Isolated iridium oxide sites on modified carbon nitride for photoreforming of plastic derivatives

Pawan Kumar, Hongguang Zhang, Asfaw G. Yohannes, Jiu Wang, Ali Shayesteh Zeraati, Soumyabrata Roy, Xiyang Wang, Karthick Kannimuthu, Abdelrahman M. Askar, Kristen A. Miller, Kexin Ling, Muflih Adnan, Sung-Fu Hung, Jian-Jie Ma, Wei-Hsiang Huang, Dhwanil Trivedi, Maria Molina, Heng Zhao, Angel A. Martí, Adam F. G. Leontowich, George K. H. Shimizu, David Sinton, Michael M. Adachi, Yimin A. Wu, Pulickel M. Ajayan, Samira Siahrostami (), Jinguang Hu () and Md Golam Kibria ()
Additional contact information
Pawan Kumar: University of Calgary
Hongguang Zhang: University of Calgary
Asfaw G. Yohannes: University of Calgary
Jiu Wang: University of Calgary
Ali Shayesteh Zeraati: University of Calgary
Soumyabrata Roy: Indian Institute of Technology Kanpur
Xiyang Wang: University of Waterloo
Karthick Kannimuthu: University of Calgary
Abdelrahman M. Askar: Simon Fraser University
Kristen A. Miller: Rice University
Kexin Ling: Rice University
Muflih Adnan: University of Calgary
Sung-Fu Hung: National Yang Ming Chiao Tung University
Jian-Jie Ma: National Yang Ming Chiao Tung University
Wei-Hsiang Huang: National Synchrotron Radiation Research Center
Dhwanil Trivedi: University of Calgary
Maria Molina: University of Calgary
Heng Zhao: University of Calgary
Angel A. Martí: Rice University
Adam F. G. Leontowich: Canadian Light Source, 44 Innovation Boulevard
George K. H. Shimizu: University of Calgary
David Sinton: University of Toronto
Michael M. Adachi: Simon Fraser University
Yimin A. Wu: University of Waterloo
Pulickel M. Ajayan: Rice University
Samira Siahrostami: Simon Fraser University
Jinguang Hu: University of Calgary
Md Golam Kibria: University of Calgary

Nature Communications, 2025, vol. 16, issue 1, 1-17

Abstract: Abstract The rising concentration of plastics due to extensive disposal and inefficient recycling of plastic waste poses an imminent and critical threat to the environment and ecological systems. Photocatalytic reforming of plastic derivatives to value-added chemicals under ambient conditions proceeds at lower oxidation potential which galvanizes the hydrogen evolution. We report the synthesis of a narrow band gap NCN-functionalized O-bridged carbon nitride (MC) through condensation polymerization of hydrogen-bonded melem (M)-cyameluric acid (C) macromolecular aggregate. The MC scaffold hosts well-dispersed Ir single atom (MCIrSA) sites which catalyze oxidative photoreforming of alkali-treated polylactic acid (PLA) and polyethylene terephthalate (PET) derivatives to produce H2 at a rate of 147.5 and 29.58 μmol g−1cat h−1 under AM1.5G irradiation. Solid-state electron paramagnetic resonance (EPR) and time-resolved photoluminescence (TRPL) reveals efficient charge carrier generation and separation in MCIrSA. X-ray absorption spectroscopy (XAS) and Bader charge analysis reveal undercoordinated IrN2O2 SA sites pinned in C6N7 moieties leading to efficient hole quenching. The liquid phase EPR, in situ FTIR and density functional theory (DFT) studies validate the facile generation of •OH radicals due to the evolution of O-Ir-OH transient species with weak Ir--OH desorption energy barrier.

Date: 2025
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DOI: 10.1038/s41467-025-57999-w

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