LiBH_(4) containing 18.5 wt.%H_(2) is an attractive high-capacity hydrogen storage material,however,it suffers from high operation temperature and poor reversibility.Herein,a novel and low-cost bifunctional additive,w...LiBH_(4) containing 18.5 wt.%H_(2) is an attractive high-capacity hydrogen storage material,however,it suffers from high operation temperature and poor reversibility.Herein,a novel and low-cost bifunctional additive,waxberry-like Fe_(3)O_(4) secondary nanospheres assembled from ultrafine primary Fe_(3)O_(4) nanoparticles,is synthesized,which exhibits significant destabilization and bidirectional catalyzation towards(de)hydrogenation of LiBH_(4).With an optimized addition of 30 wt.% waxberry-like Fe_(3)O_(4),the system initiated dehydrogenation below 100℃ and released a total of 8.1 wt.%H_(2) to 400℃.After 10 cycles,a capacity retention of 70% was achieved,greatly superior to previously reported oxides-modified systems.The destabilizing and catalyzing mechanisms of waxberry-like Fe_(3)O_(4) on LiBH_(4) were systematically analyzed by phase and microstructural evolutions during dehydrogenation and hydrogenation cycling as well as density functional theory(DFT)calculations.The present work provides new insights in developing advanced nano-additives with unique structural and multifunctional designs towards LiBH4 hydrogen storage.展开更多
基金supported by the National Natural Science Foundation of China(No.52071287)the Natural Science Foundation of Zhejiang Province(No.LZ23E010002)the Basic and Applied Basic Research Foundation of Guangdong Province(Nos.2021A1515110676,2022A1515011832).
文摘LiBH_(4) containing 18.5 wt.%H_(2) is an attractive high-capacity hydrogen storage material,however,it suffers from high operation temperature and poor reversibility.Herein,a novel and low-cost bifunctional additive,waxberry-like Fe_(3)O_(4) secondary nanospheres assembled from ultrafine primary Fe_(3)O_(4) nanoparticles,is synthesized,which exhibits significant destabilization and bidirectional catalyzation towards(de)hydrogenation of LiBH_(4).With an optimized addition of 30 wt.% waxberry-like Fe_(3)O_(4),the system initiated dehydrogenation below 100℃ and released a total of 8.1 wt.%H_(2) to 400℃.After 10 cycles,a capacity retention of 70% was achieved,greatly superior to previously reported oxides-modified systems.The destabilizing and catalyzing mechanisms of waxberry-like Fe_(3)O_(4) on LiBH_(4) were systematically analyzed by phase and microstructural evolutions during dehydrogenation and hydrogenation cycling as well as density functional theory(DFT)calculations.The present work provides new insights in developing advanced nano-additives with unique structural and multifunctional designs towards LiBH4 hydrogen storage.
