以MCM-41作载体的磷化镍催化剂的加氢脱氮性能

HYDRODENITROGENATION PERFORMANCE OF MCM-41-SUPPORTED NICKEL PHOSPHIDES

采用原位还原方法制备了以MCM-41作载体的磷化镍催化剂，并以喹啉作模型化合物考察了其加氢脱氮（HDN）反应性能。结果表明，由MCM-41担载制备的磷化镍催化剂的HDN活性远高于传统的硫化态Ni—W催化剂，最佳Ni／P摩尔比为1．0～1．25。从反应中间体和产物分析结果可以看出，磷化镍催化剂表现出很高的加氢活性，这可能是磷化镍催化剂具有较高脱氮活性的主要原因。当NiO和P2O5总担载量低于40％时，催化剂活性随着NiO和P2O5总担载量的增加而增加，其最佳担载量为30％。XRD结果表明，NiaP与Ni12P5同为HDN活性相。但Ni2P活性更高。

MCM-41-supported nickel phosphides were prepared by an in-situ-reduction method. Their hydrodenitrogenation （HDN） activities were evaluated by means of 1 % quinoline in decalin. It was indicated that the HDN activity of the MCM-41-supported nickel phosphides was much higher than that of the supported Ni-W sulfide. The optimal initial molar ratio of Ni/P was 1.0 1.25. It could be concluded from the distribution of the intermediates and the products that high hydrogenation activity of the MCM-41-supported nickel phosphides should be responsible for their high HDN activity. When the total loading of NiO and P2O5 was below 40%, the HDN activity of the MCM-41-supported nickel phosphides increased with increasing the total loading of NiO and P2O5 , and the optimal total loading of NiO and P2O5 was 30 %. XRD patterns of the high-performance phosphide catalysts suggested that both the Ni2P and Ni12P5 were active in the HDN reactions, and Ni2P was more active.