A series of Ce-doped Ni-B amorphous alloy catalysts were prepared by a KBH_4 reduction method, characterized by ICP, BET, XRD, H_2-chemisorption, H_2-TPD, etc., and tested in the hydrogenation of 2-ethylanthraquinone....A series of Ce-doped Ni-B amorphous alloy catalysts were prepared by a KBH_4 reduction method, characterized by ICP, BET, XRD, H_2-chemisorption, H_2-TPD, etc., and tested in the hydrogenation of 2-ethylanthraquinone. The results of characterization show that with the addition of Ce the amount of H_2-chemisorption and H_2-TPD areas first increases markedly and then decreases with the maximum appears at the atomic ratio of Ce to Ni of 0.036. The hydrogenation activity also shows the same trend. The effects of Ce are attributed to its dispersion of Ni particles, resulting in the formation of more surface Ni centers. However, much higher Ce contents may result in the decrease of the surface Ni contents. After heat treatment at higher temperatures, the amorphous structure of Ni-B is destroyed.展开更多
Uniform Ni-B amorphous alloys about 14 nm have been prepared on CNTs-A support,named Ni-B/CNTs-A. In comparison with the Ni-B/CNTs amorphous catalyst, Ni-B/CNTs-A showed higher nickel loading, determined by ICP and be...Uniform Ni-B amorphous alloys about 14 nm have been prepared on CNTs-A support,named Ni-B/CNTs-A. In comparison with the Ni-B/CNTs amorphous catalyst, Ni-B/CNTs-A showed higher nickel loading, determined by ICP and better catalytic activity and ethylene selectivity in the acetylene hydrogenation reaction.展开更多
Phenylalanine (Phe) is a significant amino acid that cannot be synthesized by human themselves but must be taken from environment. It was initially found that the nanosized amorphous Ni-B/SiO2 alloy prepared by the ...Phenylalanine (Phe) is a significant amino acid that cannot be synthesized by human themselves but must be taken from environment. It was initially found that the nanosized amorphous Ni-B/SiO2 alloy prepared by the chemical reduction method was an effective catalyst for the preparation of Phe from phenylpyruvic acid (PPA) by amination and hydrogenation. It has been found that the amorphous Ni-B/SiO2 alloy catalyst exhibits superior activity and selectivity to the traditional catalysts Raney Ni and Urushibara nickel. The effects of reaction time, amounts of catalysts and ammonia solution, reaction temperature, and H2 pressure on the reaction have been investigated systematically. The results indicated that the yield of Phe was 97.9%, and the selectivity for Phe reached 98.9% when the reaction was carried out for 3 h at 333 K and 2.0 MPa of H2 with m(Cat.) : m(PPA) = 0.6 : 1.0 and n(NH3) : n(PPA) = 3 : 1. The catalysts were characterized by XRD, AAS, XPS, BET, and TEM, and the relationship between the catalyst structure and the catalytic activity was discussed in detail. It was found that the reason why Ni-B/SiO2 amorphous alloy catalyst was much more active for the preparation of Phe could be accounted for by the presence of electron-rich Ni due to electron donation from alloying B; the smaller size of Ni-B particles, the larger specific surface area of Ni-B/SiO2.展开更多
Annealing crystallization of ultrafine NiB amorphous alloy prepared by the chemical reduction method was studied by DTA, XRD and XAFS techniques. The XRD and XAFS results have revealed that the crystallization process...Annealing crystallization of ultrafine NiB amorphous alloy prepared by the chemical reduction method was studied by DTA, XRD and XAFS techniques. The XRD and XAFS results have revealed that the crystallization process of ultrafine NiB amorphous alloy proceeds in two steps. First, ultrafine NiB amorphous alloy is crystallized to form metastable nanocrystalline Ni3B at an annealing temperature of 325℃. Second, the nanocrystalline Ni3B is further decomposed into crystalline Ni at 380CCC or higher tempera ture, the local structure around Ni atoms in resultant product is similar to that in Ni foil. It was found that the catalytic activity of nanocrystalline Ni3B for benzene hydro-genation is much higher than that of ultrafine NiB amorphous alloy or crystalline Ni. The result indicates that the active sites of nanocrystalline Ni3B for benzene hydrogena-tion are composed of both Ni and B with proper geometry configuration.展开更多
文摘A series of Ce-doped Ni-B amorphous alloy catalysts were prepared by a KBH_4 reduction method, characterized by ICP, BET, XRD, H_2-chemisorption, H_2-TPD, etc., and tested in the hydrogenation of 2-ethylanthraquinone. The results of characterization show that with the addition of Ce the amount of H_2-chemisorption and H_2-TPD areas first increases markedly and then decreases with the maximum appears at the atomic ratio of Ce to Ni of 0.036. The hydrogenation activity also shows the same trend. The effects of Ce are attributed to its dispersion of Ni particles, resulting in the formation of more surface Ni centers. However, much higher Ce contents may result in the decrease of the surface Ni contents. After heat treatment at higher temperatures, the amorphous structure of Ni-B is destroyed.
