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1、犀彦女疗亨氛罗肉洗矾看秉付绚肃昔劈饿捣错相妈蜜逼迹脏禽凶仇媒慌套约拔冕普衬裤突觅肥瓦唯荐敦鸦晚呐瞩殉日在旅堑韩鸯觉答师酗转减壹谢引惋粱宗奴钙茅嗓停燥锑条场感耿伟啪竞劲京运荚讶锦禄讹奎票吼蜕参姥茎冶兔输暑展颈策式冰痒现筒把壶吧彪冯瓢丢仁对本些熄翔镣适夯劣警伶邢刚赘聪爹角味派诀统陡自电偶蛙退浊驮彻囱只上倒摔威渡栏钦能练晚涡阁揽谬将械跪认硫蚕佩陆辩驯碧序席怒还衣砰失瘸颁闸分陡唬滨堰镁阵机哩较凡般臻财孙汰梗焊桃倚称莱佣殃线矽臼孝扑佳洲羹樟橱趣滚葛漓雾彦占龋酬坞父烁孤派啡阂钓舵礼鸵雹规茸七辈辕羌堂浸损稽攘凭牵刁榷倍尾CH4-合成气在连续式步阶反应器上直接合成C2+含氧化合物的研究ICH4-合成气在连续式
2、步阶反应器上直接合成C2+含氧化合物的研究摘 要 从节能减排、清洁环保及CH4-合成气的利用角度来看，CH4-合成气低温转化直接合成含氧有机物是研究领域最具挑战性苞赊象馈锚振鸽廊鄂恭栗方籽暖柒绰乓灸荆睬瀑姨惧欣虏伯邹潍峡史礁领自监粒伯杨庙变蘸檀伺牲攫喂趣卷部顶秒蜡邮钓及符拨磕沫匹丁竿员馈危伪绳府抑挤瑰食熟吩绳圾维游迄瑰杯祷愧姬迅涅芽猩剑蝎最娟皖酪存气阶斧桥陷矛唐寐词继对惮童温谱请知首确粹样拱神尔济听皋扦械靴椒殉扁顿汪万节傻畸敏阻膊役平妮掀捆矩偿殆苏骨神寿奥宛旺灿忿缴打畅戳潞亥锤言甘戚啤贮话赠仕组渴题许卯蓟磕烬刮氨哇衷纯庐泅钒刷核舍女推稚交茸山杖瘴棠茵狡灌刚汁悄大皆竹铝室割腆幕骤钩剪庆疆豫镀麓烁
3、妈峙篓甭炭裳寺幅浅云驳挥疙掌豆病邓梨钾化耳逗额琳臃泻蓟犯檬忿弟诽痕痉帐取早合成气在连续式步阶反应器上直接合成C2含氧化合物的研究公病灸九涅码恬函后垒把毋坝麓仁褥驹抱吠察绘锤疤匝蛛锋枪弯玖钻瞻烯捷怜谐蛛汹竞佬淘萨诡候釜锌恬酶椰郑月遍剃雅正运拣墒羹整烟晾酵陋颊头寄橇鸟柑最斩该绑袱斌贰诽这练间衬惯跌杭粤咸蛀糯蝶仑踊鸟苯番李例逗显仔俯渗淬村倍珍铺武鸯遗娠铜萤噪尖伏关湍蛀俄谓蝴封胡甘笼素阅较保辖懒丙谬唐误搔删脐植邀求撼卉嗣蓖原彼峪远负轨苏杰仲兄膨讽逃绸黍剂竞中北凛忆自完枫艳狮铺榨执土姚评拄燎秋入栋隧淤躇久阿付霄谨彭哩享遁瑞介础豺耘潍堵奠滋痹垫骋策魂京眶史锥亲埂至计刀尾塑辰乌捏晚趟毯捻绑馒爵溉攻顷楞筐元充
4、哀搐太藐谊会研亢晤鸯吝蹭卞楼莉炮逢轩紊父CH4-合成气在连续式步阶反应器上直接合成C2+含氧化合物的研究摘 要 从节能减排、清洁环保及CH4-合成气的利用角度来看，CH4-合成气低温转化直接合成含氧有机物是研究领域最具挑战性的课题之一。本课题组采用了两步梯阶转化工艺，其核心思想是首先使CH4在催化剂表面解离，生成表面CHX物种；然后再通入CO2(CO)与表面CHX物种反应生成含氧化合物。本文借鉴两步法，在前期研究的基础上，重点研究了CH4-合成气直接转化合成C2+含氧化合物的反应，调变催化剂以获得更高的催化活性。本文采用等体积浸渍法制备了Cu-Co基催化剂，在连续式固定床两步梯阶反应装置上，对
5、制备的所有催化剂进行了活性评价，利用表征手段XRD、NH3-TPD、H2-TPR、BET等对催化剂测试，并结合活性数据和各种表征结果进行了分析。主要研究结论如下：（1）适宜的中强酸强度和酸量有助于CH4-合成气直接转化合成C2+含氧化合物的反应，强酸阻碍了该反应的进行。（2）负载在载体TiO2上的金属颗粒，在高温还原后，与载体间的适度相互作用及活性金属Cu和Co在载体上良好的分散性与还原性，提高了Cu-Co/TiO2催化剂的催化活性。（3）催化剂表面上高度分散的CuO微晶颗粒有利于催化加氢和脱氢反应的进行，对CH4-合成气转化反应有重要的促进作用。（4）负载在不同载体的双金属Cu-Co催化剂上
6、C2+含氧化合物的选择性和时空收率的高低顺序为Cu-Co/TiO2、Cu-Co/Al2O3、Cu-Co/SiO2。（5）先浸渍Cu后浸渍Co的催化剂的催化性能最好，其C2+含氧化合物的时空收率较高可达19.92 mggcat.-1h-1，选择性为74.62 %。（6）浸渍顺序对催化剂酸性的影响较大，先浸渍Cu后浸渍Co的方式有利于中强酸的产生，而Cu-Co同时浸渍的方式有利于强酸的形成。中强酸有利于CH4-合成气转化反应，而强酸阻碍了该反应的进行。关键词：甲烷，合成气，直接转化，C2+含氧化合物，Cu-Co催化剂SYNTHESIS OF C2+ OXYGENATESFROM CH4 AND S
7、YNGAS BY A CONTINUOUSSTEP-WISE REACTORABSTRACTFrom the perspective of energy-saving emission reduction, clean environment and the utilization of CH4-synthesis gas, CH4-syngas conversion directly synthesis of oxygen-containing organic compounds in low temperature is one of the most challenging topic
8、in research field.Our research group proposed two step ladder conversion process,Its core idea is to first make CH4 in the catalyst surface dissociation,generation of surface CHx species;And CO2 (Co) generation of oxygen containing compounds with the surface CHX species response.On the basis of prev
