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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >pH Oscillations in the BrO_3-SO_3~(2-)/HSO_3~-Reaction in a CSTR
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pH Oscillations in the BrO_3-SO_3~(2-)/HSO_3~-Reaction in a CSTR

机译：CSTR中BrO_3-SO_3〜（2-）/ HSO_3〜反应的pH振荡

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Large-amplitude pH oscillations have been measured during the oxidation of sulfur(IV)species by the bromate ion in aqueous solution in a continuous-flow stirred tank reactor in the absence of any additional oxidizing or reducing reagent.The source of the oscillation in this simple chemical reaction is a two-way oxidation of sulfur(IV)by the bromate ion:(1)the hydrogen-ion-producing self-accelerating oxidation to sulfur(VI)(SO_4~(2-)),and(2)a hydrogen-ion-consuming oxidation to sulfur(V)(S_2O_6~(2-)).In such a way,both the H~+-producing and H~+-consuming composite processes required for a pH oscillator take place in parallel in a reaction between two reagents in this system.A simple reaction scheme,consisting of the protonation equilibria of SO_3~(2-)and HSO_3~-,the oxidation of HSO_3~-and H_2SO_3 by BrO_3~ to SO_4~(2-),and the oxidation of H_2SO_3 to S_2O_6~(2-)has successfully been used to simulate the observed dynamical behavior.Simulation with this simple scheme shows that oscillations can be calculated even if only about 1% of sulfur(IV)is oxidized to S_2O_6~(2-)along with the main product SO_4~(2-).Agreement between calculated and measured dynamical behavior is found to be quite good.Increasing temperature decreases both the period length of oscillations in a CSTR and the Landolt time measured in a closed reactor.No temperature compensation of the oscillatory frequency is found in this reaction.
机译：在连续流搅拌釜反应器中，在水溶液中通过溴酸根离子在没有任何其他氧化或还原试剂的情况下，通过水溶液中的溴酸根离子氧化了硫（IV）物种时，已测量到大幅度的pH振荡。简单的化学反应是通过溴酸根离子对硫（IV）进行双向氧化：（1）产生氢离子的自加速氧化为硫（VI）（SO_4〜（2-）），和（2）氢离子氧化为硫（V）（S_2O_6〜（2-））。以这种方式，pH振荡器所需的产生H〜+和消耗H〜+的复合过程同时进行一个简单的反应方案，由SO_3〜（2-）和HSO_3〜-的质子平衡，BrO_3〜氧化HSO_3〜-和H_2SO_3到SO_4〜（2-）组成。 ，成功地将H_2SO_3氧化为S_2O_6〜（2-）来模拟观察到的动力学行为。即使只有大约1％的硫（IV）与主要产物SO_4〜（2-）一起氧化为S_2O_6〜（2-），也可以计算出ons。发现动力学行为的计算值与实测值之间的一致性很好。温度升高既降低了CSTR的振荡周期长度，也降低了在密闭反应器中测得的Landolt时间。在该反应中未发现振荡频率的温度补偿。

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