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## [PDF] 210100 Einführungsgesetz zum schweizerischen Zivilgesetzbuch 1

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## [PDF] ZGB surface reaction model with high diffusion rates - CORE

for inclusion in Physics and Astronomy Publications by an authorized administrator of Iowa State University Digital Repository For more information

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### GB surface reaction model with hi

gh difffusion J ames W. EvansI owa State University, e vans@ameslab.govF ollow thi s and additional works at:,### F3/-&(5-%67%7))(83,<6%6752$38&6

%572*7,) -2/2+-'%/%1(,)0-'%/,<6-'6200216hThe c omplete bibliographic information for this item can be found at,### F3/-&(5-%67%7))(83,<6%6752$38&6

#### 25-1*250%7-2121,2:72'-7)7,-6-7

)03/)%6)9-6-7,### F3/-&(5-%67%7))(8,2:72'-7)

,70/ C-#### 657-'/)-6&528+,772<28*25*5))%1(23)1%'')66&<7,),<6-'6%1(6752120<%72:% 7%7)!1-9)56-7<-+

-7%/)326-725<7,%6&))1%'')37)(*25-1'/86-21-1 ,<6-'6%1(6752120<8&/-'%7-216&<%1%87,25-=)(%(0-1-675%7252*2: % 7%7)!1-9)56-7<-+-7%/)326-725<25025)-1*250%7-213 /)%6)'217%'7( -+-5)3-%67%7))(8 Z GB surface reaction model with high difffusion ratesA bstracthThe difffusionless ZGB (monomer-dimer) surface reaction model exhibits a discontinuous transition to a02120)

#### 5@32-621)(67%7):,)17,)*5%'7-212*02120)5%(62537-21%F)0376);'))(67,%6&))1'/

%-0)(7,%77,-675%16-7-216,-E672:-7,-1752(8'7-212*5%3-((-B86-212*7,)02120)563)'-)6252*&27,63) '-)6")6,2:7,-6-61277,)'%6)5)35)6)17-1+7,)63-12(%/5%7,)57,%17,)75%16-7-2132-1725)#### 48%/(-B86-215%7)62*&27,63)'-)6:)D1(7,%77,)75%16-7-2121/<6,-E672

?Di sciplinesB iological and Chemical Physics | PhysicsC ommentshThi s article is published as Evans, J. W. "ZGB surface reaction model with high difffusion rates."hTh e Journal of#### 98, no

. 3 (1993): 2463-2465, doi:#### 267)(:-7,3)50-66-21hThi

s article is available at Iowa State University Digital Repository:,### F3/-&(5-%67%7))(83,<6%6752$38&6

ZGB surface reaction model with high diffusion rates### J. W. Evans

Ames Laboratory and Department of Mathematics, Iowa State University, Ames, Iowa 50011 (Received 22 October 1992; accepted 18 November 1992) The diffusionless ZGB (monomer-dimer) surface reaction model exhibits a discontinuous transition to a monomer-poisoned state when the fraction of monomer adsorption attempts exceeds 0.525. It has been claimed that this transition shifts to 2/3 with introduction of rapid diffusion of the monomer species, or of both species. We show this is not the case, 2/3 representing the spinodal rather than the transition point. For equal diffusion rates of both species, we find that the transition only shifts to 0.5951 ± 0.0002.### SinceS

its introduction in 1986, there has been much interest in the diffusionless ZGB (monomer-dimer) sur face reaction model, I primarily focusing on the "kinetic phase transitions" which it supports. 2-5### In this model,

monomers (A) adsorb at single empty sites (*) on an infinite square lattice at rate PA, dimers (B 2) absorb at adjacent pairs of empty sites at rate P B= 1-P A' and differ ent species adsorbed on adjacent sites react instanta neously. Schematically, one has### A(g) +*->A(ad),

### B2(g) +2*->2B(ad), A(ad) +B(ad) ->AB(g).

Here, "g" denotes gas phase and "ad" denotes adsorbed species.### The model supports a reactive steady state for PI

zmkpvnSyP-ymkrorzPocSand exhibits a continuous transi tion to a B-poisoned phase at "low" PA=PI> and a discon tinuous transition to an A-poisoned phase at "high" PA zPo·S In actual surface reactions, diffusion rates for one or more reactant species typically dominate adsorption rates. Such diffusion has the effect of "mixing" adsorbed species, reducing spatial correlations, and validating the traditional "mean-field" treatment of the chemical kinetics. What is perhaps less clear is that such diffusion reduces the effect of fluctuations, thus enhancing metastability and hysteresis. 4,6 Subsequent studies of the ZGB model have considered (i) the influence of diffusion of A(ad) and B(ad) with equal rates;7,8 and (ii) the influence of diffusion of A(ad), with### B(ad) still immobile.

