CONFIRMATION OF HIGH FLOW-RATE CHAOS IN THE BELOUSOV-ZHABOTINSKY REACTION

被引:57
作者
GYORGYI, L
FIELD, RJ
NOSZTICZIUS, Z
MCCORMICK, WD
SWINNEY, HL
机构
[1] UNIV MONTANA,DEPT CHEM,MISSOULA,MT 59812
[2] UNIV TEXAS,CTR NONLINEAR DYNAM,AUSTIN,TX 78712
[3] UNIV TEXAS,DEPT PHYS,AUSTIN,TX 78712
[4] EOTVOS LORAND UNIV,INST INORGAN & ANALYT CHEM,H-1528 BUDAPEST,HUNGARY
[5] TECH UNIV BUDAPEST,DEPT CHEM PHYS,H-1521 BUDAPEST,HUNGARY
关键词
D O I
10.1021/j100182a038
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Past experiments and simulations on the Belousov-Zhabotinsky (BZ) reaction clearly demonstrated the existence of chaos in stirred flow reactors at low flow rates. However, the existence of chaos at high flow rates has remained the subject of controversy. The controversy is resolved by the present experiments at high flow rates, which accurately reproduce the complex sequence of periodic, complex periodic, and chaotic states observed by Hudson and co-workers (Hudson et al., 1979; Hudson and Mankin, 1981); the flow rates observed here for the different dynamical regimes agree with those of Hudson et al. within a few percent. This striking reproducibility of the complex periodic and chaotic dynamics is found to be insensitive to stirring rate, size of the reactor, purity of the reagents, temperature, and type of pumping (peristaltic or piston pumps, premixed or nonpremixed feeds). Moreover, the observed sequence is reproduced qualitatively by a four-variable model of the BZ reaction. Thus, this work provides definitive evidence for the existence of deterministic chaos in the BZ reaction at high flow rates. We conclude that past descriptions of aperiodic behavior at high flow rates in terms of various stochastic mechanisms, including incomplete mixing or switching between adjacent periodic states, are inappropriate for the conditions of the Hudson's experiments.
引用
收藏
页码:1228 / 1233
页数:6
相关论文
共 33 条
[1]   FROM QUASI-PERIODICITY TO CHAOS IN THE BELOUSOV-ZHABOTINSKII REACTION .1. EXPERIMENT [J].
ARGOUL, F ;
ARNEODO, A ;
RICHETTI, P ;
ROUX, JC .
JOURNAL OF CHEMICAL PHYSICS, 1987, 86 (06) :3325-3338
[2]  
Belousov B. P., 1958, SB REF RADIATS MED C, P145
[3]   UNIVERSALITY, MULTIPLICITY, AND THE EFFECT OF IRON IMPURITIES IN THE BELOUSOV-ZHABOTINSKII REACTION [J].
COFFMAN, KG ;
MCCORMICK, WD ;
NOSZTICZIUS, Z ;
SIMOYI, RH ;
SWINNEY, HL .
JOURNAL OF CHEMICAL PHYSICS, 1987, 86 (01) :119-129
[4]  
Field RJ., 1985, OSCILLATIONS TRAVELI
[5]   CHEMICAL OSCILLATIONS AND INSTABILITIES .44. A DISCREPANCY BETWEEN EXPERIMENTAL AND COMPUTATIONAL EVIDENCE FOR CHEMICAL CHAOS [J].
GANAPATHISUBRAMANIAN, N ;
NOYES, RM .
JOURNAL OF CHEMICAL PHYSICS, 1982, 76 (04) :1770-1774
[6]  
GRAY P, 1990, CHEM OSCILLATIONS IN
[7]  
GYORGYI L, 1990, J CHEM PHYS, V93, P2159, DOI 10.1063/1.459046
[8]   APERIODICITY RESULTING FROM 2-CYCLE COUPLING IN THE BELOUSOV-ZHABOTINSKII REACTION .2. MODELING OF THE EFFECT OF DEAD SPACES AT THE INPUT PORTS OF A CONTINUOUS-FLOW STIRRED TANK REACTOR [J].
GYORGYI, L ;
FIELD, RJ .
JOURNAL OF PHYSICAL CHEMISTRY, 1989, 93 (07) :2865-2867
[9]   SIMPLE-MODELS OF DETERMINISTIC CHAOS IN THE BELOUSOV-ZHABOTINSKY REACTION [J].
GYORGYI, L ;
FIELD, RJ .
JOURNAL OF PHYSICAL CHEMISTRY, 1991, 95 (17) :6594-6602
[10]   A NOVEL MODEL FOR THE SIMULATION OF CHAOS IN LOW-FLOW-RATE CSTR EXPERIMENTS WITH THE BELOUSOV ZHABOTINSKY REACTION - A CHEMICAL MECHANISM FOR 2 FREQUENCY OSCILLATIONS [J].
GYORGYI, L ;
REMPE, SL ;
FIELD, RJ .
JOURNAL OF PHYSICAL CHEMISTRY, 1991, 95 (08) :3159-3165