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Continuous high-purity hydrogen production by sorption enhanced steam reforming of ethanol over modified lithium silicate
International Journal of Hydrogen Energy ( IF 7.2 ) Pub Date : 2020-05-23 , DOI: 10.1016/j.ijhydene.2020.04.225
Nana Wang , Yuchuan Feng , Xin Guo , Shiyi Ni

Sorption-enhanced steam reforming of ethanol (SE-SRE) with in-situ CO2 removal is an environmentally friendly and sustainable approach for hydrogen production. Researches on continuous production of high-purity H2 by SE-SRE over the modified Li4SiO4 sorbent were conducted using two parallel reactor in this work. The low cost Li4SiO4 derived from rice husk ash (RHA) is a promising high-temperature CO2 sorbent. However, the poor adsorption kinetics of RHA-Li4SiO4 sorbent at low CO2 concentration is the major challenge. The metallic elements (K, Ca, Al, Mg) were employed to modify the RHA-Li4SiO4 for efficient CO2 capture. The developed sorbents were characterized and tested to study the role of dopants on the crystal, textural, microstructure and CO2 adsorption kinetics and cyclic stability. Results indicated that K doping effectively inhibited the growth of crystal aggregation and resulted in a fluffy morphology with abundant pores and higher specific surface area, while the addition of Ca, Al and Mg formed a nubby structure with larger particle size. K-doped RHA-Li4SiO4 exhibited the best CO2 uptake properties and the optimal K doping molar content was 0.02 with the maximum capture capacity of 34.16 wt%, which is higher than 27.1 wt% of pure RHA-Li4SiO4. Then, the effect of operating conditions on the enhancement behaviors was considered in the SE-SRE system. High-purity H2 (above 96%) was achieved by coupling K(0.02)/RHA-Li4SiO4 sorbent with Ni-based catalyst under the optimum condition (T: 525 °C, liquid hourly space velocity: 0.9 mL/(g·h), sorbent/catalyst: 4 and steam/carbon: 8.0). The adsorption activity of K(0.02)/RHA-Li4SiO4 maintained at a high level in ten SE-SRE/regeneration cycles. Finally, a scheme including two parallel fixed-bed reactors was designed and operated periodically for continuous production of high-purity H2. The reaction switching time was shown to depend strongly on the pre-breakthrough time and operating conditions. As the reaction switching time was 40 min, the products were always only H2 and CH4 (no CO and CO2 appear) and the H2 purity remained above 90% during 400 min, confirming high purity hydrogen stream can be obtained continuously.



中文翻译:

在改性硅酸锂上通过吸附增强乙醇的水蒸气重整来连续高纯度制氢

原位去除CO 2的乙醇的吸附增强蒸汽重整(SE-SRE)是一种环保且可持续的制氢方法。这项工作是使用两个并联反应器进行的,研究了在改性的Li 4 SiO 4吸附剂上用SE-SRE连续生产高纯度H 2的方法。源自稻壳灰(RHA)的低成本Li 4 SiO 4是一种有前途的高温CO 2吸附剂。但是,RHA-Li 4 SiO 4吸附剂在低CO 2下的吸附动力学较差。集中精神是主要挑战。金属元素(K,Ca,Al,Mg)用于修饰RHA-Li 4 SiO 4以便有效捕获CO 2。对已开发的吸附剂进行表征和测试,以研究掺杂剂对晶体,织构,微观结构以及CO 2吸附动力学和循环稳定性的作用。结果表明,钾掺杂有效地抑制了晶体聚集的生长,并导致了蓬松的形貌,具有丰富的孔洞和更高的比表面积,而钙,铝和镁的添加形成了较大粒径的块状结构。掺K的RHA-Li 4 SiO 4表现出最好的CO 2的吸收特性和最佳的K掺杂摩尔含量为0.02,最大捕获容量为34.16 wt%,高于纯RHA-Li 4 SiO 4的27.1 wt%。然后,在SE-SRE系统中考虑了操作条件对增强行为的影响。在最佳条件下(T:525°C,液时空速:0.9 mL / min),通过将K(0.02)/ RHA-Li 4 SiO 4吸附剂与镍基催化剂偶联,可实现高纯度H 2(96%以上)(g·h),吸附剂/催化剂:4,蒸汽/碳:8.0)。K(0.02)/ RHA-Li 4 SiO 4的吸附活性在十个SE-SRE /再生周期中保持较高的水平。最后,设计并包括两个平行的固定床反应器的方案并定期运行以连续生产高纯度H 2。已显示反应切换时间很大程度上取决于预突破时间和操作条件。当反应切换时间为40分钟时,产物始终仅是H 2和CH 4(没有CO和CO 2出现),并且在400min内H 2纯度保持在90%以上,证实可以连续获得高纯度氢流。

更新日期:2020-05-23
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