Single atoms coordinated on graphitic carbon nitrides to photocatalytic conversion of methane

• Grant number: 21/13271-9
• Support Opportunities: Scholarships in Brazil - Doctorate
• Start date: July 01, 2022
• Status: Discontinued
• Field of knowledge: Physical Sciences and Mathematics - Chemistry - Inorganic Chemistry
• Principal Investigator: Ivo Freitas Teixeira
• Grantee: Marcos Augusto Ribeiro da Silva
• Host Institution: Centro de Ciências Exatas e de Tecnologia (CCET). Universidade Federal de São Carlos (UFSCAR). São Carlos , SP, Brazil
• Associated research grant: 20/14741-6 - Graphitic carbon nitrides as platforms for single-atom photocatalysis: moving towards design principles for improved performance, AP.JP
• Associated scholarship(s): 24/16292-5 - Single Atoms Coordinated on Graphitic Carbon Nitrides for the Photocatalytic Conversion of Methane, BE.EP.DR

Abstract

The unique electronic configuration and distribution of metal single atoms are desirable features for catalysts in chemical conversions. Stabilization of isolated atoms in heterogeneous supports is a powerful strategy to improve catalytic turnover and decrease the number of metals in a reaction. Furthermore, properties from homogeneous catalysts can be achieved in single atoms heterogeneous systems, with intrinsic benefits of solids compounds like stability and recycling. Crystalline carbon nitride rises as a compelling support for metal single atoms stabilization through a simple and controlled method. These metals can be employed in different chemical reactions, such as key reactions in the petrochemical industry. Emerging as an alternative for traditional fossil fuels for energy supply, methane is a carbon source with huge potential reserves. Despite its abundance, methane is a greenhouse gas and its emission has a global warming impact 25 times greater than carbon dioxide. It is necessary to convert this excess of methane into other value-added chemicals. Photocatalysis is considered one of the best alternatives for the direct conversion of methane to other high-value products because it uses electromagnetic radiation (UV or visible) to drive chemical reactions under mild conditions (low temperatures and pressures). Also, it can provide a less oxidative route, avoiding overoxidation to CO and CO2, increasing the selectivity to oxygenate products, such as methanol and ethanol. In this project, we aim to synthesize carbon nitrides with poly (heptazine imide) structures (PHI) and introduce transition metals single atoms via a cation exchange method, recently developed by our group. These catalysts will be applied in the photocatalytic methane oxidation reactions, under mild conditions, to produce oxygenates aiming to obtain mainly methanol, a platform molecule in the petrochemical industry. (AU)

Scientific publications

(8)

(References retrieved automatically from Web of Science and SciELO through information on FAPESP grants and their corresponding numbers as mentioned in the publications by the authors)

DA SILVA, MARCOS A. R.; TARAKINA, NADEZDA V.; FILHO, JOSE B. G.; CUNHA, CARLA S.; ROCHA, GUILHERME F. S. R.; DIAB, GABRIEL A. A.; ANDO, ROMULO AUGUSTO; SAVATEEV, OLEKSANDR; AGIRREZABAL-TELLERIA, IKER; SILVA, INGRID F.; et al. Single-Atoms on Crystalline Carbon Nitrides for Selective C―H Photooxidation: A Bridge to Achieve Homogeneous Pathways in Heterogeneous Materials. Advanced Materials, v. 35, n. 52, p. 13-pg., 2023-11-20. (20/14741-6, 22/16273-5, 21/12394-0, 21/13271-9, 21/11162-8)

BATISTA, WALKER VINICIUS FERREIRA DO CARMO; DE OLIVEIRA, WANESSA LIMA; DE OLIVEIRA, EDUARDA FERREIRA; CRUZ, TAIS SANTOS; FERRARI, JEFFERSON LUIS; ARCHANJO, BRAULIO SOARES; GRIGOLETTO, SABRINA; FERREIRA, DALVA ESTER DA COSTA; PEREIRA, FABIANO VARGAS; DIAB, GABRIEL ALI ATTA; et al. Ni Single-Atoms Supported on N-Doped Carbon Prepared by Cation Exchange: Ultrafast Catalyst For The Reduction of Nitroarene Compounds Under Ambient Conditions. CHEMCATCHEM, v. 16, n. 18, p. 13-pg., 2024-07-16. (21/14006-7, 21/12394-0, 20/14741-6, 21/13271-9)

