Hao Liu , Bingxian Chu , Tianxiang Chen , Jie Zhou , Lihui Dong , Tsz Woon Benedict Lo , Bin Li , Xiaohui He , Hongbing Ji
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引用次数: 0
摘要
将金属从纳米颗粒分散成团簇或单原子通常会表现出独特的特性,例如抑制结构敏感的副反应。在此,我们报告了使用离子交换(IE)方法和直接氢还原法在硅酸锌上实现 Co 物种的高度分散。获得的 2Co/Zn-4-IE 催化剂在 25% 丙烷和 75% 氮气气氛中进行 550 °C 丙烷脱氢反应时,丙烷的初始转化率为 41.4%。通过像差校正扫描透射电子显微镜观察到了特定环(α-α、β-β 和 delta-δ)中 Co 物种的存在。一系列傅立叶变换红外光谱证实了硅酸锌中特定羟基对 Co 的锚定作用,以及 Co 的特定配位环境和它在环中基本上作为单一位点的存在。密度泛函理论计算也证实了 Zn 框架对微环境的调节作用以及 Co 物种作为路易斯酸活性位点(Co-O4)的存在。
Modulation of the cobalt species state on zincosilicate to maximize propane dehydrogenation to propylene
Dispersing metals from nanoparticles into clusters or single atoms often exhibits unique properties such as the inhibition of structure-sensitive side reactions. Here, we reported the use of ion exchange (IE) methods and direct hydrogen reduction to achieve high dispersion of Co species on zincosilicate. The obtained 2Co/Zn-4-IE catalyst achieved an initial propane conversion of 41.4% at a temperature of 550 °C in a 25% propane and 75% nitrogen atmosphere for propane dehydrogenation. Visualization of the presence of Co species within specific rings (alpha-α, beta-β and delta-δ) was obtained by aberration-corrected scanning transmission electron microscopy. A series of Fourier transform infrared spectra confirmed the anchoring of Co by specific hydroxyl groups in zincosilicate and the specific coordination environment of Co and its presence in the rings essentially as a single site. The framework Zn for the modulation of the microenvironment and the presence of Co species as Lewis acid active sites (Co-O4) was also supported by density functional theory calculations.
期刊介绍:
The journal covers a broad scope, encompassing new trends in catalysis for applications in energy production, environmental protection, and the preparation of materials, petroleum chemicals, and fine chemicals. It explores the scientific foundation for preparing and activating catalysts of commercial interest, emphasizing representative models.The focus includes spectroscopic methods for structural characterization, especially in situ techniques, as well as new theoretical methods with practical impact in catalysis and catalytic reactions.The journal delves into the relationship between homogeneous and heterogeneous catalysis and includes theoretical studies on the structure and reactivity of catalysts.Additionally, contributions on photocatalysis, biocatalysis, surface science, and catalysis-related chemical kinetics are welcomed.