地下水典型氧化还原敏感组分迁移转化的研究热点和趋势

doi:10.13745/j.esf.sf.2022.1.37

摘要/Abstract

摘要：

C-N-S反应体系是地下水系统中氧化还原敏感组分循环和能量流动的关键系统,但它如何与Fe、Mn循环过程、相关功能微生物代谢路径耦合并控制氧化还原敏感组分的迁移转化却并不清楚。本文在对国内外相关文献进行归纳总结的基础上,把地下水中的氧化还原敏感组分分为氧化富集型和还原富集型,较为系统地梳理了地下水系统C、N、S循环驱动的典型氧化还原敏感组分(主要以U、Cr、Fe、As为例)迁移转化过程,指出了该领域的主要研究热点,包括C-N反应体系中典型氧化还原敏感组分的迁移转化、C-S反应体系中还原富集型组分活化和氧化富集型组分固定机理、典型氧化还原敏感组分之间的相互作用、微生物作用下典型氧化还原敏感组分的转化和富集等,并提出基于代谢路径的C-N-S反应体系及其驱动下地下水典型氧化还原敏感组分转化过程和富集机理,将成为本领域的发展趋势。

关键词: 含水系统, 砷, 铀, 微生物, 同位素, 水岩相互作用

Abstract:

Although C, N, S cycling is essential to cycling of redox-sensitive components and energy flux in groundwater systems, the mechanism of its couplings to Fe-Mn cycling and relavent functional microbial metabolic pathway in controlling the transport and transformation of redox-sensitive components is poorly understood. Based on comprehensive national and international literature surveys, this paper divided the groundwater redox-sensitive components into oxic condition-related enrichment type (oxic type, enriched in oxic groundwater) and reducing condition-related enrichment type (reducing type, enriched in reducing groundwater), and systematically sorted out C, N, and/or S cycling-driven transport and transformation processes of typical redox-sensitive components (U, Cr, Fe, As as main examples) in groundwater systems. The research highlights of the relevant research fields mainly included coupling of C, N cycling and transport-transformation of typical redox-sensitive components, C, S cycling-driven mechanisms for the mobilization of reducing type components and the immobilization of the oxic type components, hydrogeochemical interactions bewteen typical redox-sensitive components, and microbe-mediated transformation and enrichment of typical redox-sensitive components. The research trends revealed by this study were metabolic pathway-based C, N, S cycling and its control on the transformation processes and enrichment mechanisms of typical redox-sensitive components in groundwater systems.

Key words: aquifer system, arsenic, uranium, microbe, isotope, water-rock interaction

中图分类号:

X523

郭华明, 高志鹏, 修伟. 地下水典型氧化还原敏感组分迁移转化的研究热点和趋势[J]. 地学前缘, 2022, 29(3): 64-75.

GUO Huaming, GAO Zhipeng, XIU Wei. Typical redox-sensitive components in groundwater systems: Research highlights and trends[J]. Earth Science Frontiers, 2022, 29(3): 64-75.

图/表 4

图1 典型干旱-半干旱盆地地下水砷、铀浓度关系图(据文献[13⇓⇓⇓⇓-18])

Fig.1 Relationship between As and U concentrations in groundwaters of typical arid-semiarid basins. Adapted from [13⇓⇓⇓⇓-18].

表1 C-N-S反应体系对As、U、Cr迁移转化影响的主要化学反应及其热力学参数

Table 1 The main chemical reactions of As, U, and Cr transform affected by the C-N-S reaction system and the related thermodynamic parameters

