Effect of pyrite removal by chromous chloride on organic matter structure in Huadian oil shale

LI Yang; LIU Qing-ya; ZHAO Xiao-sheng; TANG Rui-xiang; LU Zheng-hua; SHI Lei

Volume 47 Issue 2

Feb. 2019

Turn off MathJax

Article Contents

Article Navigation > Journal of Fuel Chemistry and Technology > 2019 > 47(2): 144-152

LI Yang, LIU Qing-ya, ZHAO Xiao-sheng, TANG Rui-xiang, LU Zheng-hua, SHI Lei. Effect of pyrite removal by chromous chloride on organic matter structure in Huadian oil shale[J]. Journal of Fuel Chemistry and Technology, 2019, 47(2): 144-152.

Citation:

LI Yang, LIU Qing-ya, ZHAO Xiao-sheng, TANG Rui-xiang, LU Zheng-hua, SHI Lei. Effect of pyrite removal by chromous chloride on organic matter structure in Huadian oil shale[J]. Journal of Fuel Chemistry and Technology, 2019, 47(2): 144-152.

Citation:

LI Yang, LIU Qing-ya, ZHAO Xiao-sheng, TANG Rui-xiang, LU Zheng-hua, SHI Lei. Effect of pyrite removal by chromous chloride on organic matter structure in Huadian oil shale[J]. Journal of Fuel Chemistry and Technology, 2019, 47(2): 144-152.

PDF( 923 KB)

Effect of pyrite removal by chromous chloride on organic matter structure in Huadian oil shale

College of Chemical Engineering, Beijing University of Chemical Technology, Beijing 100029, China

Funds:

the National Basic Research Program of China 973 program

the National Basic Research Program of China 2014CB744301

More Information

Corresponding author: ZHAO Xiao-sheng, Tel: 010-64429158, E-mail: zhaoxs811@163.com
Received Date: 2018-10-29
Rev Recd Date: 2018-12-16

Available Online: 2021-01-23

Publish Date: 2019-02-10

Abstract

Abstract

Influence of pyrite removal by chromous chloride (CrCl₂) on structure of organic matter in Huadian oil shale was examined using ultimate analysis, ¹³C NMR, XPS and TG-MS technology. The results show that CrCl₂ treatment leads to 96.19% removal of pyrite from oil shale. The relative contents of aliphatic, aromatic, and carboxyl/carbonyl carbons of organic matter remain about the same level after pyrite removal by CrCl₂, so does the pyrolysis characteristic temperature, indicating the carbon skeleton of organic matter is less affected by CrCl₂. However, the CrCl₂ treatment can break C-O bond in organic matter and reduce content of C-O/C-OH and O=C-O, leading to about 0.98% and 12.54% loss for organic carbon and organic matter, respectively. In addition, carbon content of organic matter significantly increases, hydrogen content slightly increases, and oxygen content is markedly reduced after pyrite removal by CrCl₂, resulting in a slight decrease of H/C but a marked decrease of O/C in organic matter. The mass loss of organic matter treated by CrCl₂ increases during pyrolysis because aliphatic carbon content of unit mass of organic matter increases 5.28%. Besides, the residual chromium oxide may also promote decomposition of organic matter during pyrolysis.
- oil shale,
- pyrite,
- chromous chloride,
- organic matter,
- structure

FullText(HTML)

References(35)

