亚临界水处理模拟有机-矿质复合体形成机制探讨

Abstract
Figure/Table
References (40)
Related Citation (15)

Download: PDF (682 KB) HTML (1 KB)
Export: BibTeX | EndNote (RIS)

Abstract

Humification of organic matter and formation of organic-mineral complexes were simulated with subcritical water treatment method. A series of samples containing commercial humic acid, kaolin, and organic-mineral complexes were prepared under designed temperature, pressure and reaction time, respectively, in a high-temperature and high-pressure reaction kettle. Changing characteristic and mechanism of these samples under different conditions were investigated by means of specific surface area analysis (SSA), Fourier infrared spectrum (FTIR), particular wavelength absorbance ratio (E₄/E₆), X-ray diffraction (XRD) and ¹³C nuclear magnetic resonance (¹³C-NMR). The results showed that SSA, molecular weight, and degree of aromatization (from 59.52% to 70.90%) of humic acids increased significantly with increasing temperature and pressure. This was caused by the cyclization and polymerization of free carboxyl and chain hydrocarbon in humic acid, which led to a more complicated structure and an improvement of chemical stability of humic acids. Increasing temperature and pressure resulted in dehydration and a complete and orderly structure of kaolin. There were several interactions involved in the formation of organic-mineral complexes. At first, aromatic components of humic acid intercalated into kaolin and caused a relatively dense inner structure. Then, the cyclized and polymerized free carboxyl, alkanes and chain structures patched loosely on the kaolin and formed the outer space. The change trend of humic acid, kaolin and their complexes in the experiments was consistent with the direction of mineralization and humification of these substances in nature.

Key words： humic acid kaolin organic-mineral complexes subcritical water treatment method

Received: 06 March 2016

X523

	Service

	E-mail this article
	Add to my bookshelf
	Add to citation manager
	E-mail Alert
	RSS
	Articles by authors
	WANG Fei
	HE Jiang-tao
	HE Bao-nan

Cite this article:

WANG Fei,HE Jiang-tao,HE Bao-nan. Formation mechanism of organic-mineral complexes simulated by subcritical water treatment method[J]. CHINA ENVIRONMENTAL SCIENCECE, 2016, 36(8): 2495-2504.

URL:

