TY - JOUR
T1 - Sc/Ti functionalized defective C20 as promising materials for hydrogen storage
T2 - a theoretical study
AU - Tang, Yupeng
AU - Chang, Tong
AU - Yang, Haiying
AU - Li, Nan
N1 - Publisher Copyright:
© The Author(s), under exclusive licence to Springer Science+Business Media, LLC, part of Springer Nature 2026.
PY - 2026
Y1 - 2026
N2 - In present work, we theoretically designed and addressed the H2 uptake properties of TM2C16 (TM = Sc, Ti) cages originating from C20 to overcome TM clustering. The Sc2C16/Ti2C16 cluster can adsorb a maximum of 12/10 H2 molecules with a gravimetric H2 uptake capacity of 7.85/6.50 wt% and a volumetric density of 97.39/83.10 g H2·L− 1, surpassing the target set by the US-DOE for onboard hydrogen storage in light-duty vehicles. For Sc2C16(H2)12, 4 H2 molecules are decomposed into H atoms and bonded with the parent body, forming Sc2C16H4(H2)10. The average binding energy of Sc2C16H4(H2)2n and Ti2C16(H2)2n (n = 1–5) fall within the ideal range for reversible hydrogen storage. The results of Gibbs free energy correction suggest that all H2 molecules adsorbed in molecular form in Sc2C16H4(H2)2n and Ti2C16(H2)2n (n = 1–5) can be efficiently adsorbed and desorbed under atmospheric pressure. The reversible characteristics of the adsorption/desorption cycle were verified through ADMP-MD simulations. The thermodynamic analysis indicates that the majority of the adsorbed hydrogen molecules in Sc2C16H4(H2)10/Ti2C16(H2)10 can be desorbed under practical temperature and pressure conditions, with a practical capacity of 5.31/5.60 wt%, being close to the target specified by the US-DOE.
AB - In present work, we theoretically designed and addressed the H2 uptake properties of TM2C16 (TM = Sc, Ti) cages originating from C20 to overcome TM clustering. The Sc2C16/Ti2C16 cluster can adsorb a maximum of 12/10 H2 molecules with a gravimetric H2 uptake capacity of 7.85/6.50 wt% and a volumetric density of 97.39/83.10 g H2·L− 1, surpassing the target set by the US-DOE for onboard hydrogen storage in light-duty vehicles. For Sc2C16(H2)12, 4 H2 molecules are decomposed into H atoms and bonded with the parent body, forming Sc2C16H4(H2)10. The average binding energy of Sc2C16H4(H2)2n and Ti2C16(H2)2n (n = 1–5) fall within the ideal range for reversible hydrogen storage. The results of Gibbs free energy correction suggest that all H2 molecules adsorbed in molecular form in Sc2C16H4(H2)2n and Ti2C16(H2)2n (n = 1–5) can be efficiently adsorbed and desorbed under atmospheric pressure. The reversible characteristics of the adsorption/desorption cycle were verified through ADMP-MD simulations. The thermodynamic analysis indicates that the majority of the adsorbed hydrogen molecules in Sc2C16H4(H2)10/Ti2C16(H2)10 can be desorbed under practical temperature and pressure conditions, with a practical capacity of 5.31/5.60 wt%, being close to the target specified by the US-DOE.
KW - Atom centered density matrix propagation (ADMP)
KW - Density functional theory
KW - Gibbs free energy correction
KW - Hydrogen storage
KW - TMC (TM = Sc
KW - Ti) clusters
UR - https://www.scopus.com/pages/publications/105043102842
U2 - 10.1007/s11224-026-02835-0
DO - 10.1007/s11224-026-02835-0
M3 - Article
AN - SCOPUS:105043102842
SN - 1040-0400
JO - Structural Chemistry
JF - Structural Chemistry
ER -