化工进展
化工進展
화공진전
CHEMICAL INDUSTRY AND ENGINEERING PROGRESS
2015年
6期
1646-1651
,共6页
王豪%赵婉莹%刘振伟%尧振宇%吴雁
王豪%趙婉瑩%劉振偉%堯振宇%吳雁
왕호%조완형%류진위%요진우%오안
催化剂%加氢%微波%水热%磷
催化劑%加氫%微波%水熱%燐
최화제%가경%미파%수열%린
catalyst%hydrogenation%microwave%hydrothermal%phosphorous
采用微波水热法(MWH)制备含磷 W/Al2O3加氢精制催化剂,分别以磷酸(PA)、磷酸三乙酯(TEP)和羟基乙叉二磷酸(HEDP)为磷源,考察磷源、制备方法和磷含量对催化剂物化性质和加氢脱氮(HDN)性能的影响。结果表明,使用HEDP为磷源不仅可减弱活性组分-载体间的相互作用,其结构中的羟基还可与MWH产生的H2WO4形成氢键而吸附在H2WO4表面,抑制H2WO4团聚,从而实现WO3的高分散。MWH快速均匀加热的特点可以有效抑制H2WO4的过度生长,并促进其在Al2O3表面的均匀快速分散,使得以HEDP为磷源制备的W/Al2O3中WO3的分散度和HDN活性远高于浸渍法制备的相同磷源、磷含量和金属含量的催化剂。MWH法制备的磷质量分数为3%的催化剂兼具高的WO3分散度和弱的WO3-Al2O3相互作用,有最佳的HDN活性。
採用微波水熱法(MWH)製備含燐 W/Al2O3加氫精製催化劑,分彆以燐痠(PA)、燐痠三乙酯(TEP)和羥基乙扠二燐痠(HEDP)為燐源,攷察燐源、製備方法和燐含量對催化劑物化性質和加氫脫氮(HDN)性能的影響。結果錶明,使用HEDP為燐源不僅可減弱活性組分-載體間的相互作用,其結構中的羥基還可與MWH產生的H2WO4形成氫鍵而吸附在H2WO4錶麵,抑製H2WO4糰聚,從而實現WO3的高分散。MWH快速均勻加熱的特點可以有效抑製H2WO4的過度生長,併促進其在Al2O3錶麵的均勻快速分散,使得以HEDP為燐源製備的W/Al2O3中WO3的分散度和HDN活性遠高于浸漬法製備的相同燐源、燐含量和金屬含量的催化劑。MWH法製備的燐質量分數為3%的催化劑兼具高的WO3分散度和弱的WO3-Al2O3相互作用,有最佳的HDN活性。
채용미파수열법(MWH)제비함린 W/Al2O3가경정제최화제,분별이린산(PA)、린산삼을지(TEP)화간기을차이린산(HEDP)위린원,고찰린원、제비방법화린함량대최화제물화성질화가경탈담(HDN)성능적영향。결과표명,사용HEDP위린원불부가감약활성조분-재체간적상호작용,기결구중적간기환가여MWH산생적H2WO4형성경건이흡부재H2WO4표면,억제H2WO4단취,종이실현WO3적고분산。MWH쾌속균균가열적특점가이유효억제H2WO4적과도생장,병촉진기재Al2O3표면적균균쾌속분산,사득이HEDP위린원제비적W/Al2O3중WO3적분산도화HDN활성원고우침지법제비적상동린원、린함량화금속함량적최화제。MWH법제비적린질량분수위3%적최화제겸구고적WO3분산도화약적WO3-Al2O3상호작용,유최가적HDN활성。
Phosphorous-containing W/Al2O3 hydrotreating catalysts were prepared via microwave hydrothermal (MWH) method,in which phosphoric acid (PA),triethyl phosphate (TEP) and 1-hydroxy ethylidene-1,1-diphosphonic acid (HEDP) were used as phosphorus sources,respectively. The effects of phosphorus sources,catalyst preparation methods and phosphorus contents on the physicochemical properties and hydrodenitrogenation (HDN) activity of catalysts were studied. The results show that the introduction of HEDP can weaken tungsten-alumina interaction and keep highly dispersed tungsten species by forming H-bonding between the hydroxyl groups of HEDP and H2WO4 to prevent tungsten species from aggregation. The MWH method,characterized by rapid and uniform heating,can greatly inhibit the excess growth of H2WO4 colloids and help to disperse tungsten oxide on alumina uniformly and quickly. When the HEDP is used as phosphorus resource,catalyst prepared via MWH method shows much higher WO3 dispersion and HDN activity than that with the same phosphorus and metal contents prepared by impregnation method. The catalyst prepared via MWH method with 3%phosphorus combines high WO3 dispersion with weak tungsten-alumina interaction,leading to the highest HDN activity.