalysts for various key reactions from the viewpoint of the environment and energy. Not only electrocatalytic activity but also selectivity can be precisely tuned via the construction of SACs with a defined coordination structure, such as homogeneous organometallics. Covalent organic frameworks (COFs) are promising supports for single-atom sites with designed coordination environments due to their unique physicochemical properties, which include porous structures, robustness, a wide range of possible designs, and abundant heteroatoms to coordinate single-metal sites. The rigid frameworks of COFs can hold unstable single-metal atoms, such as coordinatively unsaturated sites or easily aggregated Pt-group metals, which exhibit unique electrocatalytic selectivity. This minireview summarizes recent advances in the selective reactions catalysed by SACs, mainly those supported on triazine-based COFs.
Highlights
Electrochemical devices are attracting increasing attention in applications such as batteries,[1] arti cial photosynthesis,[2] and Kazuhide Kamiya received his PhD degree from the University of Tokyo under the supervision of Prof
An electrocatalytic durability test of the Ni-CTF for the carbon dioxide reduction reaction (CRR) revealed that the decrease in faradaic efficiency (FE) for CO production was almost negligible during 3 h of electrolysis, whereas the cathodic current slowly decreased.[65]
We introduced the selective electrocatalytic properties of SACs, with particular focus on triazinebased Covalent organic frameworks (COFs) as supports
Summary
Kazuhide Kamiya received his PhD degree from the University of Tokyo under the supervision of Prof. Fe- or Cobased N4 macrocycles, in particular, have been reported to efficiently catalyse the reduction of CO2 to CO and methane.[61,62] On the basis of these reports, Lin et al synthesized new COFs comprising Co porphyrin units as CO evolution catalysts.[63] In contrast to these Co–N4 compounds, Cu- or Ni-macrocycles are known to exhibit poor activity toward CO generation from CO2 because they weakly bind COOH, the key intermediate for CO.[61,64] the choice of an appropriate metal species for electrocatalytic reactions from the viewpoint of adsorption strength of the substrate and/or intermediates is clearly important.
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