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Optimization of the electrooxidation of aqueous ammonium sulfite for hydrogen production at near-neutral pH using response surface methodology

机译:响应面法测定近中性pH氢气生产水溶液的电氧化优化

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Sulfur-based thermochemical cycles, such as the hybrid sulfur-ammonia (HySA) cycle, offer a valuable approach in which hydrogen is produced by exploiting sulfur dioxide (potentially pollutant emissions) through the electrochemical oxidation of aqueous sulfite. In this study, the effect of pH on electrooxidation rate was assessed by comparing different reaction scenarios. Then, a Central Composite Design (CCD) combined with a Response Surface Methodology (RSM) was used to optimize batch electrooxidation of ammonium sulfite at near-neutral pH. Results show that the use of an anion exchange membrane (AEM) greatly improves sulfite electrooxidation rate while pH is effectively stabilized. Furthermore, a second-order model that relates applied potential and sulfite concentration with the normalized half-life of the reaction was obtained and verified experimentally at long-term batch electrooxidations. A good agreement between the model and experimental tests, adequate hydrogen recoveries and low sulfur crossover through the membrane demonstrate practical robustness of this approach. (C) 2019 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
机译:基于硫的热化学循环,例如杂交硫 - 氨(Hysa)循环,提供了一种有价值的方法,其中通过利用二氧化硫(潜在的污染物排放)通过亚硫酸盐的电化学氧化来产生氢。在这项研究中,通过比较不同的反应情景来评估pH对电氧化率的影响。然后,使用与响应表面方法(RSM)结合的中央复合设计(CCD)来优化近中性pH下亚硫酸铵的批量电氧化。结果表明,使用阴离子交换膜(AEM)大大提高了亚硫酸盐电氧化速率,同时pH有效稳定。此外,在长期批量电氧化下,获得并在实验中获得施加施加电位和亚硫酸盐浓度与反应的归一化半衰期相关的二阶模型。模型与实验试验之间的良好一致性,充足的氢气回收和通过膜的低硫交叉表现出这种方法的实际稳健性。 (c)2019氢能源出版物LLC。 elsevier有限公司出版。保留所有权利。

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