Effect of pressure on C-N-S-Fe-H2O system in sil

doi:10.13745/j.esf.sf.2021.2.9

Abstract

Abstract:

Carbon, N, S and Fe are the main elements controlling the redox reactions in groundwater. Silt is the initial form of clay, and its transformation into clay can affect the quantity and quality of groundwater aquifers. Groundwater pollution may happen during the transformation process, where the water-rock interaction can be generalized as the C-N-S-Fe-H₂O interaction system. The essence of silt evolution is porosity reduction under pressure and gradual consolidation into rocks. Biogeochemical reactions take place in silt while the C-N-S-Fe-H₂O interaction system drives constant changes in the substance forms. Pressurization rates and modes can affect the transformation of important components, such as C, N, S and Fe, between solid and liquid phase in silt. This experiment studies the release of C, N, S and Fe to pore water under three pressurization rates (0.04 MPa per 12 h, 24 h, 36 h) and three pressurization modes (decelerating, from 0.04 to 0.02 MPa/12 h; uniform, 0.04 MPa/12 h; accelerating, from 0.04 to 0.06 MPa/12 h), using self-developed pressurization device. The results show: (1) Slower uniform pressurization rate corresponds to faster DOC, $SO 4 2 -$ release rate, more $NO 3 -$ , Fe²⁺concentration change, and more DOC, $SO 4 2 -$ , $NO 3 -$ , Fe²⁺release. (2) $NO 3 -$ , Fe²⁺ concentration fluctuation increases under accelerating pressurization, and the total DOC, $SO 4 2 -$ , $NO 3 -$ , Fe²⁺ release is greater during accelerating pressurization versus uniform pressurization. (3) During pressurization, DOC and $SO 4 2 -$ concentrations are positively correlated, and pressurization rate change can change the DOC, $NO 3 -$ , $SO 4 2 -$ , Fe²⁺ correlations. It shows that changing the pressurization rates and modes can affect DOC, $SO 4 2 -$ , $NO 3 -$ , Fe²⁺ release rate/quantity as well as C, N, S, Fe transformation, that is, essentially changing the magnitudes of redox reaction and water-rock interaction. This experiment provides a new understanding of the main elemental changes caused by pressure in the process of geological evolution, and demonstrates the aquitards can affect water quality/quantity in aquifer. This study provides new insights into the cause of naturally inferior groundwater and prevention of groundwater pollution.

Key words: pressure, pressurization rate, pressurization mode, silt, C-N-S-Fe-H₂O, pore water

CLC Number:

X523

PENG Ziqi, MA Teng, LIU Yanjun, CHEN Juan, QIU Wenkai, LIU Rui. Effect of pressure on C-N-S-Fe-H2O system in sil[J]. Earth Science Frontiers, 2021, 28(5): 79-89.

Figures/Tables 19

Fig.1 Change of water quantity during pressurization

Fig.2 Change of K+, Ca2+, Na2+, Mg2+ concentration and Eh in pore water under 0.04 MPa/12 h pressurization

Fig.3 Change of DOC concentration in pore water under different pressurization rates

Fig.4 Change of SO 4 2 - concentration in pore water under different pressurization rates

Fig.5 Change of NO 3 - concentration in pore water under different pressurization rates

Fig.6 Change of Fe2+ concentration in pore water under different pressurization rates

Fig.7 Change of DOC concentration in pore water under different pressurization modes

Fig.8 Change of SO 4 2 - concentration in pore water under different pressurization modes

Fig.9 Change of NO 3 - concentration in pore water under different pressurization modes

Fig.10 Change of Fe2+ concentration in pore water under different pressurization modes

Fig.11 Total DOC under different pressurization rates and modes

Fig.12 Total SO 4 2 -under different pressurization rates and modes

Fig.13 Total NO 3 - under different pressurization rates and modes

Fig.14 Total Fe2+ under different pressurization rates and modes

Table 1 DOC, NO 3 -, S O 4 2 -, Fe2+ correlations under 0.04 MPa/12 h pressurization

