Fabricating stable CoNi active sites and elucidating the role of N in enhancing hydrogenation and dehydrogenation of MgH2

Abstract

Magnesium hydride (MgH2) is considered a promising solid-state hydrogen storage material due to its excellent capacity and reversibility. However, its practical application is hindered by the high operating temperature. Herein, a controllable pyrolysis method was employed to synthesize N-doped carbon nanotubes anchoring highly dispersed CoNi alloy nanoparticles using a metal–organic framework (MOF) precursor, and they were introduced into a MgH2 matrix for the first time. Surprisingly, MgH2–CoNi@N-CNTs could achieve an initial H2 desorption at 174 °C, which is 201 °C lower than that of pristine MgH2 under parallel conditions. It also demonstrated excellent H2 release and absorption kinetics and can release 6.3 wt% H2 in 600 s at 275 °C, which is 1.7 and 4.8 times higher than those of N-deficient MgH2–CoNi@C and pristine MgH2, respectively. More importantly, it maintained a high desorption capacity of 5.2 wt% H2 at 250 °C with obviously low desorption activation energy (78.6 kJ mol−1). Combined with theoretical analyses, the catalytic promotion effect of N is attributed to a novel electron trafficking between the stable CoNi active sites and N-CNTs, which can significantly weaken the Mg–H bond strength and promote hydrogen absorption/desorption efficiency of MgH2. This work provides a tunable and effective strategy for designing high-performance MgH2 with superior catalytic efficiency.

Graphical abstract: Fabricating stable CoNi active sites and elucidating the role of N in enhancing hydrogenation and dehydrogenation of MgH2

Supplementary files

Article information

Article type
Paper
Submitted
01 Apr 2025
Accepted
10 May 2025
First published
30 May 2025

J. Mater. Chem. A, 2025, Advance Article

Fabricating stable CoNi active sites and elucidating the role of N in enhancing hydrogenation and dehydrogenation of MgH2

F. Li, Z. Huang, Y. Wang, S. Guan, G. Ou, Y. Wang, J. Wu, S. Cheng, L. Wu and X. Ding, J. Mater. Chem. A, 2025, Advance Article , DOI: 10.1039/D5TA02579F

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