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Insights into the active nickel centers embedded in graphitic carbon nitride for the oxygen evolution reaction

DOI: 10.1039/D3TA07389K DOI Help

Authors: Nicolò Rossetti (Università di Padova and INSTM Research Unit) , Aldo Ugolotti (Università degli Studi di Milano-Bicocca) , Claudio Cometto (Università di Padova and INSTM Research Unit) , Veronica Celorrio (Diamond Light Source) , Goran Dražič (National Institute of Chemistry (Slovenia)) , Cristiana Di Valentin (Università degli Studi di Milano-Bicocca) , Laura Calvillo (Università di Padova and INSTM Research Unit)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Journal Of Materials Chemistry A

State: Published (Approved)
Published: February 2024
Diamond Proposal Number(s): 28356

Open Access Open Access

Abstract: Experimental and theoretical studies have demonstrated that the use of single atom catalysts (SACs) for energy conversion processes is very promissing. However, their stability under catalytic conditions is the main issue that hinders their commercial use. In this work, we report an oxygen evolution catalyst based on single nickel atoms stabilized in triazine-based carbon nitride (CN) and a detailed study of the evolution of the Ni centers under catalytic conditions. The nanostructured materials have been characterized by combining experimental techniques, such as X-ray diffraction, transmission electron microscopy, X-ray absorption and X-ray photoemission spectroscopy, with DFT theoretical calculations to determine the CN structure, the metal adsorption sites, the coordination of the Ni atoms, as well as the changes undergone under catalytic conditions. Electrochemical characterization showed a linear increase of the catalytic activity with the Ni loading. The stability of the materials was studied by HR-TEM and XAS post-catalysis measurements and DFT simulations. Results indicated a partial chemical restructuration of the single Ni atoms under catalytic conditions with the formation of Ni-O-Ni moieties, stabilized in the CN cavities, which are the real catalytic species.

Subject Areas: Chemistry, Materials, Energy

Instruments: B18-Core EXAFS

Added On: 14/02/2024 13:44


Discipline Tags:

Earth Sciences & Environment Sustainable Energy Systems Energy Climate Change Physical Chemistry Catalysis Chemistry Materials Science

Technical Tags:

Spectroscopy X-ray Absorption Spectroscopy (XAS)