指标	各指标间相关系数
指标	DOC	$NO 3 -$	$SO 4 2 -$	Fe²⁺
DOC	1	0.596	0.975^**	0.184
$NO 3 -$	0.596	1	0.988^*	0.387^**
$SO 4 2 -$	0.975^**	0.988^*	1	0.806
Fe²⁺	0.184	0.387^**	0.806	1

Table 1 DOC, NO 3 -, S O 4 2 -, Fe2+ correlations under 0.04 MPa/12 h pressurization

指标	各指标间相关系数
指标	DOC	$NO 3 -$	$SO 4 2 -$	Fe²⁺
DOC	1	0.596	0.975^**	0.184
$NO 3 -$	0.596	1	0.988^*	0.387^**
$SO 4 2 -$	0.975^**	0.988^*	1	0.806
Fe²⁺	0.184	0.387^**	0.806	1

Table 2 DOC, NO 3 -, S O 4 2 -, Fe2+correlations under 0.04 MPa/24 h pressurization

指标	各指标间相关系数
指标	DOC	$NO 3 -$	$SO 4 2 -$	Fe²⁺
DOC	1	0.489^**	0.869^**	0.573^**
$NO 3 -$	0.489^**	1	0.861^**	0.198
$SO 4 2 -$	0.869^**	0.861^**	1	0.589^**
Fe²⁺	0.573^**	0.198	0.589^**	1

Table 2 DOC, NO 3 -, S O 4 2 -, Fe2+correlations under 0.04 MPa/24 h pressurization

指标	各指标间相关系数
指标	DOC	$NO 3 -$	$SO 4 2 -$	Fe²⁺
DOC	1	0.489^**	0.869^**	0.573^**
$NO 3 -$	0.489^**	1	0.861^**	0.198
$SO 4 2 -$	0.869^**	0.861^**	1	0.589^**
Fe²⁺	0.573^**	0.198	0.589^**	1

Table 3 DOC, NO 3 -, S O 4 2 -, Fe2+correlations under 0.04 MPa/36 h pressurization

指标	各指标间相关系数
指标	DOC	$NO 3 -$	$SO 4 2 -$	Fe²⁺
DOC	1	0.269	0.635^**	0.049
$NO 3 -$	0.269	1	0.041	0.376
$SO 4 2 -$	0.635^**	0.041	1	0.085
Fe²⁺	0.049	0.376	0.085	1

Table 3 DOC, NO 3 -, S O 4 2 -, Fe2+correlations under 0.04 MPa/36 h pressurization

指标	各指标间相关系数
指标	DOC	$NO 3 -$	$SO 4 2 -$	Fe²⁺
DOC	1	0.269	0.635^**	0.049
$NO 3 -$	0.269	1	0.041	0.376
$SO 4 2 -$	0.635^**	0.041	1	0.085
Fe²⁺	0.049	0.376	0.085	1

Table 4 DOC, NO 3 -, S O 4 2 -, Fe2+correlations under 0.04-0.06 MPa/12 h pressurization

指标	各指标间相关系数
指标	DOC	$NO 3 -$	$SO 4 2 -$	Fe²⁺
DOC	1	0.206	0.906^**	0.595*
$NO 3 -$	0.206	1	0.241	0.604^*
$SO 4 2 -$	0.906^**	0.241	1	0.783^**
Fe²⁺	0.595^*	0.604^*	0.783^**	1

Table 4 DOC, NO 3 -, S O 4 2 -, Fe2+correlations under 0.04-0.06 MPa/12 h pressurization

指标	各指标间相关系数
指标	DOC	$NO 3 -$	$SO 4 2 -$	Fe²⁺
DOC	1	0.206	0.906^**	0.595*
$NO 3 -$	0.206	1	0.241	0.604^*
$SO 4 2 -$	0.906^**	0.241	1	0.783^**
Fe²⁺	0.595^*	0.604^*	0.783^**	1

