石油学报(石油加工) ›› 2020, Vol. 36 ›› Issue (6): 1379-1388.doi: 10.3969/j.issn.1001-8719.2020.06.029

• 其他 • 上一篇    下一篇

铝基载氮体在煤化学链制氨过程中的吸氮和释氮行为

吴烨, 张权, 冯鸣谦, 刘冬   

  1. 南京理工大学 能源与动力工程学院, 江苏 南京 210094
  • 收稿日期:2020-04-26 修回日期:2020-07-21 出版日期:2020-11-25 发布日期:2020-12-02
  • 通讯作者: 吴烨,男,副教授,博士,从事化石能源低碳利用方面的基础研究,E-mail:ywu@njust.edu.cn E-mail:ywu@njust.edu.cn
  • 基金资助:
     国家自然科学基金项目(51506095)和中央高校基本科研基金项目(30919011238)资助

N-Adsorption/Desorption Performance of Al-Based N-Carrier During Chemical Looping Ammonia Generation

WU Ye, ZHANG Quan, FENG Mingqian, LIU Dong   

  1.  School of Energy and Power Engineering, Nanjing University of Science & Technology, Nanjing 210094, China
  • Received:2020-04-26 Revised:2020-07-21 Online:2020-11-25 Published:2020-12-02
  • Supported by:
     

摘要:

以石墨、碳黑、烟煤/无烟煤/褐煤的脱灰半焦为碳源,通过固定床反应器以及多种表征手段探究铝基载氮体(氧化铝与氮化铝)的吸氮反应特性,并研究了TiO2和ZrO2对于载氮体释氮反应特性的影响。结果表明:碳源中较高的无序化程度有利于载氮体吸氮反应的进行;Al2O3与C的摩尔比为3∶3、吸氮反应温度为1200 ℃,是制备出适用于化学链反应制氨(CLAG)的多孔型载氮体的最佳工况;通过筛选原煤煤种发现,烟煤对于吸氮反应的促进效果最好,褐煤其次,无烟煤最差;通过优化对烟煤原煤的热解方式,能够将烟煤脱灰半焦的转化率从20%提升至39%。添加TiO2作为催化剂可明显提高氮化铝的转化率,但由于氨气的高温分解,导致氨气的产率不高;利用对氨气具有分子吸附能力的ZrO2为催化剂载体,可使得载氮体在释氮反应中的氨气生成率达到80%。

关键词: 化学链制氨, 载氮体, 吸氮反应, 释氮反应

Abstract:

The N-adsorption performance of graphite, carbon black and bituminous/lignite/anthracite semi-coke were studied by the fixed bed reactor and other characterization methods, and the effects of TiO2 and ZrO2 on N-desorption performance of N-carrier. The results show that the amorphous carbon promotes the N-adsorption performance of the N-carrier, and the optimized conditions to prepare porous N-carriers for chemical looping ammonia generation (CLAG) are Al2O3 to C mole ratio and temperature 3∶3 and 1200 ℃. The reactivity of different deashing semi-coke is found in a descending order of bituminous, lignite, and anthracite. Optimizing pyrolysis methods of bituminous coal could increase the conversion efficiency from 20% to 39%. Moreover, the results indicate that addition of TiO2 could increase the conversion efficiency of AlN significantly, while the yield of NH3 is not high due to the decomposition of NH3 under high temperature. Using ZrO2, which has adsorption capacity of NH3, could enhance the yield of NH3 to 80% during the N-desorption reaction.

Key words: chemical looping ammonia generation (CLAG); N-carrier, N-adsorption reaction, N-desorption reaction

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