Ultrafine carbon-based transition metal compounds have been widely investigated as efficient catalysts for enhancing the hydrogen storage performance of magnesium hydride.In this work,the carbon ther-mal shock method ...Ultrafine carbon-based transition metal compounds have been widely investigated as efficient catalysts for enhancing the hydrogen storage performance of magnesium hydride.In this work,the carbon ther-mal shock method is applied to synthesize the ultrafine carbon-encapsulated NbC nanoparticles with an average grain size of 17.3 nm.The MgH_(2)-10 wt%NbC/C composites show excellent low-temperature hy-drogen storage performance with the onset dehydrogenation temperature of 196.1℃,which is 92.2℃ and 98℃ lower than that of MgH_(2)-10 wt%NbC and undoped MgH_(2),respectively.Specifically,MgH_(2)-10 wt%NbC/C can absorb 6.71 wt%H_(2) at 100℃ within 30 min around and retain almost 100%reversible hydrogen desorption capacity after 10 cycles.For the catalytic mechanism,the electron transfer process between multi-valence Nb cations of in-situ formed NbH x and Mg,H atoms can greatly improve the cyclic de/rehydrogenation kinetics of MgH_(2)-NbC/C.Besides,the enhancement of dehydrogenation kinetics can also be ascribed to MgH_(2) particle refinement by NbC nanoparticles,and destabilization of the Mg-H bond caused by carbon substrate.This investigation not only proves that carbon-encapsulated NbC nanoparti-cles can greatly enhance the hydrogen storage performance of MgH_(2) but provides an idea of preparing carbon-based transition metal carbides as effective catalysts for magnesium-based hydrogen storage ma-terials.展开更多
基金supported by the National Natural Science Foundation of China (No.U20A20237)the Zhejiang Provincial Nat-ural Science Foundation of China (No.LZ21E010002).
文摘Ultrafine carbon-based transition metal compounds have been widely investigated as efficient catalysts for enhancing the hydrogen storage performance of magnesium hydride.In this work,the carbon ther-mal shock method is applied to synthesize the ultrafine carbon-encapsulated NbC nanoparticles with an average grain size of 17.3 nm.The MgH_(2)-10 wt%NbC/C composites show excellent low-temperature hy-drogen storage performance with the onset dehydrogenation temperature of 196.1℃,which is 92.2℃ and 98℃ lower than that of MgH_(2)-10 wt%NbC and undoped MgH_(2),respectively.Specifically,MgH_(2)-10 wt%NbC/C can absorb 6.71 wt%H_(2) at 100℃ within 30 min around and retain almost 100%reversible hydrogen desorption capacity after 10 cycles.For the catalytic mechanism,the electron transfer process between multi-valence Nb cations of in-situ formed NbH x and Mg,H atoms can greatly improve the cyclic de/rehydrogenation kinetics of MgH_(2)-NbC/C.Besides,the enhancement of dehydrogenation kinetics can also be ascribed to MgH_(2) particle refinement by NbC nanoparticles,and destabilization of the Mg-H bond caused by carbon substrate.This investigation not only proves that carbon-encapsulated NbC nanoparti-cles can greatly enhance the hydrogen storage performance of MgH_(2) but provides an idea of preparing carbon-based transition metal carbides as effective catalysts for magnesium-based hydrogen storage ma-terials.