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A novel Ni–MoCxOy interfacial catalyst for syngas production via the chemical looping dry reforming of methane
Chem ( IF 23.5 ) Pub Date : 2022-10-04 , DOI: 10.1016/j.chempr.2022.09.007
Xiao Zhang , Yao Xu , Yang Liu , Liang Niu , Yanan Diao , Zirui Gao , Bingbing Chen , Jinglin Xie , Mingshu Bi , Meng Wang , Dequan Xiao , Ding Ma , Chuan Shi

Modulating the oxygen-metal interface that enables efficient and selective C–H activation remains challenging. Herein, we present a novel MoCxOy oxygen carrier for syngas production via the chemical looping CH4–CO2 reforming (CL-DRM) reaction. Molybdenum carbide additive induces the re-dispersion of Ni particles from Al2O3 surface to α-MoC driven by the strong interaction between Ni and α-MoC. A dynamic structure transformation between MoCx and MoCxOy occurs and new Ni–MoCxOy interfaces form during the redox cycling, which is discovered to be crucial for the low-temperature CH4 activation using surface construction experiments and in-situ spectroscopic methods. As a result, Ni–(α-MoC)/Al2O3 exhibits near 100% selectivity to syngas with a H2/CO ratio of 2:1 at 500°C, which is a significantly lower temperature than that of conventional systems. This study first employs molybdenum carbide as an oxygen storage material (OSM) in CL-DRM reaction, paving the way of utilizing transition metal carbides as OSMs in chemical looping processes.



中文翻译:

一种新型 Ni-MoCxOy 界面催化剂用于甲烷化学链干重整生产合成气

调节氧-金属界面以实现高效和选择性的 C-H 活化仍然具有挑战性。在此,我们提出了一种新型 MoC x O y氧载体,用于通过化学循环 CH 4 –CO 2重整 (CL-DRM) 反应生产合成气。在 Ni 和 α-MoC 之间的强相互作用的驱动下,碳化钼添加剂诱导 Ni 颗粒从 Al 2 O 3表面重新分散到 α-MoC。MoC x和 MoC x O y之间发生动态结构转变,新的 Ni–MoC x O y界面在氧化还原循环过程中形成,使用表面构造实验和原位光谱方法发现这对于低温 CH 4活化至关重要。因此,Ni–(α-MoC)/Al 2 O 3在 500°C 下对 H 2 /CO 比为 2:1 的合成气表现出接近 100% 的选择性,这明显低于传统系统的温度. 该研究首先在 CL-DRM 反应中采用碳化钼作为储氧材料 (OSM),为在化学链过程中利用过渡金属碳化物作为 OSM 铺平了道路。

更新日期:2022-10-04
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