石油学报(石油加工) ›› 2020, Vol. 36 ›› Issue (6): 1120-1128.doi: 10.3969/j.issn.1001-8719.2020.06.002

• 化学链燃烧 • 上一篇    下一篇

硫酸盐硫在化学链燃烧过程中的迁移转化规律

罗明1,2,张海燕1,王超1,周伦正1   

  1. 1. 江苏大学 能源与动力工程学院, 江苏 镇江 212013;
    2. 宁夏大学 省部共建煤炭高效利用与绿色化工国家重点实验室,宁夏 银川 750021
  • 收稿日期:2020-06-10 修回日期:2020-07-16 出版日期:2020-11-25 发布日期:2020-12-02
  • 通讯作者: 罗明,男,副教授,博士,从事燃料的低碳高效清洁转化利用方面的研究,E-mail:mingluo@ujs.edu.cn E-mail:mingluo@ujs.edu.cn
  • 基金资助:
    国家自然基金项目(51606087),省部共建煤炭高效利用与绿色化工国家重点实验室开放课题项目(2020-KF-07)资助

Migration and Transformation of Sulfate Sulfur During the Chemical Looping Combustion

 LUO Ming1,2, ZHANG Haiyan1, WANG Chao1, ZHOU Lunzheng1   

  1.  1. School of Energy and Power Engineering, Jiangsu University, Zhenjiang 212013,China;
    2. State Key Laboratory of High-Efficiency Utilization of Coal and Green Chemical Engineering, Ningxia University, Yinchuan 750021, China
  • Received:2020-06-10 Revised:2020-07-16 Online:2020-11-25 Published:2020-12-02
  • Supported by:
     

摘要:

2种典型的模型化合物(CaSO4和FeSO4)为研究对象,研究采用Cu基载氧体时,煤中硫酸盐硫在化学链燃烧(CLC)过程中的迁移转化规律。热力学模拟研究发现,反应温度及载氧体过氧系数均会对模型化合物中硫的气固相分布造成影响。在低温和低载氧体过氧系数条件下,CuO易被硫化生成Cu2S。与FeSO4相比,CaSO4具有更高的耐温性。进而以担载在活性炭中的模型化合物为研究对象,在小型流化床反应器中开展了CLC实验研究。结果表明,在还原反应阶段和氧化反应阶段,SO2均为主要的含硫气体。在还原反应阶段的前20.5 min内,FeSO4和CaSO4中硫转化为气相组分的摩尔分数分别为83.16%和50.09%。对还原反应阶段后载氧体的物相组成进行分析,发现有Cu2S存在。对一次还原氧化反应后载氧体表面元素进行分析发现,表面有部分硫累积及残留。

关键词: 化学链, 燃烧, 无机硫, 模型化合物, 载氧体

Abstract:

Two typical inorganic model compounds (CaSO4 and FeSO4) were selected to study the the migration and transformation law of sulfate sulfur in the CLC process of coal by using the Cu-based oxygen carrier. The thermodynamic simulation of the reduction process shows that the temperatures and the excess coefficient of oxygen carrier affect the distribution of sulfur. CuO is sulfurized to form Cu2S, especially under the conditions of low temperatures and low oxygen carrier peroxide coefficient. Compared with FeSO4, CaSO4 has a higher thermal resistance. Further more, CLC experiments were carried out in a small fluidized bed reactor with model compounds loading on activated carbon. The results show that SO2 is the main sulfur gas in both reduction and oxidation stages. In the reduction stage (20.5 min), the molar fractions of sulfur in FeSO4 and CaSO4 converted into sulfurous gases reach 83.16% and 50.09%, respectively. The existence of Cu2S is confirmed in the oxygen carrier after the reduction stage. The energy-dispersive X-ray spectroscopy (EDX) analysis reveals the accumulation of sulfur after one reduction-oxidation reaction.

Key words: chemical-looping, combustion, inorganic sulfur, model compound, oxygen carrier

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