含氧煤层气流化床催化燃烧脱氧特性研究

周福勋; 赵建涛; 张磊; 吴志伟; 王建国; 房倚天; 秦张峰

含氧煤层气流化床催化燃烧脱氧特性研究

1.
中国科学院山西煤炭化学研究所煤转化国家重点实验室, 山西太原 030001;
2.
中国科学院大学, 北京 100049

基金项目: 山西省科技重大专项(20111101005)。

详细信息

通讯作者:
房倚天, E-mail: fyt@sxicc.ac.cn。

中图分类号: TQ541
计量
- 文章访问数: 1939
- HTML全文浏览量: 13
- PDF下载量: 764
- 被引次数: 0
出版历程
- 收稿日期: 2012-12-24
- 修回日期: 2013-01-22
- 刊出日期: 2013-05-30

Catalytic deoxidization characteristic of oxygen-bearing coal mine methane in the fluidized bed reactor

1.
State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China;
2.
University of Chinese Academy of Sciences, Beijing 100049, China

摘要

摘要: 利用自制的铜基球形甲烷催化燃烧催化剂,在小型流化床反应器中对模拟含氧煤层气进行了流化床催化燃烧脱氧的实验研究,考察了床层温度、催化剂粒径、空速对脱氧效率和CO₂选择性的影响。结果表明,较高的反应床层温度使催化剂活性增强,进而提高催化脱氧效率。床层温度在450 ℃以上,脱氧效率可稳定保持在95%以上。较小的催化剂粒径降低了内扩散阻力对催化反应的影响,提高催化反应的CO₂选择性。床层温度在450 ℃以下时,降低空速可提高氧气转化率,但温度高于450 ℃时,脱氧反应速率加快,空速变化对脱氧效率影响不明显。此外,通过调节CH₄/Air比例模拟不同含氧量的煤层气,考察流化床反应器及催化剂对含氧煤层气中O₂浓度变化的适应性。模拟含氧煤层气中氧气体积分数在5%~15%,该催化剂均表现出高的脱氧活性和选择性,反应器出口气体中氧气体积分数低于0.2%,CO₂选择性高于98%。
- 煤层气 /
- 流化床 /
- 催化燃烧 /
- 脱氧
Abstract: The catalytic deoxygenating experiment of oxygen-bearing coal mine methane (CMM) was carried out in a bench-scale fluidized bed reactor with the spherical Cu-based catalyst. The effects of the bed temperature, the particle size and the space velocity were investigated on the oxygen removal efficiency and CO₂ selectivity. The raising bed temperature could promote the O₂ conversion due to the high activity of the catalyst. The O₂ conversion could reach more than 95% when the temperature was above 450 ℃. The smaller particle size was beneficial to the CO₂ selectivity of the catalyst because of the decreasing inner diffusion resistance. The lower space velocity also could improve the O₂ removal efficiency when the bed temperature was below 450 ℃ although the improvement almost disappears above 450 ℃ due to the increasing catalytic combustion rate. Additionally, by adjusting the CH₄/Air ratio, the catalytic deoxygenation adaptability of the fluidized bed reactor and the catalyst was evaluated for the variable oxygen content in CMM. The results indicate that the process has a perfect oxygen removal performance with the O₂ concentration less than 0.2% and the CO₂ selectivity more than 98% for the O₂ content from 5% to 15% in the simulated CMM.
- coal mine methane /
- fluid bed reactor /
- catalytic combustion /
- deoxidization

HTML全文

参考文献(18)

LUO D K, DAI Y J. Economic evaluation of coalbed methane production in China[J]. Energy Policy, 2009, 37(10): 3883-3889.

郑珩, 陈耀壮, 廖炯, 马磊, 曾健. 煤层气脱氧制CNG/LNG技术开发[J]. 化工进展, 2010, 29(S1): 337-341.(ZHENG Yan, CHEN Yao-zhuang, LIAO Jiong, MA Lei, ZENG Jian. Technology Development of coalbed methane prepare CNG/LNG. Chemlcal Industry and Engineering Progress, 2010, 29(S1): 337-341.)

国家发展和改革委员会, 煤层气(煤矿瓦斯)开发利用"十一五"规划[Z]. 国家发展和改革委员会, 2006.(The national development and the reform committee. The utilization of coalbed methane (coal mine gas) in "The 11th five-year plan"[Z]. The national development and the reform committee, 2006.)

国家发展和改革委员会, 煤层气(煤矿瓦斯)开发利用"十二五"规划[Z]. 国家发展和改革委员会, 2011.(The national development and the reform committee. The utilization of coalbed methane (coal mine gas) in "The 12nd five-year plan"[Z]. The national development and the reform committee, 2011.)