Table 5 DOC, NO 3 -, S O 4 2 -, Fe2+correlations under 0.04-0.02 MPa/12 h pressurization

指标	各指标间相关系数
指标	DOC	$NO 3 -$	$SO 4 2 -$	Fe²⁺
DOC	1	0.817^**	0.804^**	0.517^**
$NO 3 -$	0.817^**	1	0.808^**	0.324
$SO 4 2 -$	0.804^**	0.808^**	1	0.364
Fe²⁺	0.517^**	0.324	0.364	1

Table 5 DOC, NO 3 -, S O 4 2 -, Fe2+correlations under 0.04-0.02 MPa/12 h pressurization

指标	各指标间相关系数
指标	DOC	$NO 3 -$	$SO 4 2 -$	Fe²⁺
DOC	1	0.817^**	0.804^**	0.517^**
$NO 3 -$	0.817^**	1	0.808^**	0.324
$SO 4 2 -$	0.804^**	0.808^**	1	0.364
Fe²⁺	0.517^**	0.324	0.364	1

References 31

[1]	HUNTER K S, WANG Y F, VAN CAPPELLEN P V . Kinetic modeling of microbially-driven redox chemistry of subsurface environments: coupling transport, microbial metabolism and geochemistry[J]. Journal of Hydrology, 1998, 209(1/2/3/4):53-80. DOI URL
[2]	MYERS C R, NEALSON K H. Microbial reduction of manganese oxides: interactions with iron and sulfur[J]. Geochimica et Cosmochimica Acta, 1988, 52(11):2727-2732. DOI URL
[3]	罗莎莎, 万国江. 云贵高原湖泊沉积物: 水界面铁、锰、硫体系的研究进展[J]. 地质地球化学, 1999, 27(3):47-52.
[4]	朱茂旭, 史晓宁, 杨桂朋, 等. 海洋沉积物中有机质早期成岩矿化路径及其相对贡献[J]. 地球科学进展, 2011, 26(4):355-364.
[5]	邓通初. 黑臭河涌沉积物中硝酸盐还原硫氧化微生物氮硫共去除特性[D]. 南昌: 江西农业大学, 2015.
[6]	李学刚, 宋金明. 海洋沉积物中碳的来源、迁移和转化[G]//海洋科学集刊. 北京: 科学出版社, 2004: 106-117.
[7]	何永胜, 胡东平, 朱传卫. 地球科学中铁同位素研究进展[J]. 地学前缘, 2015, 22(5):54-71.
[8]	HUERTA-DIAZ M A, MORSE J W. A quantitative method for determination of trace metal concentrations in sedimentary pyrite[J]. Marine Chemistry, 1990, 29(2/3):119-144. DOI URL
[9]	MORSE J W, LUTHER G W III . Chemical influences on trace metal-sulfide interactions in anoxic sediments[J]. Geochimica et Cosmochimica Acta, 1999, 63(19/20):3373-3378. DOI URL
[10]	赵由之. 高原湖泊沉积物中硫形态分布与微生物地球化学行为[D]. 贵阳: 中国科学院地球化学研究所, 2006.
[11]	吴丰昌. 云贵高原湖泊沉积物和水体氮、磷和硫的生物地球化学作用和生态环境效应(摘要)[J]. 地质地球化学, 1996, 24(6):88-89.
[12]	邓峰煜. 长江口硝酸盐异化还原过程及其影响因素研究[D]. 上海: 华东师范大学, 2016.
[13]	BERG P, RISGAARD-PETERSEN N, RYSGAARD S. Interpretation of measured concentration profiles in sediment pore water[J]. Limnology and Oceanography, 1998, 43(7):1500-1510. DOI URL
[14]	周志芳, 徐海洋. 一种实验确定弱透水层水文地质参数的原理与方法[J]. 水文地质工程地质, 2014, 41(5):1-4.
[15]	WANG Y X, MA T, RYZHENKO B N, et al. Model for the formation of arsenic contamination in groundwater.1. Datong Basin, China[J]. Geochemistry International, 2009, 47(7):713-724. DOI URL
[16]	WANG Y, JIAO J J, CHERRY J A, et al. Contribution of the aquitard to the regional groundwater hydrochemistry of the underlying confined aquifer in the Pearl River Delta, China[J]. Science of the Total Environment, 2013, 461/462:663-671.
