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Plasma-assisted Co/Zr-metal organic framework catalysis of CO2 hydrogenation: influence of Co precursors
Plasma Science and Technology ( IF 1.6 ) Pub Date : 2021-04-26 , DOI: 10.1088/2058-6272/abeed9
Yanqin LI , Jing ZHAO , Decai BU , Xulei ZHANG , Teng PENG , Lanbo DI , Xiuling ZHANG

In this study, Co/Zr-metal organic framework (MOF) precursors were obtained by a room-temperature liquid-phase precipitation method and the equivalent-volume impregnation method, respectively, using a Zr-MOF as the support, and Co/Zr-MOF-M and Co/Zr-MOF-N catalysts were prepared after calcination in a hydrogen–argon mixture gases (${V}_{{\rm{Ar}}}:{V}_{{{\rm{H}}}_{{\rm{2}}}}=9:1$) at 350 C for 2 h. The catalytic activities of the prepared samples for CO2 methanation under atmospheric-pressure cold plasma were studied. The results showed that Co/Zr-MOF-M had a good synergistic effect with cold plasma. At a discharge power of 13.0 W, ${V}_{{{\rm{H}}}_{2}}:{V}_{{{\rm{CO}}}_{2}}=4:1$ and a gas flow rate of 30 mlmin−1, the CO2 conversion was 58.9% and the CH4 selectivity reached 94.7%, which was higher than for Co/Zr-MOF-N under plasma (CO2 conversion 24.8%, CH4 selectivity 9.8%). X-ray diffraction, scanning electron microscopy, transmission electron microscopy, N2 adsorption and desorption (Brunauer–Emmett–Teller) and x-ray photoelectron spectroscopy analysis results showed that Co/Zr-MOF-M and Co/Zr-MOF-N retained a good Zr-MOF framework structure, and the Co oxide was uniformly dispersed on the surface of the Zr-MOF. Compared with Co/Zr-MOF-N, the Co/Zr-MOF-M catalyst has a larger specific surface area and higher Co2+/Cototal and Co/Zr ratios. Additionally, the Co oxide in Co/Zr-MOF-M is distributed on the surface of the Zr-MOF in the form of porous particles, which may be the main reason why the catalytic activity of Co/Zr-MOF-M is higher than that of Co/Zr-MOF-N.



中文翻译:

等离子体辅助 Co/Zr-金属有机骨架催化 CO 2加氢:Co 前驱体的影响

本研究以Zr-MOF为载体,分别采用室温液相沉淀法和等体积浸渍法制备Co/Zr-金属有机骨架(MOF)前驱体,Co/Zr -MOF-M 和 Co/Zr-MOF-N 催化剂是在氢气-氩气混合气体 ( ${V}_{{\rm{Ar}}}:{V}_{{{\rm{H}}}_{{\rm{2}}}}=9:1$) 中在 350 C 下煅烧 2 小时后制备的。研究了制备的样品在常压冷等离子体下对CO 2甲烷化的催化活性。结果表明,Co/Zr-MOF-M与冷等离子体具有良好的协同作用。在 13.0 W 的放电功率${V}_{{{\rm{H}}}_{2}}:{V}_{{{\rm{CO}}}_{2}}=4:1$和 30 mlmin -1的气体流速下,CO 2转化率为 58.9%,CH 4选择性达到94.7%,高于等离子体下的Co/Zr-MOF-N(CO 2转化率24.8%,CH 4选择性9.8%)。X 射线衍射、扫描电子显微镜、透射电子显微镜、N 2吸附和解吸(Brunauer-Emmett-Teller)和 X 射线光电子能谱分析结果表明 Co/Zr-MOF-M 和 Co/Zr-MOF-N保留了良好的 Zr-MOF 骨架结构,Co 氧化物均匀分散在 Zr-MOF 表面。与Co/Zr-MOF-N相比,Co/Zr-MOF-M催化剂具有更大的比表面积和更高的Co 2+ /Co总量和 Co/Zr 比率。此外,Co/Zr-MOF-M中的Co氧化物以多孔颗粒的形式分布在Zr-MOF的表面,这可能是Co/Zr-MOF-M催化活性较高的主要原因与 Co/Zr-MOF-N 相比。

更新日期:2021-04-26
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