石油炼制与化工
石油煉製與化工
석유련제여화공
PETROLEUM PROCESSING AND PETROCHEMICALS
2014年
9期
40-46
,共7页
鄢景森%王海彦%齐振东%李晓惠
鄢景森%王海彥%齊振東%李曉惠
언경삼%왕해언%제진동%리효혜
复合载体%二氧化钛%二氧化硅%磷化镍%加氢脱氮
複閤載體%二氧化鈦%二氧化硅%燐化鎳%加氫脫氮
복합재체%이양화태%이양화규%린화얼%가경탈담
composite support%titania%silica%nickel phosphide%hydrodenitrog enation
采用溶胶-凝胶法制备了不同 Ti?Si 比的 TiO2-SiO2复合载体,其负载的磷化镍催化剂采用等体积浸渍法和 H2原位还原法制备,以喹啉为模型化合物,考察了活性组分负载量、Ni?P 比、Ti?Si 比对催化剂加氢脱氮性能的影响。采用 N2吸附、XRD、TPR、NH3-TPD 和 FT-IR 等技术对载体和催化剂进行了表征。结果表明:溶胶-凝胶法制成的复合载体具有较大的比表面积,其负载的磷化镍催化剂具有较好的可还原性,Ni?P 摩尔比小于1.0时,还原后所形成的物相为 Ni2 P;当 Ti?Si 摩尔比为1?2、Ni?P 摩尔比为1.0、Ni-P 负载量(w)为25%时,Ni2 P?TiO2-SiO2催化剂具有最佳的加氢脱氮效果。
採用溶膠-凝膠法製備瞭不同 Ti?Si 比的 TiO2-SiO2複閤載體,其負載的燐化鎳催化劑採用等體積浸漬法和 H2原位還原法製備,以喹啉為模型化閤物,攷察瞭活性組分負載量、Ni?P 比、Ti?Si 比對催化劑加氫脫氮性能的影響。採用 N2吸附、XRD、TPR、NH3-TPD 和 FT-IR 等技術對載體和催化劑進行瞭錶徵。結果錶明:溶膠-凝膠法製成的複閤載體具有較大的比錶麵積,其負載的燐化鎳催化劑具有較好的可還原性,Ni?P 摩爾比小于1.0時,還原後所形成的物相為 Ni2 P;噹 Ti?Si 摩爾比為1?2、Ni?P 摩爾比為1.0、Ni-P 負載量(w)為25%時,Ni2 P?TiO2-SiO2催化劑具有最佳的加氫脫氮效果。
채용용효-응효법제비료불동 Ti?Si 비적 TiO2-SiO2복합재체,기부재적린화얼최화제채용등체적침지법화 H2원위환원법제비,이규람위모형화합물,고찰료활성조분부재량、Ni?P 비、Ti?Si 비대최화제가경탈담성능적영향。채용 N2흡부、XRD、TPR、NH3-TPD 화 FT-IR 등기술대재체화최화제진행료표정。결과표명:용효-응효법제성적복합재체구유교대적비표면적,기부재적린화얼최화제구유교호적가환원성,Ni?P 마이비소우1.0시,환원후소형성적물상위 Ni2 P;당 Ti?Si 마이비위1?2、Ni?P 마이비위1.0、Ni-P 부재량(w)위25%시,Ni2 P?TiO2-SiO2최화제구유최가적가경탈담효과。
TiO2-SiO2 composite support was prepared by sol-gel method,and the supported nickel phosphide catalysts,Ni2 P?TiO2-SiO2 ,were prepared by incipient wetness impregnation and in situ H 2 reduction method. The samples were characterized by N2 adsorption-desorption,XRD,TPR,NH 3-TPD and FT-IR. Their hydrodenitrogenation (HDN)performance was evaluated in a continuous-flow fixed-bed reactor using quinoline as a model molecule to investigate the effect of the active component loading, Ni?P molar ratio and Ti?Si molar ratio. The results show that TiO2-SiO2 composite support has a larger specific surface area. The Ni2 P?TiO2-SiO2 catalyst precursor has a better reducibility,which helps the formation of Ni2 P phase. Ni2 P phase appears for the Ni2 P?TiO2-SiO2 catalyst at n(Ni)?n(P)≤1.0. The optimal HDN activity occurs for the Ni2 P?TiO2-SiO2 with Ti?Si molar ratio of 1?2,Ni?P molar ratio of 1.0 and the loading of (NiO+P2 O5 )of 25%.