Temperature- and pH-dependent mechanism of hydrogen production from hydrothermal reactions of sulfide
Temperature- and pH-dependent mechanism of hydrogen production from hydrothermal reactions of sulfide
复制标题
DOI：
10.1016/j.ijhydene.2012.10.013
复制
发表时间：
2012-12
影响因子：
7.2
通讯作者：
P. Setiani;N. Watanabe;Atsushi Kishita;N. Tsuchiya
中科院分区：
文献类型：
--
作者：
P. Setiani;N. Watanabe;Atsushi Kishita;N. Tsuchiya
在Hastelloy C-22反应器中，在pH 9-13和230 - 320 °C之间的温度下，在相应的饱和蒸汽压下，研究了pH和温度对以硫化物（HS-和S2-）作为水还原剂的碱性水溶液制氢的影响。在所有pH值下60分钟的反应时间在≥280 °C和相应的饱和蒸气压下产生显著量的氢气。产氢量随pH和温度的升高而增加，但随温度的升高而增加。硫化物的消耗量也随温度的升高而增加，但其对pH值的依赖性一般不显著。反应中产生的氢气与消耗的硫化物之比（mol/mol）为0.6-3.4，硫产物的量和/或氧化态随pH和温度的升高而增加。本研究的结果证实，在实验条件下，主要反应是pH值和温度依赖性的硫化物从水还原产生氢。该研究的结果还表明，基于硫化物再生过程，通过硫氧化还原循环的最佳制氢条件在300 °C和pH 13以及在320 °C和pH 11下进行了优化。
The effect of pH and temperature on hydrogen production from an aqueous alkaline solution with sulfide (HS−and S2−) as a reducing agent of water has been studied at pH 9–13 and at temperatures between 230 and 320 °C, under corresponding saturated vapor pressure, in a Hastelloy C-22 reactor. A reaction time of 60 min at all pH values produced a significant amount of hydrogen at ≥280 °C and corresponding saturated vapor pressures. Hydrogen production increased with both pH and temperature, but was more significant with temperature. Sulfide consumption also increased with temperature, but its pH dependence was generally insignificant. The ratio of hydrogen produced to sulfide consumed (mol/mol) was 0.6–3.4, and the amount and/or oxidation state of sulfur product increased with pH and temperature. Results of this study confirm that hydrogen is produced from water reduction by sulfide under the experimental conditions, where the predominant reaction was pH- and temperature-dependent. Results of this study also suggest that optimum hydrogen production conditions via a sulfur redox cycle, based on the sulfide regeneration process, is optimized at 300 °C and pH 13, and at 320 °C and pH 11.