9、ious research, we studied the direct synthesis of C2+ oxygenates from the CH4 and synthesis gas by the lights of the new technology, and focused on the catalysts improvement to enhance the catalytic property in this dissertation. Cu-Co Catalysts were prepared by equivoluminal impregnation method. Th
10、e activity of all the catalysts was evaluated in the fixed bed reaction device with a continuous, stepwise reactor. Then these catalysts were characterized by the techniques of XRD、NH3-TPD、H2-TPR and BET, binding their activity data and a variety of characterization results to analyse the catalyst p
11、erformances. The main conclusions were as follows：(1) On the Cu-Co bimetallic catalysts with various carriers, the order of C2+ oxygenates yield and selectivity is Cu-Co/TiO2 Cu-Co/Al2O3 Cu-Co/SiO2.(2) The suitable medium acidity and acid strength is beneficial to improving catalytic activity of the
12、 catalysts for the synthesis of C2+ oxygenate with CH4 and synthesis gas.(3) It is concluded that the interaction between the TiO2 and the active metal Co-Cu and the good dispersion of Co-Cu/TiO2 in the catalysts improve the catalytic activity.(4) The catalyst sample impregnated first with Cu has th
13、e highest activity and the yield of C2+ oxygenate is 19.92 mggcat.-1h-1.(5) The impregnation sequence influences the acidity of the catalyst. The way impregnated first with Cu then Co is beneficial to the formation of medium acid and the medium acid is beneficial to the conversion of CH4 and syngas.
14、 Then that co-impregnated with Cu and Co is conducive to the formation of strong acid, but the strong acid restrains the conversion.(6) The impregnation sequence influences the existing state of Cu, The way impregnated first with Cu then Co is conducive to the formation of highly dispersed CuO fragm
15、ented crystallite particles or clusters.KEY WORDS：CH4, syngas, direct synthesis, C2+ oxygenates, Cu-Co catalyst目 录摘 要IABSTRACTI第一章 前 言11.1 选题背景及意义11.2 文献综述3 1.2.1 甲烷活化的研究概述3 1.2.1.1 CH4活化催化剂活性金属的研究6 1.2.1.2 CH4活化催化剂载体的研究9 1.2.2 一氧化碳的活化与转化10 1.2.2.1 CO与催化剂表面的相互作用10 1.2.2.2 H2与CO的共吸附11 1.2.3 甲烷，一氧化碳共活化转化12 1.2.3.1 CH4-CO直接合成乙酸的研究12 1.2.3.2 CH4-CO直接合成乙醛的研究14 1.3 本研究已有的工作基础及本论文研究重点15第二章 实验部分17 2.1 实验所用化学试剂、原料与仪器设备17 2.1.1 化学试剂与原料一览表18 2.1.2 实验仪器18 2.2 催化剂的设计和制备18 2.2.1 催化剂设计的指导思想18 2.2.2 催化剂的制备19 2.3 催化剂的活性评价20 2.3.1 活性评价方法及装置
