A One‐Pot Three‐In‐One Synthetic Strategy to Immobilize Cobalt Corroles on Carbon Nanotubes for Oxygen Electrocatalysis

Abstract

Molecular electrocatalysis requires the immobilization of molecular catalysts on electrode materials for practical uses. Direct adsorption of catalyst molecules on electrode materials is simple, but grafting molecules through chemical bonds can significantly improve electrocatalytic efficiency and durability. However, designing and synthesizing catalyst molecules to simultaneously improve catalytic activities and realize easy grafting on electrodes is challenging. The study herein reports on a one‐pot strategy to graft Co corroles on pyridine‐modified carbon nanotubes (CNTs) for oxygen electrocatalysis. By modifying CNTs with pyridines, the resulting pyridine‐modified CNTs can function as platforms to grab in situ generated Co corroles through the axial pyridine ligation on Co. Such an immobilization strategy combines three effects for the regulation of electrocatalysis, including the axial ligand effect, the electron transfer effect, and the chemical bond effect. The resulting hybrid materials show high efficiency for oxygen electrocatalysis, and the Zn–air battery assembled using these materials displays comparable performance as the Pt/Ir‐based battery. Moreover, the electrocatalytic efficiency of these hybrid materials can be systematically tuned by using different pyridines, highlighting the controllable feature of this strategy. Therefore, this work is significant to present a one‐pot three‐in‐one strategy to immobilize catalyst molecules on CNTs for electrocatalysis.

Molecular palladium catalyst enabling efficient electrochemical C–C bond cleavage within lignin model compounds

“…23 Furthermore, these molecular catalysts frequently induce disparate reaction pathways and result in enhanced catalytic performance as demonstrated in various electrocatalysis conversions. 24–31 Hence, molecular catalysts hold enormous promise for augmenting selectivity in the electrochemical cleavage of C–C bonds within lignin. Nonetheless, molecular catalysts have yet to be explored as electrocatalysts for lignin conversion.…”

Covalent Tethering of Cobalt Porphyrins on Phenolic Resins for Electrocatalytic Oxygen Reduction and Evolution Reactions

“…Carbon based materials, including carbon nanotube, [54–56] carbon black, [57,58] and graphene, [59–61] have been generally used as the supporting materials. Although loading molecular electrocatalysts on these supporting materials through simple physical adsorption is straightforward, our recent works demonstrated that covalent tethering of molecular electrocatalysts on supporting materials can significantly improve their efficiency and durability for electrocatalysis [62,63] . However, because of their high chemical stability, carbon‐based materials are in general difficult to be functionalized for covalent tethering of molecular electrocatalysts.…”

Metal-free corrole-based donor–acceptor porous organic polymers as efficient bifunctional catalysts for hydrogen evolution and oxygen reduction reactions

“…19–21 The unique structures of corroles not only make them possess attractive coordination capabilities and specific reactivities but also make them ideal acceptors in D–A systems. 22–29 Not only that, functionalized corroles, such as 5,10,15-tris( p -aminophenyl)corrole (TPAPC), can be further used as acceptors to construct novel D–A systems. 20–23,30 Furthermore, corroles usually possess small HOMO–LUMO gaps that cause electrons to be easily adsorbed and released, permitting rapid electron transfer to reactants and enhancing electrocatalytic activities.…”