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Solar-driven CO2 conversion to methane and methanol using different nanostructured Cu2O-based catalysts modified with Au nanoparticles

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Author(s):
Lima Perini, Joao Angelo ; Moura Torquato, Lilian D. ; de Brito, Juliana F. ; Andolpho, Gustavo A. ; Gonsalves, Mateus A. ; De Angelis, Leonardo D. ; Germano, Lucas D. ; Cordoba de Torresi, Susana I. ; Ramalho, Teodorico C. ; Boldrin Zanoni, Maria V.
Total Authors: 10
Document type: Journal article
Source: JOURNAL OF ENERGY CHEMISTRY; v. 91, p. 12-pg., 2024-01-24.
Abstract

This work describes the use of TiO2 nanotubes-based electrodes (TNT) modified with Cu2O nanostructures and gold nanoparticles for the photoelectroreduction of CO2 to produce value-added compounds. A thin layer of polydopamine was used as both an adherent agent and an electron transfer mediator, due to its p-conjugated electron system. The highest production yield was achieved using a TNT@PDA/ Nc/Au40% electrode, with Faradaic efficiencies of 47.4% (110.5 lM cm2) and 27.8% (50.4 lM cm-2) for methanol and methane, respectively. The performance of the photoelectrodes was shown to be Cu2O facet-dependent, with cubic structures leading to greater conversion of CO2 to methanol (43%) and methane (27%), compared to the octahedral morphology, while a higher percentage of metallic gold on the nanostructured Cu2O surface was mainly important for CH4 production. Density functional theory (DFT) calculations supported these findings, attributing the superior photoelectrocatalytic performance of the TNT@PDA/Nc/Au40% electrode for CH4 generation to the formation of an OCH3 intermediate bonded to Au atoms. Studies using isotope-labeling and analysis by gas chromatograph-mass (GC-MS) demonstrated that 13CO2 was the source for photoelectrocatalytic generation of 13CH3OH and 13CH313CH2OH. (c) 2023 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved. (AU)

FAPESP's process: 21/08007-0 - Study of CO2 plasmon-assisted electroreduction over Cu2O-Au nanostructures towards C2 compounds synthesis
Grantee:Leonardo Domenico De Angelis
Support Opportunities: Scholarships in Brazil - Doctorate (Direct)
FAPESP's process: 20/15230-5 - Research Centre for Greenhouse Gas Innovation - RCG2I
Grantee:Julio Romano Meneghini
Support Opportunities: Research Grants - Research Centers in Engineering Program
FAPESP's process: 14/50945-4 - INCT 2014: National Institute for Alternative Technologies of Detection, Toxicological Evaluation and Removal of Micropollutants and Radioactivies
Grantee:Maria Valnice Boldrin
Support Opportunities: Research Projects - Thematic Grants
FAPESP's process: 19/00463-7 - Integrated and solar-driven bioelectrochemical systems for electricity and H2 production from co-digestion of crude glycerol and wastewater from citrus processing industry
Grantee:Lilian Danielle de Moura Torquato
Support Opportunities: Scholarships in Brazil - Post-Doctoral
FAPESP's process: 18/22845-6 - Controlled nanostructures based on metal hidroxides and noble metals applied to electrocatalytic of oxygen evolution reaction
Grantee:Lucas Dias Germano
Support Opportunities: Scholarships in Brazil - Doctorate (Direct)
FAPESP's process: 23/10027-5 - Reduction of species such as H+, CO2, and N2 for energy generation concomitantly with oxidation of organic contaminants
Grantee:Juliana Ferreira de Brito
Support Opportunities: Research Grants - Initial Project