ROCHA, GUILHERME F. S. R.; DA SILVA, MARCOS A. R.; ROGOLINO, ANDREA; DIAB, GABRIEL A. A.; NOLETO, LUIS F. G.; ANTONIETTI, MARKUS; TEIXEIRA, IVO F.. Carbon nitride based materials: more than just a support for single-atom catalysis. CHEMICAL SOCIETY REVIEWS, v. 52, n. 15, p. 56-pg., 2023-07-06. (21/14006-7, 21/11162-8, 22/04748-9, 20/14741-6, 21/13271-9)

DA SILVA, MARCOS AUGUSTO R.; GIL, JESSICA C.; TORRES, JULIANA A.; SILVA, GELSON T. S. T.; FILHO, JOSE BALENA GABRIEL; VICTORIA, HENRIQUE FERNANDES VIEIRA; KRAMBROCK, KLAUS; TEIXEIRA, IVO F.; RIBEIRO, CAUE. Investigating the Metal-TiO₂ Influence for Highly Selective Photocatalytic Oxidation of Methane to Methanol. ACS APPLIED MATERIALS & INTERFACES, v. 16, n. 32, p. 13-pg., 2024-07-23. (21/13271-9, 18/01258-5, 20/14741-6)

ROGOLINO, ANDREA; SILVA, INGRID F.; TARAKINA, NADEZDA V.; DA SILVA, MARCOS A. R.; ROCHA, GUILHERME F. S. R.; ANTONIETTI, MARKUS; TEIXEIRA, IVO F.. Modified Poly(Heptazine Imides): Minimizing H2O2 Decomposition to Maximize Oxygen Reduction. ACS APPLIED MATERIALS & INTERFACES, v. 14, n. 44, p. 10-pg., 2022-10-31. (21/11162-8, 20/14741-6, 22/04748-9, 21/13271-9)

ROGOLINO, ANDREA; FILHO, JOSE B. G.; FRITSCH, LORENA; ARDISSON, JOSE D.; DA SILVA, MARCOS A. R.; ATTA DIAB, GABRIEL ALI; SILVA, INGRID FERNANDES; FERREIRA MORAES, CARLOS ANDREE; FORIM, MOACIR ROSSI; BAUER, MATTHIAS; et al. Direct Synthesis of Acetone by Aerobic Propane Oxidation Promoted by Photoactive Iron(III) Chloride under Mild Conditions. ACS CATALYSIS, v. 13, n. 13, p. 8-pg., 2023-06-15. (21/14006-7, 21/13271-9, 20/14741-6, 21/11162-8)

OLIVEIRA, WANESSA L.; OLIVEIRA, EDUARDA FERREIRA DE; BATISTA, WALKER VINICIUS FERREIRA DO CARMO; MOURA, HENRIQUE A. J. L.; PIRES, MANOEL JOSE MENDES; COELHO, RAFAEL MENDES; DIAB, GABRIEL ALI ATTA; TEIXEIRA, IVO FREITAS; MARQUES, GLEISON; MASTELARO, VALMOR ROBERTO; et al. A metal-free catalyst based on g-C3N4 functionalized with cyamelurate-like groups: Catalytic properties and mechanism of a new heterogeneous Fenton-like catalyst. Carbon, v. 214, p. 12-pg., 2023-10-01. (21/14006-7, 21/13271-9, 20/14741-6, 21/11162-8)

OLIVEIRA, WANESSA L.; DA SILVA, MARCOS A. R.; DIAB, GABRIEL ALI ATTA; G FILHO, JOSE BALENA; PASTANA, VITOR G. S.; SILVA, LUANA L. B.; DE OLIVEIRA, EDUARDA FERREIRA; BATISTA, WALKER VINICIUS FERREIRA DO CARMO; DA CRUZ, TAIS DOS SANTOS; MASTELARO, VALMOR ROBERTO; et al. Selective Photocatalytic Benzene Oxidation Using Iron-Carbon Nitride Fragments Functionalized with Cyamelurate-Like Groups. CHEMPHOTOCHEM, v. N/A, p. 12-pg., 2024-11-20. (21/14006-7, 21/12394-0, 20/14741-6, 21/13271-9)