Issue 34, 2024

Built-in electrophilic/nucleophilic domain of nitrogen-doped carbon nanofiber-confined Ni2P/Ni3N nanoparticles for efficient urea-containing water-splitting reactions

Abstract

Transferring urea-containing waste water to clean hydrogen energy has received increasing attention, while challenges are still faced in the sluggish catalytic kinetics of urea oxidation. Herein, a novel hybrid catalyst of Ni2P/Ni3N embedded in nitrogen-doped carbon nanofiber (Ni2P/Ni3N/NCNF) is developed for energy-relevant urea-containing water-splitting reactions. The built-in electrophilic/nucleophilic domain resulting from the electron transfer from Ni2P to Ni3N accelerates the formation of high-valent active Ni species and promotes favourable urea molecule adsorption. A spectral study and theoretical analysis reveal that the negatively shifted Ni d-band centre in Ni2P/Ni3N/NCNF weakens the adsorption of intermediate CO2 and facilitates its desorption, thereby improving the urea oxidation reaction kinetics. The overall reaction process is also optimized by minimizing the energy barrier of the rate-determining step. Following the stability test, the surface reconstruction of the pre-catalyst is discussed, where an amorphous layer of NiOOH as the real active phase is formed on the surface/interface of Ni2P/Ni3N for urea oxidation. Benefiting from these characteristics, a high current density of 151.11 mA cm−2 at 1.54 V vs. RHE is obtained for urea oxidation catalysed by Ni2P/Ni3N/NCNF, exceeding that of most of the similar catalysts. A low cell voltage of 1.39 V is required to reach 10 mA cm−2 for urea electrolysis, which is about 200 mV less than that of the general water electrolysis. The current work will be helpful for the development of advanced catalysts and their application in the urea-containing waste water transfer to clean hydrogen energy.

Graphical abstract: Built-in electrophilic/nucleophilic domain of nitrogen-doped carbon nanofiber-confined Ni2P/Ni3N nanoparticles for efficient urea-containing water-splitting reactions

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Article information

Article type
Edge Article
Submitted
20 mar 2024
Accepted
20 jul 2024
First published
07 aug 2024
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY-NC license

Chem. Sci., 2024,15, 13659-13667

Built-in electrophilic/nucleophilic domain of nitrogen-doped carbon nanofiber-confined Ni2P/Ni3N nanoparticles for efficient urea-containing water-splitting reactions

J. Li, C. Yin, S. Wang, B. Zhang and L. Feng, Chem. Sci., 2024, 15, 13659 DOI: 10.1039/D4SC01862A

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