Effects of oxidizing environment on digestate humification and identification of substances governing the dissolved organic matter (DOM) transformation process

Highlights

• Liquid digestate humification was investigated under different oxidizing environment.

• Tryptophan-like substances dominated the transformation of the liquid digestate DOM.

• The humification sequence of the liquid digestate DOM was identified.

• UV₃₂₅ was first identified as a pre-humus intermediate during humification reaction.

Abstract

The formation of humic-like acids (HLAs) is an essential process for converting liquid digestate into organic soil amendments to enhance agricultural sustainability. The aim of this study was to investigate the impact of oxygen and/or MnO₂ on the production of HLAs. Herein, abiotic humification performance of the digestate dissolved organic matter (DOM) is investigated with fluxes of air and N₂ in the absence and presence of MnO₂. Our results demonstrated that the fate of digestate DOM greatly depends on the oxidizing environment, the MnO₂ enhanced nitrogen involved in the formation of HLAs. The synergistic effects of MnO₂ and oxygen effectively improved the production of HLAs, and the corresponding component evolution was analyzed using spectroscopic evidence. The two-dimensional correlation spectroscopy results demonstrated that the reaction sequence of digestate DOM followed the order of protein-like substances, substances with an absorbance at 325 nm, substances with UV absorbance at 254 nm and HLAs. Additionally, excitation emission matrix fluorescence combined with parallel factor analysis (EEM-PARAFAC) showed that tryptophan-like C3 was more prone to transformation than tyrosine-like C2 and was responsible for the humification process. The substance with an absorbance at 325 nm was a reaction intermediate in the transformation process of protein-like substances to HLAs. The above findings can be used to promote the production of liquid fertilizer associated with carbon sequestration as well as the sustainable development of biogas production.

Graphical abstract

Keywords

Liquid digestate / MnO₂ / Oxygen / DOM transformation / Humic-like acids

References

[1] Akhiar A, Battimelli A, Torrijos M, Carrere H (2017). Comprehensive characterization of the liquid fraction of digestates from full-scale anaerobic co-digestion. Waste Management (New York, N.Y.), 59: 118–128

[2] Amir S, Jouraiphy A, Abdelilah M, Gharous M E, Hafidi M (2010). Structural study of humic acids during composting of activated sludge-green waste: Elemental analysis, FTIR and ¹³C NMR. Journal of Hazardous Materials, 177(1–3): 524–529 doi:10.1016/j.jhazmat.2009.12.064 PMID:20106591

[3] Bankston E, Wang Q, Higgins B (2020). Algae support populations of heterotrophic, nitrifying, and phosphate-accumulating bacteria in the treatment of poultry litter anaerobic digestate. Chemical Engineering Journal, 398: 125550

[4] Berto S, Laurentiis E D, Scapuzzi C, Chiavazza E, Corazzari I, Turci F, Minella M, Buscaino R, Daniele P, Vione D (2018). Phototransformation of l-tryptophan and formation of humic substances in water. Environmental Chemistry Letters, 16(3): 1035–1041

[5] Bodappa N, Stepan S, Smith R D L (2021). Analysis of solid-state reaction mechanisms with two-dimensional fourier transform infrared correlation spectroscopy. Inorganic Chemistry, 60(4): 2304–2314

[6] Campitelli P, Ceppi S (2008). Effects of composting technologies on the chemical and physicochemical properties of humic acids. Geoderma, 144(1–2): 325–333

[7] Chen H, Li Q, Wang M, Ji D, Tan W (2020). XPS and two-dimensional FTIR correlation analysis on the binding characteristics of humic acid onto kaolinite surface. Science of the Total Environment, 724(5): 138154

[8] Chen W, Teng C Y, Qian C, Yu H Q (2019). Characterizing properties and environmental behaviors of dissolved organic matter using two-dimensional correlation spectroscopic analysis. Environmental Science & Technology, 53(9): 4683–4694

