Author(s): RAJA, S.; SILVA, G. T. S. T. da; REIS, E. A.; CRUZ, J. C. da; SILVA, A. B.; ANDRADE, M. B.; PERIYASAMI, G.; KARTHIKEYAN, P.; PEREPICHKA, I. F.; MASCARO, L. H.; RIBEIRO, C.

Summary: ABSTRACT: Here, we show that a perylenediimide-incorporated covalent triazine framework (PDI-CTF) leads to an adequate conductive carbon support for copper single-atom catalysts (Cu-SACs), allowing the selective electroreduction of CO2 to methanol. CTF-Cu-SACs converted CO2 into methanol with a faradaic efficiency of 72.6% at a low overpotential (0.2 V vs RHE). While increasing the overpotential (0.2 to ?0.4 V vs RHE), CTF-Cu-SACs promoted syngas (CO and H2) production with faradaic efficiencies of 53.2 and 39.5%, respectively. Moreover, CTF-Cu-SACs led to robust catalytic stability for 20 h of continuous electrolysis in an aqueous solution. Notably, it was observed that additional nitrogen doping to the PDI-CTF profoundly influences product selectivity, possibly due to the synergetic effect of highly conductive pyrolyzed CTF and N-chelating ligands with rich active sites. Our results indicate that the PDI-CTF-based Cu-SACs provide abundant active sites for CO2 adsorption, thus enhancing intermolecular ion and charge transportation that efficiently reduces CO2 into methanol in an aqueous system.

Publication year: 2024

Types of publication: Journal article

Unit: Embrapa Instrumentation

Keywords: Major environmental threat