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甲烷选择氧化制甲醇研究进展

Progress of Methane Selective Oxidation to Methanol

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【作者】 王玉孙兰兰武光军关乃佳李兰冬

【Author】 WANG Yu;SUN Lanlan;WU Guangjun;GUAN Naijia;LI Landong;School of Materials Science and Engineering, Nankai University;

【通讯作者】 李兰冬;

【机构】 南开大学材料科学与工程学院

【摘要】 甲烷作为天然气主要成分,是储量丰富的清洁低碳资源,同时甲烷也是一种强温室气体,开发有效的方法将甲烷转化为化学品或液体燃料具有重要的战略意义。目前成熟的甲烷转化路线都依赖于合成气作为中间体的间接路线,而能源消耗较低的甲烷直接转化过程开始受到全球范围的广泛关注。在所有理论上可行的甲烷直接转化路线中,在温和条件下甲烷选择氧化制备甲醇是最理想的方案,其具有成本低和能耗低的特点。尽管在甲烷制甲醇反应(MTM)已取得了重大进展,但仍无法同时获得高甲烷转化率与高甲醇选择性。本文综述了以甲烷为原料,模拟甲烷单加氧酶氧化的简单化学反应过程,调研大量以工业应用为目标的贵金属及仿生非贵金属分子筛催化剂合成甲醇及其衍生物的研究进展,综合考虑反应条件、分子筛催化剂拓扑结构及反应活性中心、机理路线对催化效果的影响,对甲醇产率较低和现有催化反应体系难以推广到工业规模的原因进行了总结与讨论。

【Abstract】 The high availability of methane as the main component of natural gas and its proliferation as a powerful greenhouse gas call for the development of effective strategies for the transformation of methane into valuable chemicals and liquid fuel. All the mature routes for methane utilization were indirect ones and exclusively rely on syngas as an intermediate, while the direct routes for methane utilization with much less energy consumption was now receiving significant attention all over the world. Among all conceptually feasible routed of methane direct conversion, the selective oxidation of methane to methanol under mild conditions became the ideal choice, which provides a low-cost and energy-efficient route of methane utilization. Although significant progresses had been made in methane to methanol conversion(MTM), it was still extremely challenging to achieve the methane conversion and high methanol selectivity at the same time. In the review article, recent research progresses on MTM reaction, simulating the simple chemical reaction catalyzed by nature methane monooxygenase, were summarized. Representative noble metal and biomimetic non-noble metal zeolite catalysts were surveyed for the conversion of methane to methanol and its derivatives, targeting the industrial applications. The influences of reaction conditions, topology of zeolite catalysts, active metal centers and reaction mechanism on the catalytic reactivity were discussed in details.Finally, the reasons for the low methanol productivity and the difficulties of MTM reaction for industrial applications were illustrated and prospected.

  • 【文献出处】 化学反应工程与工艺 ,Chemical Reaction Engineering and Technology , 编辑部邮箱 ,2021年06期
  • 【分类号】TQ223.121;TQ426
  • 【被引频次】1
  • 【下载频次】589
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