化工学报 ›› 2021, Vol. 72 ›› Issue (S1): 482-493.DOI: 10.11949/0438-1157.20201771
收稿日期:
2020-12-09
修回日期:
2021-01-15
出版日期:
2021-06-20
发布日期:
2021-06-20
通讯作者:
王志刚,谭小耀
作者简介:
陈晨(1995—),女,硕士研究生,基金资助:
CHEN Chen(),WANG Mingming,WANG Zhigang(),TAN Xiaoyao()
Received:
2020-12-09
Revised:
2021-01-15
Online:
2021-06-20
Published:
2021-06-20
Contact:
WANG Zhigang,TAN Xiaoyao
摘要:
采用纺丝-烧结技术制备了具有内表面致密皮层的外支撑式金属镍非对称中空纤维膜,并用于乙醇自热重整(EATR)制氢,研究了温度、进料流速、吹扫气流速、水醇比(S/C)以及氧醇比(O2/C)等操作条件对膜制氢性能的影响。结果表明,金属镍非对称中空纤维膜既具有优异的EATR催化活性,又有良好的透氢性能。在500~1000℃、S/C=4、O2/C=0.8的条件下乙醇可完全转化,H2产率和H2渗透通量可分别达到81.59%和13.99 mmol/(m2·s),增加进料中氧气含量可显著抑制膜表面积炭,但同时也会降低氢气产率和一氧化碳选择性。
中图分类号:
陈晨, 王明明, 王志刚, 谭小耀. 镍基非对称中空纤维膜用于乙醇自热重整制氢[J]. 化工学报, 2021, 72(S1): 482-493.
CHEN Chen, WANG Mingming, WANG Zhigang, TAN Xiaoyao. Hydrogen production by ethanol autothermal reforming using nickel-based asymmetric hollow fiber membranes[J]. CIESC Journal, 2021, 72(S1): 482-493.
图3 不同进料浓度下镍中空纤维膜的H2渗透通量与温度的关系(H2-He进料速率= 30 ml/min;N2吹扫速率= 60 ml/min)
Fig.3 H2 permeation flux of Ni hollow fiber membrane as a function of temperature at different feed concentrations (H2-He feed rate=30 ml/min; N2 sweep rate=60 ml/min)
图4 镍中空纤维膜反应器和空白反应器中乙醇自热重整反应乙醇转化率、H2产率,MR产物浓度和Blank产物浓度随温度的变化(反应条件:S/C=4,O2/C=0.8,无吹扫气,进料流速为13 μl/min)
Fig.4 Ethanol autothermal reforming in Ni hollow fiber membrane reactor and blank reactor at different temperatures, ethanol conversion, hydrogen yield, product concentration of MR and Blank (Reaction conditions: S/C=4, O2/C=0.8, no sweep gas, feed flow rate=13 μl/min)
图5 不同吹扫气流速对乙醇自热重整反应乙醇转化率、H2产率、CO选择性和H2渗透通量的影响(反应条件:S/C=4,O2/C=0.8,吹扫气流速分别为0、30、50、70 ml/min,进料流速为13 μl/min)
Fig.5 Effect of sweep gas flow rate on ethanol conversion, hydrogen yield, CO selectivity and hydrogen penetration flux at different temperatures (Reaction conditions: S/C=4, O2/C=0.8, sweep gas flow rate=0,30,50,70 ml/min, feed flow rate=13 μl/min)
图6 不同蒸汽/乙醇比对乙醇自热重整反应乙醇转化率、H2产率、CO选择性和H2渗透通量的影响(反应条件:S/C=3、4、5、6,O2/C=0.8,吹扫气流速为30 ml/min,进料流速为13 μl/min)
Fig.6 Effect of S/C on ethanol conversion, hydrogen yield, CO selectivity and hydrogen penetration flux at different temperatures (Reaction conditions: S/C=3,4,5,6, O2/C=0.8, sweep gas flow rate=30 ml/min, feed flow rate=13 μl/min)
图7 不同氧气/乙醇比对乙醇自热重整反应乙醇转化率、H2产率、CO选择性和H2渗透通量的影响(反应条件:S/C=4,O2/C=0、0.5、0.8、1,吹扫气流速为30 ml/min,进料流速为13 μl/min)
Fig.7 Effect of O2/C on ethanol conversion, hydrogen yield, CO selectivity and hydrogen penetration flux at different temperatures (Reaction conditions: S/C=4, O2/C=0,0.5,0.8,1, sweep gas flow rate=30 ml/min, feed flow rate=13 μl/min)
图8 不同进料流速对乙醇自热重整反应乙醇转化率、H2产率、CO选择性和H2渗透通量的影响(反应条件:S/C=4,O2/C=0.8,吹扫气流速为30 ml/min,进料流速分别为13、19、26、39 μl/min)
Fig.8 Effect of feed flow rate on ethanol conversion, hydrogen yield, CO selectivity and hydrogen permeation flux at different temperatures (Reaction conditions: S/C=4, O/C=0.8, sweep gas flow rate=30 ml/min, feed flow rate=13,19,26,39 μl/min)
图10 ESR、EATR氢气渗透测试后镍中空纤维膜的形貌(a)、(b),ESR、EATR氢气渗透测试前后镍中空纤维的EDS映射(c)和元素分析(d)
Fig.10 Morphology of Ni hollow fiber membranes after ESR (a) and EATR (b) hydrogen permeation tests; EDS mappings (c) and EDS patterns (d) of nickel hollow fiber membranes before and after ESR and EATR hydrogen permeation tests
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