反应体系	化学反应式	标准状态 ΔG⁰/(kJ·mol^-1)	与氧化还原敏感组分的关系
C-Fe-(As)体系	CH₃COO^-+8Fe(OH)₃+15H⁺=2 $HCO 3 -$ +8Fe²⁺+20H₂O	-612^[28]	砷释放
	C₃H₅ $O 3 -$ +4Fe(OH)₃+7H⁺=CH₃COO^-+ $HCO 3 -$ +4Fe²⁺+10H₂O	-347.3^[28]	砷释放
	CH₂O +7CO₂+4Fe(OH)₃=4Fe²⁺+8 $HCO 3 -$ +3H₂O	-114^[29]	砷释放
	CH₄+8 Fe(OH)₃+15H⁺= $HCO 3 -$ +8Fe²⁺+21H₂O	-494.37^[30]*	砷释放
	Fe²⁺+ $CO 3 2 -$ =FeCO₃	-62.2^[31]	砷去除
N-Fe-(As)体系	2 $NO 2 -$ +6Fe²⁺+8H⁺=6Fe³⁺+N₂+4H₂O	-438^[32]	砷去除
	2 $NO 3 -$ +10Fe²⁺+12H⁺=10Fe³⁺+N₂+6H₂O	-457^[32]	砷去除
	3Fe(OH)₃+5H⁺+NH₄₊=3Fe²⁺+9H₂O +0.5N₂	-245^[32]	砷释放
S-Fe-(As)体系	2Fe(OH)₃+HS^-+5H⁺=2Fe²⁺+S⁰+6H₂O	-175.4^[30]*	砷释放
	10S⁰+4Fe(OH)₃=4Fe²⁺+3 $SO 4 2 -$ +7HS^-+5H⁺	369.5^[30]*	砷释放
	FeS₂+14Fe(OH)₃+15 $HCO 3 -$ +11H⁺=15FeCO₃+2 $SO 4 2 -$ +34H₂O	-806^[33]	砷释放
	FeS +8Fe(OH)₃+9 $HCO 3 -$ +7H⁺=FeCO₃+ $SO 4 2 -$ +20H₂O	-515^[33]	砷释放
	Fe²⁺+H₂S=FeS +H₂ (g)	-45^[34]	砷去除
N-Cr体系	6 $NO 3 -$ +10Cr(OH)₃=10Cr $O 4 2 -$ +8H₂O +3N₂+14H⁺	-181.15^[31]	铬释放
N-U体系 (以U $O 2 2 +$ 为例)	5UO₂+2 $NO 3 -$ +12H⁺=5U $O 2 2 +$ +6H₂O +N₂	-973.3^[31,35]	铀释放

表1 C-N-S反应体系对As、U、Cr迁移转化影响的主要化学反应及其热力学参数

Table 1 The main chemical reactions of As, U, and Cr transform affected by the C-N-S reaction system and the related thermodynamic parameters

反应体系	化学反应式	标准状态 ΔG⁰/(kJ·mol^-1)	与氧化还原敏感组分的关系
C-Fe-(As)体系	CH₃COO^-+8Fe(OH)₃+15H⁺=2 $HCO 3 -$ +8Fe²⁺+20H₂O	-612^[28]	砷释放
	C₃H₅ $O 3 -$ +4Fe(OH)₃+7H⁺=CH₃COO^-+ $HCO 3 -$ +4Fe²⁺+10H₂O	-347.3^[28]	砷释放
	CH₂O +7CO₂+4Fe(OH)₃=4Fe²⁺+8 $HCO 3 -$ +3H₂O	-114^[29]	砷释放
	CH₄+8 Fe(OH)₃+15H⁺= $HCO 3 -$ +8Fe²⁺+21H₂O	-494.37^[30]*	砷释放
	Fe²⁺+ $CO 3 2 -$ =FeCO₃	-62.2^[31]	砷去除
N-Fe-(As)体系	2 $NO 2 -$ +6Fe²⁺+8H⁺=6Fe³⁺+N₂+4H₂O	-438^[32]	砷去除
	2 $NO 3 -$ +10Fe²⁺+12H⁺=10Fe³⁺+N₂+6H₂O	-457^[32]	砷去除
	3Fe(OH)₃+5H⁺+NH₄₊=3Fe²⁺+9H₂O +0.5N₂	-245^[32]	砷释放
S-Fe-(As)体系	2Fe(OH)₃+HS^-+5H⁺=2Fe²⁺+S⁰+6H₂O	-175.4^[30]*	砷释放
	10S⁰+4Fe(OH)₃=4Fe²⁺+3 $SO 4 2 -$ +7HS^-+5H⁺	369.5^[30]*	砷释放
	FeS₂+14Fe(OH)₃+15 $HCO 3 -$ +11H⁺=15FeCO₃+2 $SO 4 2 -$ +34H₂O	-806^[33]	砷释放
	FeS +8Fe(OH)₃+9 $HCO 3 -$ +7H⁺=FeCO₃+ $SO 4 2 -$ +20H₂O	-515^[33]	砷释放
	Fe²⁺+H₂S=FeS +H₂ (g)	-45^[34]	砷去除
N-Cr体系	6 $NO 3 -$ +10Cr(OH)₃=10Cr $O 4 2 -$ +8H₂O +3N₂+14H⁺	-181.15^[31]	铬释放
N-U体系 (以U $O 2 2 +$ 为例)	5UO₂+2 $NO 3 -$ +12H⁺=5U $O 2 2 +$ +6H₂O +N₂	-973.3^[31,35]	铀释放

图2 与地下水砷富集有关的N循环过程

Fig.2 Nitrogen cycling related to As enrichment in groundwater

图3 C-S反应体系中地下水系统的铁氧化物还原和砷迁移转化过程

Fig.3 Reduction of Fe oxides and As transform in the C-S reaction system of groundwaters

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