Assisting Ni catalysis by CeO_(2) with oxygen vacancy to optimize the hydrogen storage properties of MgH_(2)

摘要

Although MgH_(2) has been widely regarded as a promising material for solid-state hydrogen storage,its high operating temperature and slow kinetics pose a major bottleneck to its practical application.Here,a nanocomposite catalyst with interfacial coupling and oxygen defects,Ni/CeO_(2),is fabricated to promote H_(2) desorption and absorption properties of MgH_(2).The interface of Ni/CeO_(2) contributes to both strong mechanical coupling towards stabilizing partial Ni and electronic coupling towards inducing a high con-centration of oxygen vacancies in CeO_(2).Theoretical calculations evidence that CeO_(2) with oxygen vacancy assist Ni in weakening the energy of Mg-H bond as well as enhancing the adsorption energy of Ni upon hydrogen atoms,and the extent of this assistance surprisingly increases with increasing oxygen vacancies concentration.As a result,an impressive performance is achieved by MgH_(2)-5 wt.%Ni/CeO_(2) with onset desorption temperature of only 165°C,and it absorbs approximately 80%hydrogen in just 800 s at 125°C.The generation mechanism of intermediate active species concerning Ni/CeO_(2) in different states has been analyzed for the first time,and the relationship between interfacial coupling and phase evolution has been elucidated.Therefore,a mechanism of the catalysis-assisting effect regarding oxygen defects is proposed.It is believed that this work provides a unique perspective on the mechanism of interfacial coupling and the generation of defects in composite catalysts.