Apparent kinetics of the Bunsen reaction in I-2/HI solution for the iodine-sulfur hydrogen production process

Apparent kinetics of the Bunsen reaction in I-2/HI solution for the iodine-sulfur hydrogen production process
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I-2/HI 溶液中碘-硫制氢过程中本生反应的表观动力学

DOI:
10.1016/j.ijhydene.2017.04.117
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发表时间:
2017-06
影响因子:
7.2
通讯作者:
Chen Songzhe
Chen Songzhe
中科院分区:
工程技术2区
文献类型:
--
作者:
Zhou Chenglin;Zhang Ping;Wang Laijun;Chen Songzhe

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以高效、无二氧化碳、低成本为特征的大规模氢气生产是氢经济面临的严峻挑战。通过热化学碘-硫(IS)工艺生产核氢是一种潜在的候选方法。化学反应动力学数据对于开发高性能的反应器以及放大该工艺是必不可少的。用初速度法研究了该反应在模拟循环条件下的表观动力学。通过测量SO2压力随反应时间的变化,系统地考察了搅拌速度、SO2分压、I2浓度、反应温度等关键参数对反应速率的影响。初始速率分析方法表明,本生反应速率与SO2压力和I2浓度的关系分别为0.23±0.01和0.77±0.0.01个数量级。表观活化能为5.86±0.21kJ/mol。在此基础上,建立了本森反应的指数速率表达式。此外,还提出了一种简化的动力学参数计算方法,并与常规方法进行了比较。实验结果为本生反应器的设计和研制以及阐明反应过程提供了理论依据。
Massive hydrogen production featuring high efficiency, CO2free, and cost effectiveness is a crucial challenge for the hydrogen economy. Nuclear hydrogen production through thermochemical iodine–sulfur (IS) process is a potential candidate for this purpose. Chemical reaction kinetics data are indispensable for developing a high-performance reactor as well as the scaling up of the process. The apparent kinetics of the reaction under simulated recycling conditions of IS closed cycle operation was studied by initial rate method. The effects of key parameters, including agitation speed, SO2partial pressure, I2concentration, and reaction temperature, on reaction rate, were systematically investigated by measuring the variation in SO2pressure with reaction time. Initial rate analysis method indicated that the Bunsen reaction rates were 0.23 ± 0.01 and 0.77 ± 0.01 order with respect to SO2pressure and I2concentration. The apparent activation energy was 5.86 ± 0.21 kJ/mol. Based on these results, an exponential rate expression of the Bunsen reaction was established. In addition, a simplified method for calculation of kinetics parameters was proposed and compared with conventional techniques. Experimental results provide theoretical basis for design and development of Bunsen reactors and for elucidating the reaction process.
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