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| Author(s): |
Rafael Luiz Romano
Total Authors: 1
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| Document type: | Doctoral Thesis |
| Press: | São Carlos. |
| Institution: | Universidade de São Paulo (USP). Instituto de Química de São Carlos (IQSC/BT) |
| Defense date: | 2025-09-17 |
| Examining board members: |
Fabio Henrique Barros de Lima;
Cauê Ribeiro de Oliveira;
Lucia Helena Mascaro Sales;
Raphael Nagao de Sousa
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| Advisor: | Fabio Henrique Barros de Lima |
| Abstract | |
The Electrochemical Reduction of CO2 (RECO2) enables the production of several products of commercial interest. However, the use of the RECO2 in practical devices is limited by the high required overpotentials and poor selectivity. Therefore, efforts have been directed towards the development of more active, selective and stable electrocatalysts. In this work, the electrocatalytic properties of water-insoluble copper complexes were studied for the RECO2. Particularly, [Cu(bzimpy)Cl2] and [Cu(pyrben)2(NO3)]NO3 were considered, where bzimpy and pyrben refer to the ligands 2,6-bis(2-benzimidazolyl)pyridine and 2-(2-pyridyl)benzimidazole, respectively. Both complexes were found to be active for RECO2, promoting the formation of up to 7 products at -1.24 V vs. RHE: H2, CO, CH4, C2H4, C2H5OH, HCOOH and CH3COOH. In-situ X-ray absorption spectroscopy and lead underpotential deposition measurements suggested that the active sites for RECO2 are formed by undercoordinated Cu0 species, showing the (100) plan as the dominant facet, which is in line with the high faradaic efficiency towards C2 products (~45%) shown by both complexes at -1,24 V. Through spectroscopy experiments and quantitative product analyses, it was shown that [Cu(bzimpy)Cl2] should present a partially reversible restructuring under anodic conditions, regenerating the main complex moiety, [Cu(bzimpy)]2+, and its geometry. (AU) | |
| FAPESP's process: | 21/03263-9 - Electrochemical CO2 Reduction to C1 and C2 Products on Catalysts Made up of Copper Complexes with Potential Dynamic Behavior between Cu2-Ligand and Metallic Cu |
| Grantee: | Rafael Luiz Romano |
| Support Opportunities: | Scholarships in Brazil - Doctorate |