期刊
CATALYSIS SCIENCE & TECHNOLOGY
卷 9, 期 18, 页码 5058-5076出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c9cy01543d
关键词
-
资金
- Catalysis Center for Energy Innovation, a U.S. Department of Energy - Energy Frontier Research Center [DE-SC0001004]
Catalytic reactions on surfaces with forced oscillations in physical or electronic properties undergo controlled acceleration consistent with the selected parameters of frequency, amplitude, and external stimulus waveform. In this work, the general reaction of reversible A-to-B chemistry is simulated by varying the catalytic (heat of reaction, transition state and intermediate energies) and oscillation parameters (frequency, amplitude, endpoints, and waveform) to evaluate the influence on the overall catalytic turnover frequency and steady state extent of conversion. Variations of catalytic cycle energies are shown to comprise a superVolcano of superimposed individual Balandin-Sabatier volcano plots, with variations in linear scaling relationships leading to unique turnover frequency response to forced oscillation of the catalyst surface. Optimization of catalytic conditions identified a band of forced oscillation frequencies leading to resonance and rate enhancement as high as 10 000x above the static Sabatier maximum. Dynamic catalytic reactions conducted at long times achieved oscillatory steady state differing from equilibrium consistent with the imposed surface oscillation amplitude acting as a 'catalytic pump' relative to the Gibbs free energy of reaction.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据