催化学报

催化学报 ›› 2009, Vol. 30 ›› Issue (10): 1022-1028.

• 研究论文 • 上一篇    下一篇

甲烷水蒸气重整与甲烷无氧芳构化反应耦合提高Mo/MCM-49催化剂稳定性

姚颂东, 孙长勇, 李娟, 顾立军, 申文杰   

  1. 中国科学院大连化学物理研究所催化基础国家重点实验室, 辽宁大连 116023
  • 收稿日期:2009-10-25 出版日期:2009-10-25 发布日期:2013-06-06

Reaction Coupling of Methane Steam Reforming and Methane Dehydroaroma-tization for Improving Durability of Mo/MCM-49 Catalyst

YAO Songdong, SUN Changyong, LI Juan, GU Lijun, SHEN Wenjie*   

  1. State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China
  • Received:2009-10-25 Online:2009-10-25 Published:2013-06-06

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摘要： 甲烷无氧芳构化 (MDA) 和甲烷水蒸气重整 (MSR) 的耦合反应可以大幅度提高甲烷无氧芳构化反应的稳定性. 单独的甲烷无氧芳构化反应失活较快, 甲烷转化率从 0.5 h 的 14.5% 很快下降至 15 h 的 3.5%. 而采用联合 MSR/MDA 反应体系, 甲烷的转化率从 12.5 h 的 11.5% 非常缓慢地下降至 60 h 后的 6.5%. MSR 反应原位生成的 CO 和 H2 能降低反应中生成的 CHx物种数量, 减少催化剂上积炭的生成, 进而延长反应时间. MSR 反应过程中高比例 H2 的生成更能有效地减少与 B 酸相关的积炭的生成, 从而更好地抑制反应的失活.

关键词: 甲烷无氧芳构化甲烷水蒸气重整反应耦合钼MCM-49, 积炭

Abstract: The durability of methane dehydroaromatization (MDA) has been improved by its combination with methane steam reforming (MSR). The methane conversion in the combined MSR/MDA system decreases very slowly from 11.5% at 12.5 h to 6.5% at 60 h, whereas it decreases rapidly from 14.5% at 0.5 h to 3.5% at 15 h for the MDA reaction alone. CO and H2 produced in-situ through the MSR reaction may reduce the amount of CHx species during the reaction, which in turn reduces the formation of coke deposited on the catalyst, prolonging the durability of the MDA reaction. High content of H2 from the MSR process plays a major role in suppressing coke accumulation on the catalyst, especially the coke associated with the Brönsted acidic sites that are mainly responsible for the deactivation.

Key words: methane dehydroaromatization, methane stream reforming, reaction coupling, molybdenum, MCM-49, coke deposition