http://www.zghjkx.com.cn/EN/ OR http://www.zghjkx.com.cn/EN/Y2016/V36/I8/2495

[1]	Schmidt M W, Torn M, Abiven S, et al. Persistence of soil organic matter as an ecosystem property[J]. Nature, 2011,478(7367): 49-56.
[2]	Theng B, Hashizume H. Clay-activated transformation of humic acid at high pressure and temperature[J]. Applied Clay Science, 1996,10(6):431-437.
[3]	Kenji O, Keizo H, Sayaka M, et al. Organic carbon accumulation processes on a forest floor during an early humification stage in a temperate deciduous forest in Japan: Evaluations of chemical compositional changes by 13C NMR and their decomposition rates from litterbag experiment[J]. Geoderma, 2009,151(3/4): 351-356.
[4]	Funatsu T, Seto M, Shimada H, et al. Combined effects of increasing temperature and confining pressure on the fracture toughness of clay bearing rocks[J]. International Journal of Rock Mechanics and Mining Sciences, 2004,41(6):927-938.
[5]	Larissa C C, Rommulo V C, Norberto D, et al. Structural changes of potassium-saturated smectite at high pressures and high temperatures: Application for subduction zones[J]. Applied Clay Science, 2014,102:164-171.
[6]	张美芳,樊孝俊.BDE-47在土壤矿物质与有机质上的吸附解吸特征[J]. 中国环境监测, 2015,31(4):82-85.
[7]	曹罡,莫汉宏,安凤春.除草剂2,4-D在胡敏酸上的吸附[J]. 环境科学学报, 2002,22(1):120-122.
[8]	张晓林,邹道安,池涌.十氯联苯的超(亚)临界水降解特性[J]. 环境科学学报, 2015,7(2):2099-2106.
[9]	Hawthorne S B, Yang Y, Miller D J. Extraction of organic pollutants from environmental solid with sub and supereritieal water[J]. Analytieal Chemistry, 1994,66(11):2912-2920.
[10]	Miller D J, Hawthorne S B.Solubility of liquid organics of environmental interest in subcritieal(Hot/Liquid) water from 298K to 473K[J]. J.Chem. Eng. Data., 2000,45(1):78-81.
[11]	Alan R, Steven M, et al. Aquathermolvsis: reactions of organic compounds with superheated water[J]. Accounts of Chemical Research, 1996,29(8):399-406.
[12]	Johnson M D, Huang W L, Weber W J. A distributed reactivity model for sorption by soils and sedments. 13. simulated diagenesis of sediment organic matter and its impact on sorption/desorption equilibria[J]. Environmental Science and Technology. 2001,35(8):1680-1687.
[13]	Lopez L, Rovira P. Sequential chemical extractions of the mineral-associated soil organic matter: An integrated approach for the fractionation of organo-mineral complexes[J]. Soil Biology and Biochemistry, 2013,62(10):57-67.
[14]	Hickey J P, Passino D R. Linear solvation energy relationships: "rule of thumb" for estimation of variable values[J]. Environmental Science and Technology, 1991,25(10):1753-1760.
[15]	周国清.粘土矿物的热模拟研究[J]. 石油实验地质, 1995, 17(3):286-292.
[16]	姬景超,刘钦甫,张士龙,等.插层-磨剥法制备不同径厚比的高岭石[J]. 矿物学报, 2015,35(2):197-202.
[17]	包镇红,江伟辉,苗立锋,等.几种常用高岭土的组成和结构比较[J]. 陶瓷学报, 2014,35(1):53-56.
[18]	Balan E, Saitta A M, Mauti F, et al. First-principles modeling of the infrared spectrum of kaolinite[J]. American Mineralogist. 2001,86(12):1321-1330.
[19]	李小红,江向平,陈超,等.几种不同产地高岭土的漫反射傅里叶红外光谱分析[J]. 光谱学与光谱分析, 2011,31(1):114-118.
[20]	宋冠群,林金明.环境样品中多环芳烃的前处理技术[J]. 环境科学学报, 2005,25(10):1287-1296.
[21]	窦森,张继宏,颜丽.农业持续发展的土壤培肥研究[M]. 沈阳:东北大学出版社, 1995:23-25.
[22]	钱国平,钱进.安徽省地带性土壤腐殖质组成和性质[J]. 土壤, 1992,25(2):58-62.
[23]	刘丽琼,江韬,魏世强,等.胡敏酸对不同矿物结合汞的还原作用[J]. 中国环境科学, 2011,31(12):1998-2004.
[24]	任东,杨小霞,马晓冬,等. DOM结构特征及其对17β-雌二醇光降解的影响[J]. 中国环境科学, 2015,35(5):1375-1383.
[25]	Cook R L, Langford C H. Structual characterization of a fulvic acid and a humic acid using solid state ramp-CP-MAS C-13nuclear magnetic resonance. Environmental Science and Technology, 1998,32(5):719-725.
[26]	Gunasekara A S, Xing B S. Sorption and desorption of naphthalene by soil organic matter: importance of aromatic and aliphatic components[J]. Journal of Environmental quality, 2003,32(1):240-246.
[27]	Simpson M J, Hatcher P G. Determination of black carbon in natural organic matter by chemical oxidation and solid-state 13C nuclear magnetic resonance spectroscopy[J]. Organic Geochemistry, 2004,35(8):923-935.
[28]	Simpson M J, Simpson A J, Hatcher P G. Noncovalent interactions between aromatic compounds and dissolved humic acid examined by nuclear magnetic resonance spectroscopy[J]. Environmental Toxicology and Chemistry, 2004,23(2):355-362.
[29]	Xing B S, Chen Z Q. Spectroscopic evidence for condensed domins in soil organic matter[J]. Soil Science, 1999,164(1): 40-47.
[30]	Kile D E, Wershaw R L, Chiou C T. Correlation of soil and sediment organic matter polarity to aqueous sorption of nonionic compounds[J]. Environmental Science and Technology, 1999, 33(12):2053-2056.
[31]	陈梦妍,朱亮,张静.腐殖酸对高锰酸钾氧化苯酚的影响及其作用机制[J]. 中国环境科学, 2015,35(10):3041-3045.
[32]	朱晓婧,何江涛,苏思慧.腐殖酸-高岭土复合体形成机制及对三氯乙烯的吸附[J]. 环境科学, 2015,36(1):227-236.
[33]	Kolokassidou C, Pashalidis I, Costa C N, et al. Thermal stability of solid and aqueous solutions of humic acid[J]. Thermochimica Acta, 2007,454(2):78-83.
[34]	Ellerbrock R, Kaiser M. Stability and composition of different soluble soil organic matte fractionsá-áevidence from[delta] 13C and FTIR signatures[J]. Geoderma, 2005,12(8):28-37.
[35]	厦华,佟健,侯常娥.高岭石——聚丙烯腈夹层复合物的制备[J]. 矿物岩石, 2001,21(4):7-10.
[36]	张生辉,周亚冲,欧雪梅,等. FTIR和XRD研究甲酰胺在高岭石插层复合体系中的形态及其复合物的微观结构[J]. 光谱学与光谱分析, 2013,33(11):2978-2982.
[37]	左小超,刘钦甫,姬景超,等.脂肪酸/高岭石插层复合物的制备及结构模型[J]. 硅酸盐学报, 2015,43(9):1294-1299.
[38]	Aparicio P, Galan E. Mineralogical interference on kaolinite crystallinity index measurements[J]. Clays and Clay Minerals, 1999,47(1):12-27.
[39]	Wiewiora A, Brindley G W. Potassium acetate intercalation kaolinites and its removal: effect of material characteristic[M]. Jerusalem, 1969,723-733.
[40]	Mayes M, Jagadamma S, Ambaye H. Neutron reflectometry reveals the internal structure of organic compounds deposited on aluminum oxide[J]. Geoderma, 2013,192:182-188.