Chemical looping steam methane reforming (CL-SMR) is a promising technology for co-producing syngas and pure hydrogen without additional purification processes. As a typical gas-solid reaction, the size and geometry of oxygen carriers strongly influence the dynamic conditions of this process, especially for large-scale application. In the present work, we prepared the monolithic oxygen carrier using Ce-Fe-Zr-O(40wt%)/MgO as active component and cordierite honeycomb as structural support by a slurry coating method, and their activity for CL-SMR were compared with the pellet ones. The monolithic oxygen carrier shows higher activity for both methane oxidation and water splitting than pellet oxygen carriers, which results in much higher CH₄ conversion (63.2% vs. 52.9%) and yields of syngas (2.85 mol·kg^-1) and hydrogen (1.14mol·kg^-1). The honeycomb also enhances the resistance to carbon deposition during methane selective oxidation, which helps to prolong the running cycle of CL-SMR and improve the purity of produced H₂. The comparison on the morphology of the cross section of the fresh and cycled monolithic oxygen carriers indicates that the oxygen carrier particles on the inner-surface of honeycomb channels are very stable during the long-term cycling. These results highlight the significance of designing a high-performance oxygen carrier by using a honeycomb support.

化学循环蒸汽甲烷重整（CL-SMR）是一种有前途的技术，可用于联合生产合成气和纯氢而无需其他纯化工艺。作为典型的气固反应，氧气载体的大小和几何形状会强烈影响此过程的动态条件，尤其是对于大规模应用而言。在本工作中，我们以浆液涂覆法制备了以Ce-Fe-Zr-O（40wt％）/ MgO为活性成分和堇青石蜂窝体为结构载体的整体式氧载体，并将其对CL-SMR的活性进行了比较。颗粒的。整体式氧气载体对甲烷氧化和水分解的活性均高于粒状氧气载体，从而导致CH ₄转化率更高（63.2％对52.9％）和合成气产率（2.85 mol·kg）^-1）和氢（1.14mol·kg ^-1）。蜂窝还增强了甲烷选择性氧化过程中对碳沉积的抵抗力，这有助于延长CL-SMR的运行周期并提高产生的H ₂的纯度。对新鲜的和循环的整体式氧气载体的横截面形态的比较表明，在长期循环过程中，蜂窝状通道内表面上的氧气载体颗粒非常稳定。这些结果突出了通过使用蜂窝状载体设计高性能氧气载体的重要性。