煤表面硫与氮官能团低温氧化规律XPS技术研究

张兰君; 李增华; 杨永良; 李金虎; 周银波

煤表面硫与氮官能团低温氧化规律XPS技术研究

计量
- 文章访问数: 0404
- HTML全文浏览量: 0
- PDF下载量: 0
出版历程
- 发布日期: 2016-05-19

XPS Research on Sulfur and Nitrogen Surface Functional Groups of Coal During Low-temperature Oxidation

摘要

摘要: 利用XPS测试技术对兴成肥煤低温氧化规律进行实验研究。硫元素XPS氧化前后测试结果对比分析表明原煤硫元素中硫化物硫和硫铁矿硫占比最高，而有机硫中噻吩硫含量最高，其次为砜和亚砜。氧化后煤表面噻吩硫相对含量降低，有机硫中的部分硫化物硫氧化成亚砜，亚砜进一步氧化成砜，导致砜相对浓度增加，而亚砜缺失。原煤氮元素谱图分析可知兴成煤中氮主要存在于煤分子的边缘，约21%氮以季氮形式镶嵌于煤分子芳香结构中，煤中吡咯氮含量最高。氧化后XPS结果表明在氧化过程中与氮相连的氧原子脱除，氧化型氮转变为其他形态，且很大一部分转化为吡啶。
- 煤 /
- 低温氧化 /
- XPS /
- 有机硫官能团 /
- 有机氮官能团
Abstract: We use XPS technology to research Xinchen fat coal low temperature oxidation experiment. The XPS results of sulfur on the coal surface before and after oxidation show that the sulfide and pyrite content is highest for raw coal sample; thiophenic sulfur content is the highest in organic sulfur, followed by sulfoxide and sulfone; there is also some sulfate existing on the coal surface. The result of oxidized coal is different from raw sample; the relative contents of thiophenic sulfur is reduced; the sulfide oxide into sulfoxide which further oxidized to sulfone, that is the reason why sulfone relative concentration increased meanwhile sulfoxide disappeared. The nitrogen spectrogram of raw coal analysis shows that the nitrogen mainly exists on the edge of coal molecules; about 21% of nitrogen is embedded into coal molecular structure in the quaternary nitrogen form; the pyrrole nitrogen content is the highest. The XPS results of oxidation sample show that the oxygen atom linked to nitrogen removal in the process of oxidation; the oxidation nitrogen changes into other forms and most parts of it change into pyridine.
- coal /
- low-temperature oxidation /
- XPS /
- organic sulfur functional group /
- organic nitrogen functional group

HTML全文

参考文献(21)

