Abstract
Microbially mediated NO3−-N and Cr(VI) reduction is being recognized as an eco-friendly and cost-effective remediation strategy. Iron sulfide mineral, as a natural inorganic electron donor, has a strong influence on NO3−-N and Cr(VI) transformation, respectively. However, little is known about the simultaneous nitrate and chromium removal performance and underlying mechanism in an iron sulfide mineral-involved mixotrophic biofilter. This study demonstrated that the NO3−-N and Cr(VI) removal efficiencies were stable at 62 ± 8% and 56 ± 10%, and most of them were eliminated in the 0–100-mm region of the biofilter. Cr(VI) was reduced to insoluble Cr(III) via microbial and chemical pathways, which was confirmed by the SEM–EDS morphology and the XPS spectra of biofilm and pyrite particles. SO42− was as a main byproduct of pyrite oxidation; however, the bacterial SO42− reduction synchronously occurred, evidenced by the variations of TOC and SO42− concentrations. These results suggested that there were complicated and intertwined biochemical relations between NO3−-N/Cr(VI)/SO42−/DO (electron acceptors) and pyrite/organics (electron donors). Further investigation indicated that both the maximal biomass and greatest denitrifiers’ relative abundances in microbial sample S1 well explained why the pollutants were removed in the 0–100-mm region. A variety of denitrifiers such as Pseudoxanthomona, Acidovorax, and Simplicispira were enriched, which probably were responsible for both NO3−-N and Cr(VI) removal. Our findings advance the understanding of simultaneous nitrate and chromium removal in pyrite-involved mixotrophic systems and facilitate the new strategy development for nitrate and chromium remediation.
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References
Burow KR, Nolan BT, Rupert MG, Dubrovsky NM (2010) Nitrate in groundwater of the United States, 1991–2003. Environ Sci Technol 44:4988–4997
Costa M (1997) Toxicity and carcinogenicity of Cr(VI) in animal models and humans. Crit Rev Toxicol 27:431–442
Demoisson F, Mullet M, Humbert B (2005) Pyrite oxidation by hexavalent chromium: investigation of the chemical processes by monitoring of aqueous metal species. Environ Sci Technol 39:8747–8752
Fruchter J (2002) In situ treatment of chromium-contaminated groundwater. Environ Sci Technol 36:464A-472A
Guo H, Chen Y, Hu H, Zhao K, Li H, Yan S, Xiu W, Coyte RM, Vengosh A (2020a) High hexavalent chromium concentration in groundwater from a deep aquifer in the Baiyangdian Basin of the North China Plain. Environ Sci Technol 54:10068–10077
Guo W, Cecchetti AR, Wen Y, Zhou Q, Sedlak DL (2020b) Sulfur cycle in a wetland microcosm: extended 34S-stable isotope analysis and mass balance. Environ Sci Technol 54:5498–5508
Guo W, Wen Y, Chen Y, Zhou Q (2020c) Sulfur cycle as an electron mediator between carbon and nitrate in a constructed wetland microcosm. Front Environ Sci Eng 14:57
Haaijer SCM, Lamers LPM, Smolders AJP, Jetten MSM, Op den Camp HJM (2007) Iron sulfide and pyrite as potential electron donors for microbial nitrate reduction in freshwater wetlands. Geomicrobiol J 24:391–401
Hausladen DM, Alexander-Ozinskas A, McClain C, Fendorf S (2018) Hexavalent chromium sources and distribution in california groundwater. Environ Sci Technol 52:8242–8251
He J, Zhang B, Wang Y, Chen S, Dong H (2023) Vanadate bio-detoxification driven by pyrrhotite with secondary mineral formation. Environ Sci Technol 57:1807–1818
Hu Y, Liu T, Chen N, Feng C (2022) Changes in microbial community diversity, composition, and functions upon nitrate and Cr(VI) contaminated groundwater. Chemosphere 288:132476
Kong Q, Guo W, Sun R, Qin M, Zhao Z, Du Y, Zhang H, Zhao C, Wang X, Zhang R, Zhang X (2021) Enhancement of chromium removal and energy production simultaneously using iron scrap as anodic filling material with pyrite-based constructed wetland-microbial fuel cell. J Environ Chem Eng 9:106630
Leiro JA, Mattila SS, Laajalehto K (2003) XPS study of the sulphur 2p spectra of pyrite. Surf Sci 547:157–161
Li Y, Han Q, Li B (2023) Engineering-scale application of sulfur-driven autotrophic denitrification wetland for advanced treatment of municipal tailwater. Biores Technol 379:129035
Liu Y, Gan H, Tian L, Liu Z, Ji Y, Zhang T, Alvarez PJJ, Chen W (2022) Partial oxidation of FeS nanoparticles enhances Cr(VI) sequestration. Environ Sci Technol 56:13954–13963
Lu J, Zhang B, He C, Borthwick AGL (2020) The role of natural Fe(II)-bearing minerals in chemoautotrophic chromium (VI) bio-reduction in groundwater. J Hazard Mater 389:121911
Manaka M (2023) Extent of pyrite oxidation by dissolved oxygen in alkaline solutions including purified sodium bentonite. Appl Geochem 148:105548
Nie X, Li G, Wang Y, Luo Y, Song L, Yang S, Wan Q (2022) Highly efficient removal of Cr(VI) by hexapod-like pyrite nanosheet clusters. J Hazard Mater 424:127504
Otero N, Torrentó C, Soler A, Menció A, Mas-Pla J (2009) Monitoring groundwater nitrate attenuation in a regional system coupling hydrogeology with multi-isotopic methods: The case of Plana de Vic (Osona, Spain). Agric. Ecosyst Environ 133:103–113
