固体氧化物电解质膜反应器中甲烷在Li/TiO2上的氧化偶联Oxidative Coupling of Methane over Li/TiO2 in Solid-State Electrolyte Membrane Reactor
李俊,石勇,王宇红,卢冠忠,赵玲
摘要(Abstract)：
以Li2CO3为锂源,制备了Li/TiO2膜,并用TG-DTA和XRD等技术对其进行了表征,由TG-DTA结果并结合XRD图谱可知,陪烧过程中发生了化学反应,并形成新的物相Li1.33Ti1.66O4。在YSZ固体氧化物电解质反应器中研究了甲烷在Li/TiO2膜上氧化偶联,考查了预混合、电化学两种方式供氧时甲烷分压、反应温度及停留时间等对甲烷转化速率、各产物生成速率和选择性等影响,比较了两种方式供氧时反应速率、目标产物选择性,并基于实验结果对反应机理进行了分析。结果表明,提高甲烷分压和反应温度对甲烷转化速率和目标产物选择性有利;提高预混合时氧分压或电化学供氧时的电流均能使反应速率增大,但CO2生成速率显著增加,导致目标产物选择性减小;在相同的反应温度、甲烷分压和氧通量条件下,电化学供氧时,催化剂膜上氧浓度较大而气相氧浓度较小,甲烷的转化速率及C2选择性明显大于预混合供氧。
关键词(KeyWords)： 甲烷;氧化偶联;固体氧化物电解质;电化学供氧;预混合供氧
基金项目(Foundation): 上海市自然科学基金(07ZR14106);; 上海市科委重点项目(06-JC-14095);; 上海市教委基金(06-OZ-003)
作者(Author): 李俊,石勇,王宇红,卢冠忠,赵玲
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