Ti-based catalysts are known to improve the hydrogen storage performance of NaAlH4by facilitating the dissociation/recombination of H-H and Al-H bonds.The catalytic activity of metallic Ti species strongly depends on ...Ti-based catalysts are known to improve the hydrogen storage performance of NaAlH4by facilitating the dissociation/recombination of H-H and Al-H bonds.The catalytic activity of metallic Ti species strongly depends on its particle size and dispersity.Ti clusters and even single atoms are therefore highly desirable,but their controllable fabrication has been highly challenging.He rein,we demonstrate a novel facile sonochemical synthesis of a Ti-O clusters featuring single Ti atom catalyst at room temperature.Through reducing TiCl_(4)by MgBu_(2)with ultrasound instead of heating as driving force,numerous single Ti atoms coupled with Ti-O clusters with Ti loading on graphene(Ti_(1)/Ti-O@G)up to 22.6 wt%have been successfully obtained.The prepared Ti_(1)/Ti-O@G contributes high reactivity and superior catalytic activity,therefore enabling full dehydrogenation of NaAlH_(4)at 80℃in thermogravimetric mode and re-hydrogenation at 30℃and 10 MPa with 4.9 wt% H_(2).This fact indicates for the first time that single Ti atom catalyst with high loading is highly effective in catalyzing hydrogen cycling of NaAlH4at remarkably reduced temperatures.展开更多
基金financially supported by the National Outstanding Youth Foundation of China(No.52125104)the Natural Science Foundation of Zhejiang Province(No.LD21E010002)+2 种基金the National Natural Science Foundation of China(Nos.52071285 and 52001277)the Fundamental Research Funds for the Central Universities(Nos.2021FZZX001-09 and 226-202200246)the National Youth Top-Notch Talent Support Program。
文摘Ti-based catalysts are known to improve the hydrogen storage performance of NaAlH4by facilitating the dissociation/recombination of H-H and Al-H bonds.The catalytic activity of metallic Ti species strongly depends on its particle size and dispersity.Ti clusters and even single atoms are therefore highly desirable,but their controllable fabrication has been highly challenging.He rein,we demonstrate a novel facile sonochemical synthesis of a Ti-O clusters featuring single Ti atom catalyst at room temperature.Through reducing TiCl_(4)by MgBu_(2)with ultrasound instead of heating as driving force,numerous single Ti atoms coupled with Ti-O clusters with Ti loading on graphene(Ti_(1)/Ti-O@G)up to 22.6 wt%have been successfully obtained.The prepared Ti_(1)/Ti-O@G contributes high reactivity and superior catalytic activity,therefore enabling full dehydrogenation of NaAlH_(4)at 80℃in thermogravimetric mode and re-hydrogenation at 30℃and 10 MPa with 4.9 wt% H_(2).This fact indicates for the first time that single Ti atom catalyst with high loading is highly effective in catalyzing hydrogen cycling of NaAlH4at remarkably reduced temperatures.
