Typical redox-sensitive components in groundwater systems: Research highlights and trends

doi:10.13745/j.esf.sf.2022.1.37

Abstract

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

CLC Number:

X523

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.

Figures/Tables 4

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

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

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

Fig.2 Nitrogen cycling related to As enrichment in groundwater

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

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