催化作用
过渡金属
离解(化学)
氮化物
材料科学
金属
氧气
分解
空间速度
无机化学
化学
化学工程
物理化学
冶金
纳米技术
选择性
有机化学
工程类
图层(电子)
作者
Yichao Wu,Zhiwei Xie,Xiaofeng Gao,Xian Zhou,Yangzhi Xu,Shurui Fan,Siyu Yao,Xiaonian Li,Lili Lin
标识
DOI:10.1016/j.cjche.2021.12.022
摘要
Three transition metal-like facet centered cubic structured transition metal nitrides, γ-Mo2N, β-W2N and δ-NbN, are synthesized and applied in the reaction of CO2 hydrogenation to CO. Among the three nitride catalysts, the γ-Mo2N exhibits superior activity to target product CO, which is 4.6 and 76 times higher than the other two counterparts of β-W2N and δ-NbN at 600 °C, respectively. Additionally, γ-Mo2N exhibits excellent stability on both cyclic heating–cooling and high space velocity steady state operation. The deactivation degree of cyclic heating–cooling evaluation after 5 cycles and long-term stability performance at 773 and 873 K in 50 h are all less than 10%. In-situ XRD and kinetic studies suggest that the γ-Mo2N itself is able to activate both of the reactants CO2 and H2. Below 400 °C, the reaction mainly occurs at the surface of γ-Mo2N catalyst. CO2 and H2 competitively adsorbe on the surface of catalyst and CO2 is the relatively stronger surface adsorbate. At a higher temperature, the interstitial vacancies of the γ-Mo2N can be reversibly filled with the oxygen from CO2 dissociation. Both of the surface and bulk phase sites of γ-Mo2N participate in the high temperature CO2 hydrogenation pathway.
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