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Graphitic Carbon Nitrides as Platforms for Single-Atom Photocatalysis: Moving Towards Design Principles for Improved Performance

Grant number: 22/14335-3
Support Opportunities:Scholarships in Brazil - Scientific Initiation
Effective date (Start): December 01, 2022
Effective date (End): November 30, 2023
Field of knowledge:Physical Sciences and Mathematics - Chemistry - Inorganic Chemistry
Principal Investigator:Ivo Freitas Teixeira
Grantee:Pietra Flores Rainho Martins
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


Herein, one scientific initiation student will be responsible by the controlled design of the PHI/PTI-Single-Atoms systems to be applied in organic synthesis reactions and follow their catalytic applications in organic synthesis reactions. First, we intend to test these photocatalysts for photoredox reactions, since Ir3+-PHI were already successfully prepared and Ir3+ compounds are well-known photoredox catalysts.1 We also intend to control the oxidation state for the also successfully prepared Ru3+-PHI, in order to try to obtain Ru2+-PHI, since Ru2+ complex are also well-known photoredox catalysts.1 Analogous systems of Ir3+-PTI and Ru2+-PTI also will be prepared and tested to photoredox reactions.Later, we will test the PHI/PTI-Single-Atom systems in commonly not light-driven reactions, such as Suzuki-coupling2 and C-H activations.3 In this step, we will compare the systems activity under light irradiation and without. In order to evaluate if their activity and mechanism of action can be influenced by the light excitation. For the Suzuki-coupling reaction will be prepared Pd0-PHI/PTI systems, since commonly used homogeneous catalysts have as active site the Pd0. For the C-H activation testes will be prepared PHI/PTI systems with Pd, Pt, Fe, Ir and Cu as single-atoms. These transition metals are the most commonly used as homogeneous catalyst for C-H activation.3Lastly, we will investigate the mechanism behind the activity of the active PHI/PTI-Single-Atom systems for organic synthesis reactions. Once the most important aspects of the mechanisms for the active systems are revealed, these pieces of information will be used in the retro-design synthesis of the PHI/PTI systems by design bimetallic single-atom catalyst or by controlling the single-atoms oxidation states and concentrations, in order to improve their efficiency and selectivity.

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