The Li-Mg-B-H composite(2LiBH_(4)+MgH_(2))has a high capacity of 11.4 wt%as a hydrogen storage material.However,the slow kinetics and poor cycling stability severely restrict its practical applications.In this work,a ...The Li-Mg-B-H composite(2LiBH_(4)+MgH_(2))has a high capacity of 11.4 wt%as a hydrogen storage material.However,the slow kinetics and poor cycling stability severely restrict its practical applications.In this work,a layered Nb_(2)C MXene was first synthesized and then introduced to tailor the kinetics and cycling stability of the Li-Mg-B-H composite.The milled 2LiH+MgB_(2)composites were initially hydrogenated to obtain the 2LiBH_(4)+MgH_(2)composites.The 2LiBH_(4)+MgH_(2)+5wt%Nb_(2)C can release 9.0 wt%H_(2)in 30 min at 400℃,while it is only 2.7 wt%for the undoped 2LiBH_(4)+MgH_(2).The dehydrogenation activation energies of MgH_(2)and LiBH_(4)are 123 and 154 kJ·mol^(-1)respectively for the 5 wt%Nb_(2)C-doped composite,lower than the undoped composite(164 and 165 kJ·mol^(-1)).The 2LiBH_(4)+MgH_(2)+5 wt%Nb_(2)C possesses excellent cycling stability,with the reversible capacity only slightly reduced from 9.4 wt%for the 1st cycle to 9.3 wt%for the 20th cycle.Nb_(2)C keeps stable in the composite and acts as an efficient catalyst for the Li-Mg-B-H composite.It is believed that both the layered structure and the active Nb element contribu te to the enhanced hydrogen storage performances of the Li-Mg-B-H composite.This work confirms that the Nb_(2)C MXene with layered stru cture has a significant enhancing impact on the Li-Mg-B-H hydrogen storage materials,which is different from the bulk NbC.展开更多
Many MXenes are efficient catalysts for MgH_(2)hydrogen storage material.Nevertheless,the synthesis of MXenes should consume a large amount of corrosive HF to etch out the Al layers from the transition metal aluminum ...Many MXenes are efficient catalysts for MgH_(2)hydrogen storage material.Nevertheless,the synthesis of MXenes should consume a large amount of corrosive HF to etch out the Al layers from the transition metal aluminum carbides or nitrides(MAX) phases,which is environmentally unfriendly.In this work,Ti_(3)AlCN MAX without HFetching was employed directly to observably enhance the kinetics and the cycling stability of MgH_(2).With addition of10 wt% Ti_(3)AlCN,the onset dehydrogenation temperature of MgH2 was dropped from 320 to 205℃,and the rehydrogenation of MgH2 under 6 MPa H2 began at as low as50℃.Furthermore,at 300℃,it could provide 6.2 wt% of hydrogen in 10 min.Upon cycling,the composite underwent an activation process during the initial 40 cycles,with the reversible capacity increased from 4.7 wt% to 6.5 wt%.After that,the capacity showed almost no attenuation for up to 100 cycles.The enhancing effect of Ti_(3)AICN on MgH_(2) was comparable to many MXenes.It was demonstrated that Ti_(3)AICN did not destabilize MgH_(2) but acted as an efficient catalyst for MgH_(2).Ti_(3)AICN was observed to be the active sites for the nucleation and growth of MgH_(2)and might also help in dissociation and recombination of hydrogen molecules.Such two factors are believed to contribute to the improvement of MgH_(2).This study not only provides a promising strategy for improving the hydrogen storage performances of MgH_(2) by using noncorrosive MAX materials,but also adds evidence of nucleation and growth of MgH_(2) on a catalyst.展开更多
基金financially supported by the Science and Technology Department of Guangxi Zhuang Autonomous(No.GuiKeAD21238022)the National Natural Science Foundation of China(Nos.52001079,22379030 and 52261038)Quzhou Science and Technology Project(No.2022K103)。
文摘The Li-Mg-B-H composite(2LiBH_(4)+MgH_(2))has a high capacity of 11.4 wt%as a hydrogen storage material.However,the slow kinetics and poor cycling stability severely restrict its practical applications.In this work,a layered Nb_(2)C MXene was first synthesized and then introduced to tailor the kinetics and cycling stability of the Li-Mg-B-H composite.The milled 2LiH+MgB_(2)composites were initially hydrogenated to obtain the 2LiBH_(4)+MgH_(2)composites.The 2LiBH_(4)+MgH_(2)+5wt%Nb_(2)C can release 9.0 wt%H_(2)in 30 min at 400℃,while it is only 2.7 wt%for the undoped 2LiBH_(4)+MgH_(2).The dehydrogenation activation energies of MgH_(2)and LiBH_(4)are 123 and 154 kJ·mol^(-1)respectively for the 5 wt%Nb_(2)C-doped composite,lower than the undoped composite(164 and 165 kJ·mol^(-1)).The 2LiBH_(4)+MgH_(2)+5 wt%Nb_(2)C possesses excellent cycling stability,with the reversible capacity only slightly reduced from 9.4 wt%for the 1st cycle to 9.3 wt%for the 20th cycle.Nb_(2)C keeps stable in the composite and acts as an efficient catalyst for the Li-Mg-B-H composite.It is believed that both the layered structure and the active Nb element contribu te to the enhanced hydrogen storage performances of the Li-Mg-B-H composite.This work confirms that the Nb_(2)C MXene with layered stru cture has a significant enhancing impact on the Li-Mg-B-H hydrogen storage materials,which is different from the bulk NbC.
基金financially supported by the Science and Technology Department of Guangxi Zhuang Autonomous (No.GuiKeAD21238022)the Natural Science Foundation of Guangxi Province (No.2019GXNSFBA185004)National Natural Science Foundation of China (Nos.52001079,51961005 and 52261038)。
文摘Many MXenes are efficient catalysts for MgH_(2)hydrogen storage material.Nevertheless,the synthesis of MXenes should consume a large amount of corrosive HF to etch out the Al layers from the transition metal aluminum carbides or nitrides(MAX) phases,which is environmentally unfriendly.In this work,Ti_(3)AlCN MAX without HFetching was employed directly to observably enhance the kinetics and the cycling stability of MgH_(2).With addition of10 wt% Ti_(3)AlCN,the onset dehydrogenation temperature of MgH2 was dropped from 320 to 205℃,and the rehydrogenation of MgH2 under 6 MPa H2 began at as low as50℃.Furthermore,at 300℃,it could provide 6.2 wt% of hydrogen in 10 min.Upon cycling,the composite underwent an activation process during the initial 40 cycles,with the reversible capacity increased from 4.7 wt% to 6.5 wt%.After that,the capacity showed almost no attenuation for up to 100 cycles.The enhancing effect of Ti_(3)AICN on MgH_(2) was comparable to many MXenes.It was demonstrated that Ti_(3)AICN did not destabilize MgH_(2) but acted as an efficient catalyst for MgH_(2).Ti_(3)AICN was observed to be the active sites for the nucleation and growth of MgH_(2)and might also help in dissociation and recombination of hydrogen molecules.Such two factors are believed to contribute to the improvement of MgH_(2).This study not only provides a promising strategy for improving the hydrogen storage performances of MgH_(2) by using noncorrosive MAX materials,but also adds evidence of nucleation and growth of MgH_(2) on a catalyst.