9,10### The motivation for (ii) is in ap

plication of this model to the study of CO-oxidation where CO(ad) [represented by A(ad)] is highly mobile, and O(ad) [represented by B(ad)] is relatively immobile. In both cases, the claim has been made 8 ,10 that the discontin uous transition is shifted to the "stoichiometric point" P A =2/3 (Le., P2 i|S2/3), in the regime oflarge diffusion rates. We show that this is not correct. Instead we find that P2->0.5951 ±O.OOO2 for (i) through a direct analysis of behavior in this important limiting regime.### Here we concentrate on case (i). The approach of

Refs. 7 and 8 is to introduce into the lattice-gas simulations hopping at rate h per adspecies of either type and to de termine the shifts in PI and P2, as h increases. It is found that PI quickly decreases to zero for h;:::;3, and that P2 increases toward 2/3. However such calculations are ex-pensive for large h, and strong metastability leads to over estimation ofp2' as we describe below. Thus here we adopt the alternative strategy of directly analyzing the high dif fusion regime, noting that large diffusion rates of both spe cies ensure simple mean-field behavior is displayed. Hence forth, we denote concentrations or coverages of A(ad) by### A, and of B(ad) by B.

We consider first the kinetics for a system which is spatially homogeneous.### For infinite reaction rate, in the

limit of diverging hop rate, h, there can only be one type of reactant species present on the surface at any time. Sup pose first that this species is A. Then since the adsorption rate of A iSPA(1-A), and that of B iSPB(1-A)2 (given the adlayer is random), it follows that (1) Thus for hlp B> 2, one finds that A (t) -> 1 for any initial value, A (0), of A. For PAl PSfffyohSone finds that A (t) -> mSif A (0) < 1 -Alp B (and thereafter B increases as described below),### A(t)->l if A(O) > l-}PAlpB' and A(O)

= 1-}P -lpSB corresponds to an unstable steady state. If B is the species present on the surface, then clearly (2) Thus for PAlpB> 2, one finds that B(t)->O if B(O)### B=O) and the reactive phase f3 (B=l-jp

AIPB' P hysics and Astronomy Publications ,<6-'6%1(6752120< Z### GB surface reaction model with hi

gh difffusion J ames W. EvansI owa State University, e vans@ameslab.govF ollow thi s and additional works at:,### F3/-&(5-%67%7))(83,<6%6752$38&6

%572*7,) -2/2+-'%/%1(,)0-'%/,<6-'6200216hThe c omplete bibliographic information for this item can be found at,### F3/-&(5-%67%7))(83,<6%6752$38&6

#### 25-1*250%7-2121,2:72'-7)7,-6-7

)03/)%6)9-6-7,### F3/-&(5-%67%7))(8,2:72'-7)

,70/ C-#### 657-'/)-6&528+,772<28*25*5))%1(23)1%'')66&<7,),<6-'6%1(6752120<%72:% 7%7)!1-9)56-7<-+

-7%/)326-725<7,%6&))1%'')37)(*25-1'/86-21-1 ,<6-'6%1(6752120<8&/-'%7-216&<%1%87,25-=)(%(0-1-675%7252*2: % 7%7)!1-9)56-7<-+-7%/)326-725<25025)-1*250%7-213 /)%6)'217%'7( -+-5)3-%67%7))(8 Z GB surface reaction model with high difffusion ratesA bstracthThe difffusionless ZGB (monomer-dimer) surface reaction model exhibits a discontinuous transition to a02120)

#### 5@32-621)(67%7):,)17,)*5%'7-212*02120)5%(62537-21%F)0376);'))(67,%6&))1'/

%-0)(7,%77,-675%16-7-216,-E672:-7,-1752(8'7-212*5%3-((-B86-212*7,)02120)563)'-)6252*&27,63) '-)6")6,2:7,-6-61277,)'%6)5)35)6)17-1+7,)63-12(%/5%7,)57,%17,)75%16-7-2132-1725)#### 48%/(-B86-215%7)62*&27,63)'-)6:)D1(7,%77,)75%16-7-2121/<6,-E672

?Di sciplinesB iological and Chemical Physics | PhysicsC ommentshThi s article is published as Evans, J. W. "ZGB surface reaction model with high difffusion rates."hTh e Journal of#### 98, no