Pan J, Liu L, Pan H, Yang L, Su M, Wei C (2022) A feasibility study of metal sulfide (FeS and MnS) on simultaneous denitrification and chromate reduction. J Hazard Mater 424:127491
Park M, Kim S, Kim S, Ryu J, Song YS, Jeong HY (2022) Cr(VI) immobilization by FeS-coated alumina and silica: effects of pH and surface coating density. J Hazard Mater 421:126784
Peng L, Liu Y, Gao SH, Chen X, Ni BJ (2016) Evaluating simultaneous chromate and nitrate reduction during microbial denitrification processes. Water Res 89:1–8
Peng L, Peng Y, Xu Y, Liang C (2022) Heterotrophic bio-reduction process of hexavalent chromium: toxic effects, concentration-adaptation and sustainable sludge-based bio-augmentation strategy. J Clean Prod 370:133567
Rahman Z, Thomas L (2020) Chemical-assisted microbially mediated chromium (Cr) (VI) reduction under the influence of various electron donors, redox mediators, and other additiveS: an outlook on enhanced Cr(VI) removal. Front Microbiol 11:619766
Ramli NN, Othman AR, Kurniawan SB, Abdullah SRS, Hasan HA (2023) Metabolic pathway of Cr(VI) reduction by bacteria: a review. Microbiol Res 268:127288
Sahinkaya E, Kilic A, Calimlioglu B, Toker Y (2013) Simultaneous bioreduction of nitrate and chromate using sulfur-based mixotrophic denitrification process. J Hazard Mater 262:234–239
Sahinkaya E, Yurtsever A, Ucar D (2017) A novel elemental sulfur-based mixotrophic denitrifying membrane bioreactor for simultaneous Cr(VI) and nitrate reduction. J Hazard Mater 324:15–21
Shi J, Zhang B, Qiu R, Lai C, Jiang Y, He C, Guo J (2019) Microbial chromate reduction coupled to anaerobic oxidation of elemental sulfur or zerovalent iron. Environ Sci Technol 53:3198–3207
Torrentó C, Cama J, Urmeneta J, Otero N, Soler A (2010) Denitrification of groundwater with pyrite and Thiobacillus denitrificans. Chem Geol 278:80–91
Torrentó C, Urmeneta J, Otero N, Soler A, Viñas M, Cama J (2011) Enhanced denitrification in groundwater and sediments from a nitrate-contaminated aquifer after addition of pyrite. Chem Geol 287:90–101
Wang H-c, Liu Y, Yang Y-m, Fang Y-k, Luo S, Cheng H-y, Wang A-j (2022a) Element sulfur-based autotrophic denitrification constructed wetland as an efficient approach for nitrogen removal from low C/N wastewater. Water Res 226:119258
Wang Q, Zhao Y, Chen Z, Zhang C, Jia X, Zhao M, Tong Y, Liu Y (2023a) Nitrate bioreduction under Cr(VI) stress: crossroads of denitrification and dissimilatory nitrate reduction to ammonium. Environ Sci Technol 57:10662–10672
Wang Y, Yuan S, Shi J, Ma T, Xie X, Deng Y, Du Y, Gan Y, Guo Z, Dong Y, Zheng C, Jiang G (2023) Groundwater quality and health: making the invisible visible. Environ Sci Technol 57:5125–5136
Wilkin RT, Su C, Ford RG, Paul CJ (2005) Chromium removal processes during groundwater remediation by a zerovalent iron permeable reactive. Environ Sci Technol 39:4599–4605
Xu Z, Li Y, Zhou P, Song X, Wang Y (2022) New insights on simultaneous nitrate and phosphorus removal in pyrite-involved mixotrophic denitrification biofilter for a long-term operation: performance change and its underlying mechanism. Sci Total Environ 845:157403
Zhao Y, Wang Q, Yang Z, Jia X, Cabrera J, Ji M (2022) Bio-capture of Cr(VI) in a denitrification system: electron competition, long-term performance, and microbial community evolution. J Hazard Mater 432:128697
Zhao Y, Gao J, Zhou X, Li Z, Zhao C, Jia X, Ji M (2023) Bio-immobilization and recovery of chromium using a denitrifying biofilm system: identification of reaction zone, binding forms and end products. J Environ Sci 126:70–80
Zhou X, Zhai S, Zhao Y, Liu D, Wang Q, Ji M (2021) Rapid recovery of inhibited denitrification with cascade Cr(VI) exposure by bio-accelerant: characterization of chromium distributions, EPS compositions and denitrifying communities. J Hazard Mater 411:125087
Zhou Q, Jia L, Li Y, Wu W (2023) Strengthening in microbiota dynamics and C, N, S transformation induced by novel synthesized pyrite/PHBV composites for advanced nitrogen and phosphate removal: overlooked sulfate reduction process. Chem Eng J 463:142315
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This work was supported by Shanghai Agriculture Applied Technology and Development Program (2020–02-08–00-07-F01483), and Shanghai Sailing Program (20YF1400200).
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Haigeng Zhang: conceptualization, data curation, writing. Zhongshuo Xu: conceptualization, data curation, writing, supervision. Panpan Zhou: investigation. Yulei Zhang: writing-review and editing. Yuhui Wang: writing-review and editing.
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Zhang, H., Xu, Z., Zhou, P. et al. Simultaneous nitrate and chromium removal mechanism in a pyrite-involved mixotrophic biofilter. Environ Sci Pollut Res 30, 123882–123892 (2023). https://doi.org/10.1007/s11356-023-31070-x
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DOI: https://doi.org/10.1007/s11356-023-31070-x