[1]	邓存宝. 煤的自燃机理及自燃性危险指数研究[D].阜新: 辽宁工程技术大学, 2006.
[2]	李梅, 杨俊和, 张启锋, 等. 用XPS研究新西兰高硫煤热解过程中氮、硫官能团的转变规律[J].燃料化学学报,2013(11):1287-1293.
[3]	Oka N, Sojar H T, Hamada N, et al. Surface studies of low-temperature oxidation of bituminous coal vitrain bands using XPS and SIMS[J]. Fuel, 1998,77: 1081-1087.
[4]	Frost David C, Leeder William R, Tapping Robert L. X-ray photoelectron spectroscopic investigation of coal[J]. Fuel, 1974,53(3): 206-211.
[5]	Kelemen S R, George G N, Gorbaty M. L. Direct determination and quantification of sulphur forms in heavy petroleum and coals: 1. The X-ray photoelectron spectroscopy (XPS) approach[J]. Fuel, 1990,69(90): 939-944.
[6]	张蓬洲, 赵秀荣. 用XPS研究我国一些煤中有机硫的存在形态[J].燃料化学学报,1993,21(2): 205-210.
[7]	唐跃刚, 邵绪新, 雷加锦, 等. 高硫煤中各种成因硫的光电子能谱研究[J].燃料化学学报, 1993(4): 413-418.
[8]	Zhang Lanjun, Li Zenghua, Li Jinhu, et al. Studies on the Low-Temp Oxidation of Coal Containing Organic Sulfur and Corresponding Model Compounds[J]. Molecules, 2015,20(12): 22241-22256.
[9]	Kelemen S R George GN. Direct determination and quantification of sulfur forms in heavy petroleum and coals 1. The X-ray photoelectron spectroscopy (XPS) approach[J].Fuel, 1990,69(8): 939-944.
[10]	Gorbaty Martin L, George Graham N, Kelemen Simon R. Chemistry of organically bound sulphur forms during the mild oxidation of coal[J]. Fuel, 1990,69(8): 1065-1067.
[11]	Marinov S P, Tyuliev G, Stefanova M., et al. Low rank coals sulphur functionality study by AP-TPR/TPO coupled with MS and potentiometric detection and by XPS[J]. Fuel Processing Technology, 2004,85(4): 267-277.
[12]	Gong Bin, Buckley Alan N, Lamb Robert N., et al. XPS determination of the forms of nitrogen in coal pyrolysis chars[J]. Surface & Interface Analysis, 1999,28(1): 126-130.
[13]	Gorbaty Martin L, Kelemen Simon R. Characterization and reactivity of organically bound sulfur and nitrogen fossil fuels[J]. Fuel Processing Technology, 2001,71(1): 71-78.
[14]	Pietrzak Robert, Grzybek Teresa, Wachowska Helena. XPS study of pyrite-free coals subjected to different oxidizing agents[J]. Fuel, 2007,86(16): 2616.
[15]	Perry David L, Grint Alan. Application of XPS to coal characterization[J]. Fuel, 1983,62(9): 1024-1033.
[16]	Kelemen S R, George G N, Gorbaty M L Direct determination and quantification of sulphur forms in heavy petroleum and coals: 1. The X-ray photoelectron spectroscopy (XPS) approach[J]. Fuel, 1990,69(90): 939-944.
[17]	Grzybek T., Pietrzak R., Wachowska H. The Comparison of Oxygen and Sulfur Species Formed by Coal Oxidation with O₂/Na₂CO₃ or Peroxyacetic Acid Solution. XPS Studies[J]. Energy & Fuels, 2004,18(3):804.
[18]	Pietrzak Robert, Grzybek Teresa, Wachowska Helena. XPS study of pyrite-free coals subjected to different oxidizing agents[J]. Fuel, 2007,86(16): 2616-2624.
[19]	朱珍平, 崔洪, 李允梅, 等. 二种高硫煤中硫氮化学形态的研究[J].环境化学,1995(6):483-488.
[20]	姚明宇, 刘艳华, 车得福. 宜宾煤中氮的形态及其变迁规律研究[J].西安交通大学学报, 2003(7): 759-763.
[21]	Molina A., Eddings E. G., Pershing D. W., et al. Char nitrogen conversion: implications to emissions from coal-fired utility boilers[J]. Progress in Energy & Combustion Science, 2000,26(4): 507-531.

施引文献(9)

期刊类型引用(6)

1.	张健. 坚硬顶板切顶合理参数模拟研究. 山西冶金. 2024(01): 115-116+119 . 百度学术
2.	刘坤，滕腾，杨耀辉，李梓昊，丁鹤. 不同采高下深部煤层覆岩应力场与塑性区演化数值模拟研究. 采矿技术. 2024(04): 41-45 . 百度学术
3.	宋士康，REN Ting，冯海龙，窦林名，孙炳清，张涛，任康江. 高承压水与深部应力耦合作用下顶板运移及应力显现规律. 煤矿安全. 2023(04): 169-174 . 本站查看
4.	马祥，白贤栖，曹安业，曾海利，黄锐，张德兵，秦续峰，张润兵. 基于微震分布特征的覆岩结构演化规律研究. 煤矿安全. 2023(12): 80-87 . 本站查看
5.	侯恩科，刘博，龙天文，徐维，魏启明，马进勇. 深埋缓倾斜双煤层开采导水断裂带发育规律研究. 煤矿安全. 2022(03): 50-57 . 本站查看
6.	关众. 霍洛湾煤矿22206工作面水体下安全开采技术. 煤矿安全. 2022(12): 54-61 . 本站查看

其他类型引用(3)

资源附件(0)

计量

文章访问数:
HTML全文浏览量: 0
PDF下载量: 0
被引次数: 9

煤表面硫与氮官能团低温氧化规律XPS技术研究

计量

出版历程

XPS Research on Sulfur and Nitrogen Surface Functional Groups of Coal During Low-temperature Oxidation

期刊类型引用(6)

其他类型引用(3)

计量

出版历程

目录