. 3 (1993): 2463-2465, doi:#### 267)(:-7,3)50-66-21hThi

s article is available at Iowa State University Digital Repository:,### F3/-&(5-%67%7))(83,<6%6752$38&6

ZGB surface reaction model with high diffusion rates### J. W. Evans

Ames Laboratory and Department of Mathematics, Iowa State University, Ames, Iowa 50011 (Received 22 October 1992; accepted 18 November 1992) The diffusionless ZGB (monomer-dimer) surface reaction model exhibits a discontinuous transition to a monomer-poisoned state when the fraction of monomer adsorption attempts exceeds 0.525. It has been claimed that this transition shifts to 2/3 with introduction of rapid diffusion of the monomer species, or of both species. We show this is not the case, 2/3 representing the spinodal rather than the transition point. For equal diffusion rates of both species, we find that the transition only shifts to 0.5951 ± 0.0002.### SinceS

its introduction in 1986, there has been much interest in the diffusionless ZGB (monomer-dimer) sur face reaction model, I primarily focusing on the "kinetic phase transitions" which it supports. 2-5### In this model,

monomers (A) adsorb at single empty sites (*) on an infinite square lattice at rate PA, dimers (B 2) absorb at adjacent pairs of empty sites at rate P B= 1-P A' and differ ent species adsorbed on adjacent sites react instanta neously. Schematically, one has### A(g) +*->A(ad),

### B2(g) +2*->2B(ad), A(ad) +B(ad) ->AB(g).

Here, "g" denotes gas phase and "ad" denotes adsorbed species.### The model supports a reactive steady state for PI

zmkpvnSyP-ymkrorzPocSand exhibits a continuous transi tion to a B-poisoned phase at "low" PA=PI> and a discon tinuous transition to an A-poisoned phase at "high" PA zPo·S In actual surface reactions, diffusion rates for one or more reactant species typically dominate adsorption rates. Such diffusion has the effect of "mixing" adsorbed species, reducing spatial correlations, and validating the traditional "mean-field" treatment of the chemical kinetics. What is perhaps less clear is that such diffusion reduces the effect of fluctuations, thus enhancing metastability and hysteresis. 4,6 Subsequent studies of the ZGB model have considered (i) the influence of diffusion of A(ad) and B(ad) with equal rates;7,8 and (ii) the influence of diffusion of A(ad), with### B(ad) still immobile.

9,10### The motivation for (ii) is in ap

plication of this model to the study of CO-oxidation where CO(ad) [represented by A(ad)] is highly mobile, and O(ad) [represented by B(ad)] is relatively immobile. In both cases, the claim has been made 8 ,10 that the discontin uous transition is shifted to the "stoichiometric point" P A =2/3 (Le., P2 i|S2/3), in the regime oflarge diffusion rates. We show that this is not correct. Instead we find that P2->0.5951 ±O.OOO2 for (i) through a direct analysis of behavior in this important limiting regime.### Here we concentrate on case (i). The approach of

Refs. 7 and 8 is to introduce into the lattice-gas simulations hopping at rate h per adspecies of either type and to de termine the shifts in PI and P2, as h increases. It is found that PI quickly decreases to zero for h;:::;3, and that P2 increases toward 2/3. However such calculations are ex-pensive for large h, and strong metastability leads to over estimation ofp2' as we describe below. Thus here we adopt the alternative strategy of directly analyzing the high dif fusion regime, noting that large diffusion rates of both spe cies ensure simple mean-field behavior is displayed. Hence forth, we denote concentrations or coverages of A(ad) by### A, and of B(ad) by B.

We consider first the kinetics for a system which is spatially homogeneous.### For infinite reaction rate, in the

limit of diverging hop rate, h, there can only be one type of reactant species present on the surface at any time. Sup pose first that this species is A. Then since the adsorption rate of A iSPA(1-A), and that of B iSPB(1-A)2 (given the adlayer is random), it follows that (1) Thus for hlp B> 2, one finds that A (t) -> 1 for any initial value, A (0), of A. For PAl PSfffyohSone finds that A (t) -> mSif A (0) < 1 -Alp B (and thereafter B increases as described below),### A(t)->l if A(O) > l-}PAlpB' and A(O)

= 1-}P -lpSB corresponds to an unstable steady state. If B is the species present on the surface, then clearly (2) Thus for PAlpB> 2, one finds that B(t)->O if B(O)### B=O) and the reactive phase f3 (B=l-jp

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