Ammonia-borane (AB) is an excellent material for chemical storage of hydrogen. However,t he practical utilization of AB for production of hydrogen is hindered by the need of expensive noble metal-based catalysts.H ere,w er eport Cu x Co 1Àx Onanoparticles (NPs) facilely deposited on graphene oxide (GO) as alow-cost and high-performance catalyst for the hydrolysis of AB.T his hybrid catalyst exhibits an initial total turnover frequency (TOF) value of 70.0 (H 2 )m ol/(Cat-metal) mol·min, which is the highest TOFe ver reported for noble metal-free catalysts,and agood stability keeping 94 %activity after 5c ycles.S ynchrotron radiation-based X-ray absorption spectroscopy( XAS) investigations suggested that the high catalytic performance could be attributed to the interfacial interaction between Cu x Co 1Àx ON Ps and GO.M oreover,t he catalytic hydrolysis mechanismw as studied by in situ XAS experiments for the first time,w hichr eveal asignificant water adsorption on the catalyst and clearly confirm the interaction between AB and the catalyst during hydrolysis.Controlled storage and release of hydrogen are well-known challenges in establishing av iable fuel-cell-based hydrogen economy. [1][2][3] Recently,the chemical storage of hydrogen was considered as af easible way for practical applications. [1][2][3][4][5][6][7][8] Among the chemical hydrogen-storage materials,a mmoniaborane (AB) has been regarded as aleading contender owing to its high hydrogen content (19.6 wt %), high stability in both aqueous solutions and air at room temperature,a nd nontoxicity. [1][2][3][4][5][6][7][8][9] However,u ntil now,e ffective catalysts for the hydrolysis of AB are typically based on expensive and rare noble metals (such as Pt, Ru), [4,7,8] which has largely hampered applications. [3,5,7] Thus,a lternate catalysts for high-efficiencyh ydrolysis of AB based on inexpensive nonnoble metal elements are highly required and intensely studied. [3,5,7] Despite many catalysts for the hydrolysis of AB,h igh-performance noble metal-free catalyst with practical efficiency and sustainability remains unavailable and adaunting challenge.T he catalytic mechanism regarding the electronic structure changes of the catalysts is also unclear and has largely limited the design of high-efficiencycatalysts.Graphene is an outstanding supporting material for efficient catalysts,b ecause it can enhance the catalytic performance with synergetic effects. [10][11][12][13][14][15][16][17][18] Recently,g raphene was used to support various non-noble metal nanoparticles (NPs) for efficient catalysts for the hydrolysis of AB. [14][15][16] Although the hybrids showed enhanced catalytic properties, their performance remained insufficient and their electronic structure had not been well studied. [14][15][16] Herein we report af acile way to prepare the hybrids of Cu x Co 1Àx ON Ps on graphene oxide (GO). Theo ptimized hybrid (Cu x Co 1Àx O-GO) shows superior catalytic performance in the hydrolysis of AB with ah igh initial TOF value of 70.0 (H 2 )m ol/(Catmetal) mol...