References

[1]	王擎, 孙斌, 刘洪鹏, 柏静儒, 肖冠华.油页岩热解过程矿物质行为分析[J].燃料化学学报, 2013, 41(2):163-168. doi: 10.3969/j.issn.0253-2409.2013.02.007 WANG Qing, SUN Bin, LIU Hong-peng, BAI Jing-ru, XIAO Guan-hua. Analysis of mineral behavior during pyrolysis of oil shale[J]. J Fuel Chem Technol, 2013, 41(2):163-168. doi: 10.3969/j.issn.0253-2409.2013.02.007
[2]	畅志兵, 初茉, 张超, 白书霞, 林浩.桦甸油页岩热解过程中热沥青的组成变化规律[J].燃料化学学报, 2016, 44(11):1310-1317. doi: 10.3969/j.issn.0253-2409.2016.11.005 CHANG Zhi-bing, CHU Mo, ZHANG Chao, BAI Shu-xia, LIN Hao. Variation of chemical composition of thermal bitumen during Huadian oil shale pyrolysis[J]. J Fuel Chem Technol, 2016, 44(11):1310-1317. doi: 10.3969/j.issn.0253-2409.2016.11.005
[3]	ORENDT A M, PIMIENTA I S, BADU S R, SOLUM M S, PUGMIRE R J, FACELLI J C, WINANS R E. Three-dimensional structure of the Siskin Green River Oil Shale Kerogen Model:A comparison between calculated and observed properties[J]. Energy Fuels, 2013, 27(2):702-710. doi: 10.1021/ef3017046
[4]	GUAN X H, LIU Y, WANG D, WANG Q, CHI M S, LIU S, LIU C G. Three-dimensional structure of a huadian oil shale kerogen model:An experimental and theoretical study[J]. Energy Fuels, 2015, 29(7):4122-4136. doi: 10.1021/ef502759q
[5]	王擎, 许祥成, 迟铭书, 张宏喜, 崔达, 柏静儒.干酪根组成结构及其热解生油特性的红外光谱研究[J].燃料化学学报, 2015, 43(10):1158-1166. doi: 10.3969/j.issn.0253-2409.2015.10.002 WANG Qing, XU Xiang-cheng, CHI Ming-shu, ZHANG Hong-xi, CUI Da, BAI Jing-ru. FT-IR study on composition of oil shale kerogen and its pyrolysis oil generation characteristics[J]. J Fuel Chem Technol, 2015, 43(10):1158-1166. doi: 10.3969/j.issn.0253-2409.2015.10.002
[6]	TONG J H, HAN X X, WANG S, JIANG X M. Evaluation of structural characteristics of Huadian oil shale kerogen using direct techniques (solid-state ¹³C NMR, XPS, FT-IR, and XRD)[J]. Energy Fuels, 2011, 25(9):4006-4013. doi: 10.1021/ef200738p
[7]	WANG Q, HOU Y C, WU W Z, YU Z, REN S H, LIU Q Y, LIU Z Y. A study on the structure of Yilan oil shale kerogen based on its alkali-oxygen oxidation yields of benzene carboxylic acids, ¹³C NMR and XPS[J]. Fuel Process Technol, 2017, 166:30-40. doi: 10.1016/j.fuproc.2017.05.024
[8]	畅志兵, 初茉, 张超, 白书霞, 林浩, 马良博.固有碳酸盐和硅酸盐对太姥油页岩热解产物的影响[J].化工学报, 2017, 68(4):1582-1589. http://d.old.wanfangdata.com.cn/Periodical/hgxb201704038 CHANG Zhi-bing, CHU Mo, ZHANG Chao, BAI Shu-xia, LIN Hao, MA Liang-bo. Influence of inherent carbonates and silicates on pyrolytic products of Tailao oil shale[J]. J Chem Ind Eng (China), 2017, 68(4):1582-1589. http://d.old.wanfangdata.com.cn/Periodical/hgxb201704038
[9]	BALLICE L. Effect of demineralization on yield and composition of the volatile products evolved from temperature-programmed pyrolysis of Beypazari (Turkey) oil shale[J]. Fuel Process Technol, 2005, 86(6):673-690. doi: 10.1016/j.fuproc.2004.07.003
[10]	ZHAO X S, ZHANG X L, LIU Z Y, LU Z H, LIU Q Y. Organic matter in Yilan oil shale:Characterization and pyrolysis with or without inorganic minerals[J]. Energy Fuels, 2017, 31(4):3784-3792. http://d.old.wanfangdata.com.cn/NSTLQK/NSTL_QKJJ025855287/
