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迈向可持续的氢气生产:乙醇吸附增强蒸汽重整。

Approaching sustainable H2 production: sorption enhanced steam reforming of ethanol.

机构信息

Department of Chemical Engineering, Norwegian University of Science and Technology, Sem Saelands vei 4, Trondheim, NO-7491, Norway.

出版信息

J Phys Chem A. 2010 Mar 25;114(11):3834-44. doi: 10.1021/jp906146y.

DOI:10.1021/jp906146y
PMID:19831373
Abstract

Sorption enhanced steam reforming of ethanol (SESRE), featured by yielding high purity of H(2) from one single reaction unit, is a new reaction process with a great potential for realizing sustainable H(2) production. The potential of such process with a CaO-based acceptor has been assessed by thermodynamic analysis and experimental demonstration. As predicted, ethanol can be reformed at relatively low temperatures (500-600 degrees C), still yielding high-quality H(2). Another major advantage of coupling CO(2) capture to the reforming process is predicted to be low risk in carbon formation. The SESRE reaction was carried out over a mixture of hydrotalcite-like material derived Co-Ni catalysts (Co-Ni/HTls) and calcined dolomite with a steam to carbon (S/C) ratio of 3 and temperatures ranging from 500 to 650 degrees C. The chosen reaction system was able to yield H(2) with purity fairly close to the theoretical prediction. Particularly, the best result was obtained over 40Ni and 20Co-20Ni/HTls at 550 degrees C, where the product gas had composition of more than 99 mol % H(2), ca. 0.4 mol % CH(4), 0.1 mol % CO, and 0.2 mol % CO(2). Special emphasis was put on the effect of steam on the stability of the CO(2) acceptor during the SESRE reaction. Hydration of CaO in the acceptor did not cause appreciable induction period, even at the low operating temperatures. However, different from a test under dry atmosphere (CO(2)/argon), the acceptor showed rapid deactivation in a multicycle operation of SESRE. A similar deactivation tend was given by a comparative test in a steam/CO(2)/Ar atmosphere.

摘要

吸附增强蒸汽重整乙醇(SESRE),其特点是从单个反应单元中产生高纯度的 H(2),是一种具有很大潜力的可持续 H(2)生产的新反应过程。通过热力学分析和实验验证,评估了基于 CaO 的吸收剂的这种工艺的潜力。如预测的那样,乙醇可以在相对较低的温度(500-600°C)下进行重整,仍然产生高质量的 H(2)。将 CO(2)捕集与重整过程相结合的另一个主要优点预计是碳形成的风险低。SESRE 反应在水滑石样材料衍生的 Co-Ni 催化剂(Co-Ni/HTls)和煅烧白云石的混合物上进行,蒸汽与碳(S/C)的比例为 3,温度范围为 500-650°C。所选的反应系统能够以相当接近理论预测的纯度产生 H(2)。特别是,在 550°C 下,40Ni 和 20Co-20Ni/HTls 获得了最佳结果,其中产物气体的组成超过 99 mol% H(2)、约 0.4 mol% CH(4)、0.1 mol% CO 和 0.2 mol% CO(2)。特别强调了蒸汽对 SESRE 反应中 CO(2)吸收剂稳定性的影响。吸收剂中 CaO 的水合作用即使在低操作温度下也不会引起明显的诱导期。然而,与在干燥气氛(CO(2)/氩气)下的测试不同,吸收剂在 SESRE 的多循环操作中表现出快速失活。在蒸汽/CO(2)/Ar 气氛下进行的比较测试给出了类似的失活动向。

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