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首页> 外文期刊>Catalysis science & technology >Rational screening of single-atom-doped ZnO catalysts for propane dehydrogenation from microkinetic analysis
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Rational screening of single-atom-doped ZnO catalysts for propane dehydrogenation from microkinetic analysis

机译：合理筛选single-atom-doped氧化锌丙烷脱氢的催化剂microkinetic分析

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Supported single-atom catalysts, which bridge the gap between homogeneous and heterogeneous catalysis, have attained increasing interest because of their unique catalytic properties and behaviors. In this contribution, periodic DFT+U calculations have been carried out to explore the structural stability, catalytic activity, and selectivity of 13 M-1-ZnO (M = Mn-Cu, Ru-Ag, and Os-Au) catalysts in propane dehydrogenation (PDH). Calculated results indicate that the doped single atoms show high resistance to sintering on the ZnO surface. Except on Rh-1-, Os-1-, Ir-1-, and Pt-1-ZnO(10 (1) over bar0), a Lewis acid-base interaction occurs, which would greatly enhance the co-adsorption of a pair of amphoteric species on the oxides. The linear chemisorption energy and transition state energy scaling relations hold well for the C-H and H-H bond activation steps involved in the reaction network. Microkinetic analysis is used to determine the activity trend, and volcano-shaped plots of the turnover frequency for propylene production are obtained, with the formation energies of adsorbed H and 2-propyl used as two reactivity descriptors. By using the activation energy difference between propylene dehydrogenation and desorption as a measure of the catalyst selectivity, it is found that a high selectivity can only be achieved at the expense of catalytic activity. Comparison between the energy barriers for H-2 desorption and H2O formation indicates that the reduction of ZnO can be suppressed by single-atom doping. The Mn- and Cu-doped ZnO catalysts are suggested to be good catalyst candidates for PDH with lower cost, increased activity, and improved selectivity and catalytic stability.
机译：支持单原子催化剂,这桥同类和异类之间的差距催化作用,达到增加兴趣因其独特的催化性能行为。计算进行了探讨结构稳定性、催化活性和选择性13 M-1-ZnO (M = Mn-Cu Ru-Ag,Os-Au)丙烷脱氢的催化剂(PDH)。单个原子表现出高电阻烧结氧化锌表面。和Pt-1-ZnO (10 (1) bar0),路易斯酸碱发生相互作用,这将大大增强一双两性的co吸附物种在氧化物上。和过渡态能量比例关系持有的债券活化碳氢键和高度差所涉及的步骤的反应网络。Microkinetic分析是用来确定活动趋势,volcano-shaped阴谋的丙烯生产周转频率获得,形成吸附的能量2 -丙基作为H和两个反应描述符。丙烯脱氢和之间的区别解吸的催化剂选择性,发现高选择性只能实现催化为代价吗活动。2解吸和水形成可以抑制氧化锌的还原单原子掺杂的。催化剂是建议是很好的催化剂候选人PDH较低的成本,增加了活动,提高选择性和催化稳定。

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