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Perylenediimide-Incorporated Covalent Triazine Framework: A Highly Conductive Carbon Support for Copper Single-Atom Catalysts in Electrocatalytic CO2 Conversion

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Raja, Sebastian ; da Silva, Gelson T. S. T. ; Reis, Eduardo A. ; da Cruz, Jean C. ; Silva, Anelisse Brunca ; Andrade, Marcelo B. ; Periyasami, Govindasami ; Karthikeyan, Perumal ; Perepichka, Igor F. ; Mascaro, Lucia Helena ; Ribeiro, Caue
Total Authors: 11
Document type: Journal article
Source: ENERGY & FUELS; v. 37, n. 23, p. 11-pg., 2023-12-07.
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 H-2) 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. (AU)

FAPESP's process: 13/07296-2 - CDMF - Center for the Development of Functional Materials
Grantee:Elson Longo da Silva
Support Opportunities: Research Grants - Research, Innovation and Dissemination Centers - RIDC
FAPESP's process: 17/11986-5 - Generation and storage of New Energy: bringing technological development for the country
Grantee:Ana Flávia Nogueira
Support Opportunities: Research Grants - Research Centers in Engineering Program
FAPESP's process: 22/10255-5 - Architectures based on metal phosphides and nitrides for photo(electro)chemical conversion of CO2 into C2+ compounds
Grantee:Gelson Tiago dos Santos Tavares da Silva
Support Opportunities: Scholarships in Brazil - Post-Doctoral