[17]	LIU Y J, MA T, CHEN J, et al. Contribution of clay-aquitard to aquifer iron concentrations and water quality[J]. Science of the Total Environment, 2020, 741:140061.
[18]	POLIZZOTTO M L, KOCAR B D, BENNER S G, et al. Near-surface wetland sediments as a source of arsenic release to ground water in Asia[J]. Nature, 2008, 454(7203):505-508. DOI URL
[19]	MIHAJLOV I, MOZUMDER M R, BOSTICK B C, et al. Arsenic contamination of Bangladesh aquifers exacerbated by clay layers[J]. Nature Communications, 2020, 11(1):2244. DOI URL
[20]	SMITH R, KNIGHT R, FENDORF S. Over pumping leads to California groundwater arsenic threat[J]. Nature Communications, 2018, 9:2089. DOI URL
[21]	MAZUREK M, OYAMA T, WERSIN P, et al. Pore-water squeezing from indurated shales[J]. Chemical Geology, 2015, 400:106-121. DOI URL
[22]	OKIONGBO K S, AKPOFURE E. Hydrogeophysical characterization of shallow unconsolidated alluvial aquifer in yenagoa and environs, southern Nigeria[J]. Arabian Journal for Science and Engineering, 2016, 41(6):2261-2270. DOI URL
[23]	MAZUREK M, ALT-EPPING P, BATH A, et al. Natural tracer profiles across argillaceous formations[J]. Applied Geochemistry, 2011, 26(7):1035-1064. DOI URL
[24]	HENDRY M J, WASSENAAR L I. Transport and geochemical controls on the distribution of solutes and stable isotopes in a thick clay-rich till aquitard, Canada[J]. Isotopes in Environmental and Health Studies, 2004, 40(1):3-19. DOI URL
[25]	SCHAEFER M V, GUO X X, GAN Y Q, et al. Redox controls on arsenic enrichment and release from aquifer sediments in central Yangtze River Basin[J]. Geochimica et Cosmochimica Acta, 2017, 204:104-119. DOI URL
[26]	ERBAN L E, GORELICK S M, ZEBKER H A, et al. Release of arsenic to deep groundwater in the Mekong Delta, Vietnam, linked to pumping-induced land subsidence[J]. Proceedings of the National Academy of Sciences of the United States of America, 2013, 110(34):13751-13756.
[27]	THAMDRUP B. Bacterial manganese and iron reduction in aquatic sediments[J]. Advances in Microbial Ecology, 2000, 16:41-84.
[28]	HENDRY M J, SCHWARTZ F W. An alternative view on the origin of chemical and isotopic patterns in groundwater from the Milk River Aquifer, Canada[J]. Water Resources Research, 1988, 24(10):1747-1763. DOI URL
[29]	LIU Y J, MA T, DU Y. Compaction of muddy sediment and its significance to groundwater chemistry[J]. Procedia Earth and Planetary Science, 2017, 17:392-395. DOI URL
[30]	陈娟, 马腾, 刘妍君, 等. 不同压力条件下淤泥中铵氮的释放特性[J]. 安全与环境工程, 2020, 27(4):110-120.
[31]	周俊丽. 长江口湿地生态系统中有机质的生物地球化学过程研究: 以崇明东滩为例[D]. 上海: 华东师范大学, 2005.