Abstract:

The chemical looping reforming reaction of methane (CLRM) employs a solid oxygen carrier material as an intermediate to split the traditional methane reforming reaction into two reactions, reduction and oxidation, in which the oxygen carrier is continuously oxidized and reduced, forming a cyclic reaction and realizing the continuous production of syngas or hydrogen. More importantly, the CLRM reaction delivers a high purity product without the requirement of a costly air separation unit compared to conventional reforming reactions. And the key to the research of CLRM reaction lies on the design and selection of oxygen carriers. This paper summarized the recent research progress of metal-based oxygen carriers (Ni, Fe, Cu, Co, Mn, Ce-based) and composite oxygen carriers (including calixarenes and hexaaluminates) in recent years, focusing on the effects of the composition and structure of these oxygen carriers on the reactivity, and concluded the strategy of design and optimization of these oxygen carriers. Furthermore, the methods for the synthesis of the oxygen carriers were summarized and discussed. In addition, the current status of reactor process design was reviewed and potential issues were proposed in terms of the industrialization of CLRM. Finally, some existing challenges and future perspectives on the current studies of oxygen carriers for CLRM reactions were presented.

Key words: methane, chemical looping reforming, oxygen carrier, syngas, hydrogen

摘要：

甲烷化学链重整（CLRM）反应利用固体载氧体材料作为中间体，将传统甲烷重整反应分成还原和氧化两个反应，载氧体在这个过程中不断地被氧化还原，形成链式循环反应，实现了合成气或氢气的连续生产。相比传统重整反应而言，CLRM反应无须高成本的空分装置即可得到高纯度的产物。CLRM反应研究的关键在于载氧体的设计与选择，本文总结了近年来金属基载氧体（Ni、Fe、Cu、Co、Mn、Ce基）、复合型载氧体（包括钙钛矿和六铝酸盐）的最新研究进展，重点讨论了这些载氧体的组成、结构对反应性能的影响以及材料的设计与优化策略。进一步地，对载氧体的合成方法也做了总结和论述。此外，在甲烷化学链重整的工业化方面，探讨了反应器工艺流程设计的相关内容并提出了潜在问题。最后，对CLRM反应载氧体的研究现状提出了一些存在的挑战和未来的展望。

关键词: 甲烷, 化学链重整, 载氧体, 合成气, 氢气