Frequency response analysis of nonsuperimposable systems using a pseudo-transfer function: Application to systems with coverage-dependent adsorption
The concept of a pseudo-transfer function is introduced to characterize the frequency response behaviour of nonsuperimposable systems, i.e. those described by nonlinear differential equations or by linear differential equations with time-dependent coefficients. The pseudo-transfer function shapes ca...
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Published in | Chemical engineering science Vol. 41; no. 3; pp. 495 - 510 |
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Main Authors | , , |
Format | Journal Article |
Language | English |
Published |
Elsevier Ltd
1986
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Abstract | The concept of a pseudo-transfer function is introduced to characterize the frequency response behaviour of nonsuperimposable systems, i.e. those described by nonlinear differential equations or by linear differential equations with time-dependent coefficients. The pseudo-transfer function shapes can be used to match experimentally measured frequency response data to the most probable system model and to identify model parameters. The concepts are illustrated using a model system of coverage-dependent adsorption of the reactant on a partially exposed sample, followed by surface diffusion of the reactant and first-order chemical reaction in a modulated reactive molecular beam scattering experiment.
From an exact analysis of the example system, features of nonsuperimposable systems are inferred. Nonsuperimposable systems can cause both a cusp and an inflection at the first harmonic in the pseudo-transfer function. The cusp is distinguishable from that observed for a superimposable, parallel reaction mechanism in that its position depends on the chopping frequency and other experimentally controllable parameters. The inflection also depends on chopping frequency and is not observed in superimposable systems. Thus, the pseudo-transfer function can be a sensitive means for discriminating between entirely different mechanisms that lead to similar overall system behaviour. |
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AbstractList | The concept of a pseudo-transfer function is introduced to characterize the frequency response behaviour of nonsuperimposable systems, i.e. those described by nonlinear differential equations or by linear differential equations with time-dependent coefficients. The pseudo-transfer function shapes can be used to match experimentally measured frequency response data to the most probable system model and to identify model parameters. The concepts are illustrated using a model system of coverage-dependent adsorption of the reactant on a partially exposed sample, followed by surface diffusion of the reactant and first-order chemical reaction in a modulated reactive molecular beam scattering experiment.
From an exact analysis of the example system, features of nonsuperimposable systems are inferred. Nonsuperimposable systems can cause both a cusp and an inflection at the first harmonic in the pseudo-transfer function. The cusp is distinguishable from that observed for a superimposable, parallel reaction mechanism in that its position depends on the chopping frequency and other experimentally controllable parameters. The inflection also depends on chopping frequency and is not observed in superimposable systems. Thus, the pseudo-transfer function can be a sensitive means for discriminating between entirely different mechanisms that lead to similar overall system behaviour. |
Author | Schwartz, Jeffrey P. Sawin, Herbert H. Hatton, T.Alan |
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Cites_doi | 10.1002/kin.550080416 10.1002/cjce.5450470512 10.1002/cjce.5450470616 10.1016/0009-2509(74)80170-3 10.1016/0039-6028(77)90298-9 10.1016/0039-6028(74)90094-6 10.1016/0009-2509(83)85047-7 10.1002/cjce.5450480610 10.1016/0300-9467(79)80003-9 10.1116/1.571014 10.1002/aic.690100508 10.1116/1.1317055 10.1016/0009-2509(74)80159-4 10.1016/0009-2509(79)80026-3 10.1021/i260006a002 10.1016/0039-6028(74)90260-X 10.1016/0039-6028(78)90350-3 10.1016/0009-2509(75)85118-9 10.1016/0009-2509(84)80005-6 10.1016/0378-5963(79)90017-5 |
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Engng Sci. doi: 10.1016/0009-2509(75)85118-9 contributor: fullname: El-Rifai – year: 1969 ident: 10.1016/0009-2509(86)87031-2_BIB13 contributor: fullname: Olander – volume: 39 start-page: 1469 year: 1984 ident: 10.1016/0009-2509(86)87031-2_BIB20 article-title: Temperature effects on separate values of adsorption and surface reaction rates by dynamic studies publication-title: Chem. Engng Sci. doi: 10.1016/0009-2509(84)80005-6 contributor: fullname: Recasens – volume: 4th edn start-page: 360 year: 1975 ident: 10.1016/0009-2509(86)87031-2_BIB25 contributor: fullname: Wylie – volume: 3 start-page: 168 year: 1979 ident: 10.1016/0009-2509(86)87031-2_BIB4 article-title: Modulated molecular beam scattering from solid surfaces: the “pulse testing” method of analysis publication-title: Applic. Surface Sci. doi: 10.1016/0378-5963(79)90017-5 contributor: fullname: Chang |
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