Two density functional theory methods were employed to evaluate the H_(2) storage capabilities of metalloborospherenes TM_(8)B_(6)(TM=Ni,Pd).Consequently,the superatoms Ni8B6 and Pd8B6,which accommodate 40 and 32 H_(2...Two density functional theory methods were employed to evaluate the H_(2) storage capabilities of metalloborospherenes TM_(8)B_(6)(TM=Ni,Pd).Consequently,the superatoms Ni8B6 and Pd8B6,which accommodate 40 and 32 H_(2) molecules,respectively,exhibit gravimetric H_(2) uptake capacities of 13.134%and 6.562%,respectively.The average binding energies of Ni_(8)B_(6)(H_(2))_(40) and Pd_(8)B_(6)(H_(2))_(32) fall within the optimal range for reversible H_(2) storage applications.The interactions between H_(2) molecules and the parent structures were characterized using various wave function analysis methods.Polarization effects,alongside the Kubas mechanism,are pivotal to the adsorption of H_(2) on TM_(8)B_(6).Moreover,the investigations examine the effect of temperature on the H_(2) storage capacity of TM_(8)B_(6) at atmospheric pressure.Atom-centered density-matrix propagation molecular dynamics simulations confirm the reversibility of H_(2) adsorption and desorption cycles.The thermodynamic analyses of the desorption behavior of H_(2) molecules were conducted via a three-dimensional graph,plotted based on the relationship between the number of adsorbed H_(2) molecules and temperature as well as pressure,revealing that the majority of adsorbed H_(2) molecules can be released at 0.5 MPa and 358 K.Compared to the respective monomeric counterparts,the H_(2) storage densities of(TM_(8)B_(6))_(2) dimers exhibit a slight reduction.展开更多
文摘Two density functional theory methods were employed to evaluate the H_(2) storage capabilities of metalloborospherenes TM_(8)B_(6)(TM=Ni,Pd).Consequently,the superatoms Ni8B6 and Pd8B6,which accommodate 40 and 32 H_(2) molecules,respectively,exhibit gravimetric H_(2) uptake capacities of 13.134%and 6.562%,respectively.The average binding energies of Ni_(8)B_(6)(H_(2))_(40) and Pd_(8)B_(6)(H_(2))_(32) fall within the optimal range for reversible H_(2) storage applications.The interactions between H_(2) molecules and the parent structures were characterized using various wave function analysis methods.Polarization effects,alongside the Kubas mechanism,are pivotal to the adsorption of H_(2) on TM_(8)B_(6).Moreover,the investigations examine the effect of temperature on the H_(2) storage capacity of TM_(8)B_(6) at atmospheric pressure.Atom-centered density-matrix propagation molecular dynamics simulations confirm the reversibility of H_(2) adsorption and desorption cycles.The thermodynamic analyses of the desorption behavior of H_(2) molecules were conducted via a three-dimensional graph,plotted based on the relationship between the number of adsorbed H_(2) molecules and temperature as well as pressure,revealing that the majority of adsorbed H_(2) molecules can be released at 0.5 MPa and 358 K.Compared to the respective monomeric counterparts,the H_(2) storage densities of(TM_(8)B_(6))_(2) dimers exhibit a slight reduction.
