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

• Tipo de documento: Artigo Científico
• Fonte: ENERGY & FUELS; v. 37, n. 23, p. 11-pg., 2023-12-07.

Resumo

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)

• Processo FAPESP: 13/07296-2 - CDMF - Centro de Desenvolvimento de Materiais Funcionais
• Beneficiário: Elson Longo da Silva
• Modalidade de apoio: Auxílio à Pesquisa - Centros de Pesquisa, Inovação e Difusão - CEPIDs
• Processo FAPESP: 17/11986-5 - Geração e Armazenamento de Novas Energias: trazendo desenvolvimento tecnológico para o país
• Beneficiário: Ana Flávia Nogueira
• Modalidade de apoio: Auxílio à Pesquisa - Programa Centros de Pesquisa em Engenharia
• Processo FAPESP: 22/10255-5 - Arquiteturas baseadas em fosfetos e nitretos metálicos para conversão foto(eletro)química de CO2 em compostos C2+
• Beneficiário: Gelson Tiago dos Santos Tavares da Silva
• Modalidade de apoio: Bolsas no Brasil - Pós-Doutorado