[11]	YVRVM Y, DROR Y, LEVY M. Effect of acid dissolution on the mineral matrix and organic matter of Zefa Efe oil shale[J]. Fuel Process Technol, 1985, 11(1):71-86. http://www.sciencedirect.com/science/article/pii/0378382085900177
[12]	迟铭书, 王擎, 李松阳, 刘奇, 查伯宇.酸洗对桦甸油页岩矿物质以及有机结构的影响[J].燃料化学学报, 2017, 45(12):1424-1433. doi: 10.3969/j.issn.0253-2409.2017.12.003 CHI Ming-shu, WANG Qing, LI Song-yang, LIU Qi, CHA Bo-yu. Influence of demineralization on minerals and organic structure in Huadian oil shale[J]. J Fuel Chem Technol, 2017, 45(12):1424-1433. doi: 10.3969/j.issn.0253-2409.2017.12.003
[13]	LARSEN J W, PAN C S, SHAWVER S. Effect of demineralization on the macromolecular structure of coals[J]. Energy Fuels, 1989, 3(5):557-561. doi: 10.1021/ef00017a004
[14]	GAI R H, JIN L J, ZHANG J B, WANG J Y, HU H Q. Effect of inherent and additional pyrite on the pyrolysis behavior of oil shale[J]. J Anal Appl Pyrolysis, 2014, 105:342-347. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=61f70b2f5941d1bf79c4ae5456c1fb22
[15]	NEWTON R J, BOTTRELL S H, DEAN S P, HATFIELD D, RAISWELL R. An evaluation of the use of the chromous chloride reduction method for isotopic analyses of pyrite in rocks and sediment[J]. Chem Geol, 1995, 125(3/4):317-320. https://www.sciencedirect.com/science/article/abs/pii/0009254195000987
[16]	CANFIELD D E, RAISWELL R, WESTRICH J T, REAVES C M, BERNER R A. The use of chromium reduction in the analysis of reduced inorganic sulfur in sediments and shales[J]. Chem Geol, 1986, 54(1/2):149-155. doi: 10.1016-0009-2541(86)90078-1/
[17]	ACHOLLA F V, ORR W L. Pyrite removal from kerogen without altering organic matter:The chromous chloride method[J]. Energy Fuels, 1993, 7(3):406-410. doi: 10.1021/ef00039a012
[18]	GALUKHIN A, GERASIMOV A, NIKOLAEV I, NOSOV R, OSIN Y. Pyrolysis of Kerogen of Bazhenov Shale:Kinetics and influence of inherent pyrite[J]. Energy Fuels, 2017, 31(7):6777-6781.
[19]	周扬.依兰油页岩分级萃取物的结构研究[D].黑龙江: 黑龙江科技学院, 2011. http://cdmd.cnki.com.cn/Article/CDMD-10219-1011215358.htm ZHOU Yang. Study on the structures of sequential extraction of Yi-lan oil-shale[D]. Heilongjiang: Heilongjiang University of Science and Technology, 2011. http://cdmd.cnki.com.cn/Article/CDMD-10219-1011215358.htm
[20]	LIU Q, HOU Y C, WU W Z, WANG Q, REN S H, LIU Q Y. New insight into the chemical structures of Huadian kerogen with supercritical ethanolysis:Cleavage of weak bonds to small molecular compounds[J]. Fuel Process Technol, 2018, 176:138-145. doi: 10.1016/j.fuproc.2018.03.029
[21]	柏静儒, 王擎, 魏艳珍, 关晓辉.桦甸油页岩的酸洗脱灰[J].中国石油大学学报(自然科学版), 2010, 34(2):150-153. doi: 10.3969/j.issn.1673-5005.2010.02.030 BAI Jing-ru, WANG Qing, WEI Yan-zhen, GUAN Xiao-hui. Acid treatment de-ashing of Huadian oilshal[J]. J China Univ Pet (Nat Sci Ed), 2010, 34(2):150-153. doi: 10.3969/j.issn.1673-5005.2010.02.030
[22]	CHANG Z B, CHU M, ZHANG C, BAI S X, LIN H, MA L B. Influence of inherent mineral matrix on the product yield and characterization from Huadian oil shale pyrolysis[J]. J Anal Appl Pyrolysis, 2018, 130:269-276. doi: 10.1016/j.jaap.2017.12.022
[23]	VANDENBROUCKE M, LARGEAU C. Kerogen origin, evolution and structure[J]. Org Geochem, 2007, 38(5):719-833. http://d.old.wanfangdata.com.cn/NSTLQK/NSTL_QKJJ028056181/