基金The National Natural Science Foundation of China(No.20263003)supported this work.
文摘Uniform Ni-B amorphous alloys about 14 nm have been prepared on CNTs-A support,named Ni-B/CNTs-A. In comparison with the Ni-B/CNTs amorphous catalyst, Ni-B/CNTs-A showed higher nickel loading, determined by ICP and better catalytic activity and ethylene selectivity in the acetylene hydrogenation reaction.
基金Fundamental research project of South-Central University for Nationalities (No. YZZ05010)
文摘Phenylalanine (Phe) is a significant amino acid that cannot be synthesized by human themselves but must be taken from environment. It was initially found that the nanosized amorphous Ni-B/SiO2 alloy prepared by the chemical reduction method was an effective catalyst for the preparation of Phe from phenylpyruvic acid (PPA) by amination and hydrogenation. It has been found that the amorphous Ni-B/SiO2 alloy catalyst exhibits superior activity and selectivity to the traditional catalysts Raney Ni and Urushibara nickel. The effects of reaction time, amounts of catalysts and ammonia solution, reaction temperature, and H2 pressure on the reaction have been investigated systematically. The results indicated that the yield of Phe was 97.9%, and the selectivity for Phe reached 98.9% when the reaction was carried out for 3 h at 333 K and 2.0 MPa of H2 with m(Cat.) : m(PPA) = 0.6 : 1.0 and n(NH3) : n(PPA) = 3 : 1. The catalysts were characterized by XRD, AAS, XPS, BET, and TEM, and the relationship between the catalyst structure and the catalytic activity was discussed in detail. It was found that the reason why Ni-B/SiO2 amorphous alloy catalyst was much more active for the preparation of Phe could be accounted for by the presence of electron-rich Ni due to electron donation from alloying B; the smaller size of Ni-B particles, the larger specific surface area of Ni-B/SiO2.
基金the National NaturalScience Foundation of China (Grant No. 29673038) and "the One-hundred People Plan" of the Chinese Academy of Sciences.
文摘Annealing crystallization of ultrafine NiB amorphous alloy prepared by the chemical reduction method was studied by DTA, XRD and XAFS techniques. The XRD and XAFS results have revealed that the crystallization process of ultrafine NiB amorphous alloy proceeds in two steps. First, ultrafine NiB amorphous alloy is crystallized to form metastable nanocrystalline Ni3B at an annealing temperature of 325℃. Second, the nanocrystalline Ni3B is further decomposed into crystalline Ni at 380CCC or higher tempera ture, the local structure around Ni atoms in resultant product is similar to that in Ni foil. It was found that the catalytic activity of nanocrystalline Ni3B for benzene hydro-genation is much higher than that of ultrafine NiB amorphous alloy or crystalline Ni. The result indicates that the active sites of nanocrystalline Ni3B for benzene hydrogena-tion are composed of both Ni and B with proper geometry configuration.