Iron promoted MOF-derived carbon encapsulated NiFe alloy nanoparticles core-shell catalyst for CO2 methanation

被引:38
作者
Li, Yan-Ting [1 ]
Zhou, Lei [1 ]
Cui, Wen-Gang [1 ]
Li, Zhuo-Fei [1 ]
Li, Wei [1 ]
Hu, Tong -Liang [1 ]
机构
[1] Nankai Univ, Natl Inst Adv Mat, Sch Mat Sci & Engn, Tianjin 300350, Peoples R China
基金
中国国家自然科学基金;
关键词
Metal-organic framework (MOFs); NiFe alloy; Heterogeneous catalyst; Fe promoter; CO; 2; methanation; TOTAL-ENERGY CALCULATIONS; CHEMICAL-STATE; METAL; HYDROGENATION; DIOXIDE; GAS; CONVERSION; NI/AL2O3; PARTICLE; NI/CEO2;
D O I
10.1016/j.jcou.2022.102093
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The highly ordered and designable properties of MOFs make them competitive precursors to constructing highperformance catalysts for CO2 methanation, however, only a few studies have investigated the facilitation effect of promoters. Herein, a series of carbon encapsulated NiFe alloy nanoparticles core-shell catalysts (NixFe@C, x refers to the ratio of Ni to Fe) were successfully prepared by a method of pyrolyzing Ni-MOF-74 after impregnation in Fe3+ solution for CO2 hydrogenation to CH4, and their composition and structural characteristics were explored in detail by PXRD, N2 adsorption/desorption measurements, TEM, and XPS, etc. Fe-doped catalysts exhibited significantly enhanced CO2 methanation activity compared to the monometallic Ni catalysts, especially Ni7Fe@C, which reached 72.3 % CO2 conversion with CH4 selectivity of 99.3 % at 350 degrees C, and showed a CO2 conversion of 53.3 % at 300 degrees C, twice that of Ni@C. The specific effects of the Fe addition on the composition and structure of the catalysts were also investigated via a combination of experiments and DFT calculations, which indicates that appropriate incorporation of Fe was conducive to promoting the dispersion of metal particles and the adsorption ability of CO2 and CO, and thus resulted in significantly improved catalytic performance. This work provides a promising route for the rational design of MOF-derived CO2 methanation catalysts and makes a new attempt to investigate the influence of promoters.
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页数:10
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