LANDI G, BARBATO P S, CIMINO S, LISI L, RUSSO G. Fuel-rich methane combustion over Rh-LaMnO₃ honeycomb catalysts[J]. Catal Today, 2010, 155(1-2): 27-34.

王树东, 袁中山, 王胜, 张纯希, 倪长军. 一种煤层气脱氧催化剂、其制备方法及应用:中国,公开号:CN101664679A[P].2010-03-10.(WANG Shu-dong,YUAN Zhong-shan,WANG Sheng,ZHANG Chun-xi,NI Chang-jun. A kind of oxygen-bearing coal mine methane deoxidization catalyst, its preparation and utilization: CN, 101664679A[P]. 2010-03-10.)

LEE J H, TRIMM D L. Catalytic combustion of methane[J]. Fuel Process Technol, 1995, 42(2): 339-359.

SU S, AGNEW J. Catalytic combustion of coal mine ventilation air methane[J]. Fuel, 2006, 85(9): 1201-1210.

DENG Y, NEVELL T G. Oscillations of methane combustion over alumina-supported palladium catalysts under oxygen-deficient conditions[J]. J Mol Catal A, 1999, 142(1): 51-60.

廖炯, 陈耀壮, 胡善霖, 姚松柏, 雷菊梅, 白燕. 一种含氧煤层气脱氧催化剂及其制备方法及应用: 中国, 公开号: CN101322942A[P]. 2008-12-17.(LIAO Jiong,CHEN Yao-zhuang,HU Shan-lin,YAO Song-bai,LEI Ju-mei,BAI Yan. A kind of oxygen-bearing coal mine methane deoxidization catalyst and its preparation, utilization: CN, 101322942A[P]. 2008-12-17.)

董卫果, 李雪飞, 王鹏, 徐春霞, 杨宗仁, 文芳, 张科达, 李小亮, 国晖, 刘春兰, 段超, 吴涛. 一种煤层气脱氧和浓缩分离甲烷的方法: 中国, 公开号: CN101921642A[P]. 2010-12-22.(DONG Wei-guo, LI Xue-fei, WANG Peng, XU Chun-yan, YANG Zong-ren, WEN Fang, ZAHNG Ke-da, LI Xiao-liang, GUO Hui, LIU Chun-lan, DUAN Chao, WU Hao. A process of coal mine methane deoxidization, concentration and separation of methane: CN, 101921642A[P]. 2010-12-22.)

张力, 张俊广, 杨仲卿, 唐强. 超低浓度甲烷在Cu/γ-Al₂O₃催化剂颗粒流化床中的燃烧特性[J]. 燃料化学学报, 2012, 40(7): 886-891.(ZHANG Li, ZHANG Jun-guang, YANG Zhong-qing, TANG Qiang. Combustion characteristics of ultra-low content methane in a fluidized bed reactor with Cu/[WTBZ]γ[WTB1]-Al₂O₃ as catalytic particles[J]. Journal of Fuel Chemistry and Technology, 2012, 40(7): 886-891.)

LYUBOVSKY M, SMITH L L, CASTALDI M, KARIM H, NENTWICK B, ETEMAD S, LAPIERRE R, PFEFFERLE W C. Catalytic combustion over platinum group catalysts: Fuel-lean versus fuel-rich operation[J]. Catal Today, 2003, 83(1-4): 71-84.

陈甘棠. 化学反应工程[M]. 3版. 北京: 化学工业出版社, 2007.(CHEN Gan-tang. Chemical reaction engineering[M]. 3rd ed. Beijing: Chemical Industry Press, 2007.)

常剑, 高金森, 徐春明. 大颗粒FCC汽油芳构化催化剂表面烧焦过程的数值模拟[J]. 燃料化学学报, 2007, 35(4): 423-430.(CHANG Jian, GAO Jin-sen, XU Chun-ming. Simulation of the regeneration of large particle FCC naphtha aromatization catalyst[J]. Journal of Fuel Chemistry and Technology, 2007, 35(4): 423-430.)

TRIMM D L, LAM C W. The combustion of methane on platinum-alumina fibre catalysts-I: Kinetics and mechanism[J]. Chem Eng Sci, 1980, 35(6): 1405-1413.

MOUADDIB N, FEUMI-JANTOU C, GARBOWSKI E, PRIMET M, Catalytic oxidation of methane over palladium supported on alumina: Influence of the oxygen-to-methane ratio[J]. Appl Catal A, 1992, 87(1): 129-144.

ÖZGEN KARACANA C, RUIZ F A, COTC M, PHIPPS S, Coal mine methane: A review of capture and utilization practices with benefits to mining safety and to greenhouse gas reduction[J], Int J Coal Geol, 2011, 86(2/3): 121-156.

施引文献

资源附件(0)

访问统计