小型商用车
材料科学
催化作用
甲醇
甲烷
氧化还原
金属有机骨架
星团(航天器)
密度泛函理论
金属
无机化学
物理化学
化学
计算化学
有机化学
冶金
吸附
程序设计语言
计算机科学
作者
Melissa Barona,Randall Q. Snurr
标识
DOI:10.1021/acsami.0c06241
摘要
Density functional theory is used to study the tunability of trigonal prismatic SBUs found in metal–organic frameworks (MOFs) such as MIL-100, MIL-101, and PCN-250/MIL-127 of chemical composition M3+2M2+(μ3-O)(RCOO)6 for the partial oxidation of methane to methanol. We performed a combinatorial screening by varying the composition of the trimetallic node (M13+)2(M22+) (where M1 and M2 = V, Cr, Mn, Fe, Co, and Ni) and calculated the reaction pathway on both M1 and M2 sites. The systematic replacement of metals in the trimetallic cluster allowed us to study the influence of spectator atoms on the catalytic activity of a specific metal site in the cluster toward the N2O activation and C–H bond activation steps of the reaction. In the screening, we identified the top-performing node compositions with predicted barriers lower than those already reported for experimentally tested MOFs with trigonal prismatic SBUs. This work demonstrates the opportunity to tune the catalytic activity of MOFs for redox reactions by changing their metal node composition.
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