[24]	张晓亮.油页岩有机质结构组成及其热断裂行为研究[D].北京: 北京化工大学, 2015. http://cdmd.cnki.com.cn/Article/CDMD-10010-1015723645.htm ZHANG Xiao-liang. Study on sturcture composition and thermal fracture behavior of oil shale organic matter[D]. Beijing: Beijing University of Chemical Technology, 2015. http://cdmd.cnki.com.cn/Article/CDMD-10010-1015723645.htm
[25]	ABOULKAS A, EL HARFI K. Effects of acid treatments on Moroccan Tarfaya oil shale and pyrolysis of oil shale and their kerogen[J]. J Fuel Chem Technol, 2009, 37(6):659-667. doi: 10.1016/S1872-5813(10)60013-8
[26]	刘建忠, 齐庆杰, 周俊虎, 曹欣玉, 岑可法.煤中氟化物在燃烧产物中的分布特征[J].环境科学, 2003, 24(4):127-130. doi: 10.3321/j.issn:0250-3301.2003.04.025 LIU Jian-zhong, QI Qing-jie, ZHOU Jun-hu, CAO Xin-yu, CEN Ke-fa. Distribution of fluoride in the combustion products of coal[J]. Environ Sci, 2003, 24(4):127-130. doi: 10.3321/j.issn:0250-3301.2003.04.025
[27]	蒋旭光, 徐旭, 严建华, 何杰, 池涌, 岑可法.煤燃烧过程中氯析出特性的试验研究[J].煤炭学报, 2002, 27(4):398-401. doi: 10.3321/j.issn:0253-9993.2002.04.014 JIANG Xu-guang, XU Xu, YAN Jian-hua, HE Jie, CHI Yong, CEN Ke-fa. Experimental study on the release characteristic of chlorine in coal combustion process[J]. J China Coal Soc, 2002, 27(4):398-401. doi: 10.3321/j.issn:0253-9993.2002.04.014
[28]	GELINAS Y, BALDOCK J A, HEDGES J I. Demineralization of marine and freshwater sediments for CP/MAS 13C NMR analysis[J]. Org Geochem, 2001, 32(5):677-693. doi: 10.1016/S0146-6380(01)00018-3
[29]	ZHAO X S, LIU Z Y, LU Z H, SHI L, LIU Q Y. A study on average molecular structure of eight oil shale organic matters and radical information during pyrolysis[J]. Fuel, 2018, 219:399-405. doi: 10.1016/j.fuel.2018.01.046
[30]	HILLIER J L, FLETCHER T H, SOLUM M S, PUGMIRE R J. Characterization of macromolecular structure of pyrolysis products from a Colorado Green River oil shale[J]. Ind Eng Chem Res, 2013, 52(44):15522-15532. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=03237402c85d458cbb882a4130fdadb3
[31]	KOSATEVA A, STEFANOVA M, MARINOV S, CZECH J, CARLEER R, YPERMAN J. Characterization of organic components in leachables from Bulgarian lignites by spectroscopy, chromatography and reductive pyrolysis[J]. Int J Coal Geol, 2017, 183:100-109. doi: 10.1016/j.coal.2017.10.005
[32]	LI Q Y, HAN X X, LIU Q Q, JIANG X M. Thermal decomposition of Huadian oil shale. Part 1. Critical organic intermediates[J]. Fuel, 2014, 121:109-116. doi: 10.1016/j.fuel.2013.12.046
[33]	石剑, 李术元, 马跃.爱沙尼亚油页岩及其热解产物的电子顺磁共振研究[J].燃料化学学报, 2018, 46(1):1-7. doi: 10.3969/j.issn.0253-2409.2018.01.001 SHI Jian, LI Shu-yuan, MA Yue. Electron paramagnetic resonance (EPR) properties of Estonia oil shale and its pyrolysates[J]. J Fuel Chem Technol, 2018, 46(1):1-7. doi: 10.3969/j.issn.0253-2409.2018.01.001
[34]	PAN L W, DAI F Q, HUANG J N, LIU S, LI G Q. Study of the effect of mineral matters on the thermal decomposition of Jimsar oil shale using TG-MS[J]. Thermochim Acta, 2016, 627:31-38. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=49b42da1b671a61ba510f15fa6c1cbbd
[35]	TORRENTE M C, GALAN M A. Kinetics of the thermal decomposition of oil shale from Puertollano (Spain)[J]. Fuel, 2001, 80(3):327-334. doi: 10.1016/S0016-2361(00)00101-0