Ammonia(NH_(3)) decomposition to release CO_x-free hydrogen(H_(2)) over non-noble catalysts has gained increasing attention.In this study,three nanostructured CeO_(2) with different morphologies,viz.rod(R).sphere(Sph)...Ammonia(NH_(3)) decomposition to release CO_x-free hydrogen(H_(2)) over non-noble catalysts has gained increasing attention.In this study,three nanostructured CeO_(2) with different morphologies,viz.rod(R).sphere(Sph),and spindle(Spi),were fabricated and served as supports for Ni/CeO_(2) catalyst.The CeO_(2)supports are different in particle sizes,specific surface area and porosity,resulting in the formation of Ni nanoparticles with distinguished sizes and dispersions.The surface properties of the Ni/CeO_(2) catalysts are not only distinct but also influential,affecting the adsorption and desorption of NH_(3),N_(2),and/or H_(2)molecules.The Ni/CeO_(2)-R catalyst shows superior catalytic activity compared to the other two,owing to its smaller Ni crystallite size and larger BET surface area.The most abundant strong basic sites are observed for Ni/CeO_(2)-Spi catalyst based on its exposed CeO_(2)(110) planes,which facilitates the donation of electrons to the Ni particles,benefiting the associative desorption of N atoms.Thus,Ni/CeO_(2)-Spi shows higher catalytic activity than Ni/CeO_(2)-Sph,despite their almost identical Ni crystallite sizes.展开更多
基金Project supported by the National Key R&D Program of China (2020YFB1505604)the National Natural Science Foundation of China(22178058,22078062)。
文摘Ammonia(NH_(3)) decomposition to release CO_x-free hydrogen(H_(2)) over non-noble catalysts has gained increasing attention.In this study,three nanostructured CeO_(2) with different morphologies,viz.rod(R).sphere(Sph),and spindle(Spi),were fabricated and served as supports for Ni/CeO_(2) catalyst.The CeO_(2)supports are different in particle sizes,specific surface area and porosity,resulting in the formation of Ni nanoparticles with distinguished sizes and dispersions.The surface properties of the Ni/CeO_(2) catalysts are not only distinct but also influential,affecting the adsorption and desorption of NH_(3),N_(2),and/or H_(2)molecules.The Ni/CeO_(2)-R catalyst shows superior catalytic activity compared to the other two,owing to its smaller Ni crystallite size and larger BET surface area.The most abundant strong basic sites are observed for Ni/CeO_(2)-Spi catalyst based on its exposed CeO_(2)(110) planes,which facilitates the donation of electrons to the Ni particles,benefiting the associative desorption of N atoms.Thus,Ni/CeO_(2)-Spi shows higher catalytic activity than Ni/CeO_(2)-Sph,despite their almost identical Ni crystallite sizes.