[9] Chen W, Westerhoff P, Leenheer J A, Booksh K (2003). Fluorescence excitation-emission matrix regional integration to quantify spectra for dissolved organic matter. Environmental Science & Technology, 37(24): 5701–5710

[10] Chien S W C, Chen H L, Wang M C, Seshaiah K (2009). Oxidative degradation and associated mineralization of catechol, hydroquinone and resorcinol catalyzed by birnessite. Chemosphere, 74(8): 1125–1133

[11] Claudio Z, César P, Claudio C, Miano T M, William S (2018). Advances in the determination of humification degree in peat since achard (1786): applications in geochemical and paleoenvironmental studies. Earth-Science Reviews, 185: 163–178 doi:10.1016/j.earscirev.2018.05.017

[12] Ding Y, Teppen B J, Boyd S A, Li H (2013). Measurement of associations of pharmaceuticals with dissolved humic substances using solid phase extraction. Chemosphere, 91(3): 314–319

[13] Gan D, Kotob S, Walia S (2007). Evaluation of a spectrophotometric method for practical and cost effective quantification of fulvic acid. Animal Science Journal, 1: 11–15

[14] Grigatti M, Barbanti L, Hassan M U, Ciavatta C (2020). Fertilizing potential and CO₂ emissions following the utilization of fresh and composted food-waste anaerobic digestates. Science of the Total Environment, 698: 134198

[15] Joodaki F, Martin L M, Greenfield M L (2019). Planarity and out-of-plane vibrational modes of tryptophan and tyrosine in biomolecular modeling. Physical Chemistry Chemical Physics, 21(43): 23943–23965

[16] Kanno H, Tachibana N, Fukushima M (2011). Optimization of conditions for thermal treatment of rice bran using an accelerator including an organo-iron compound. Bioresource Technology, 102(3): 3430–3436

[17] Kieber R J, Willey J D, Whitehead R F, Reid S N (2007). Photobleaching of chromophoric dissolved organic matter (CDOM) in rainwater. Journal of Atmospheric Chemistry, 58(3): 219–235

[18] Lee Y K, Murphy K R, Hur J (2020). Fluorescence signatures of dissolved organic matter leached from microplastics: polymers and additives. Environmental Science & Technology, 54(19): 11905–11914

[19] Li G, Bai X, Li H, Lu Z T, Zhang Z G (2019). Nutrients removal and biomass production from anaerobic digested effluent by microalgae: A review. International Journal of Agricultural and Biological Engineering, 12(5): 8–13

[20] Li G, Zhang J, Li H, Hu R C, Yao X L, Liu Y, Zhou Y G, Lyu T (2021). Towards high-quality biodiesel production from microalgae using original and anaerobically-digested livestock wastewater. Chemosphere, 273: 128578

[21] Liu X, Wang Y, Wang W, Huang W, Yu Z, Zhou S (2021). Protein-derived structures determines the redox capacity of humic acids formed during hyperthermophilic composting. Waste Management (New York, N.Y.), 126: 810–820

[22] Miadenov N, Yan Z, Simone B, Bilinski T M, McKnight D M, Nemergut D, Radloff K A, Rahman M M, Ahmed K M (2015). Dissolved organic matter quality in a shallow aquifer of bangladesh: implications for arsenic mobility. Environmental Science & Technology, 49(18): 10815–10824

[23] Miranda G A P, Júnior J T A, Brocchi E D A, Wang H (2021). Humic substances reduce the erodibility of soils in mining areas. Journal of Cleaner Production, 279(5): 123700

[24] Mohinuzzaman M, Yuan J, Yang X, Senesi N, Li S L, Ellam R M, Mostofa K M G, Liu C Q (2020). Insights into solubility of soil humic substances and their fluorescence characterisation in three characteristic soils. Science of the Total Environment, 720: 137395

[25] Monlau F, Sambusiti C, Ficara E, Aboulkas A, Barakat A, Carrère H (2015). New opportunities for agricultural digestate valorization: current situation and perspectives. Energy & Environmental Science, 8(9): 2600–2621

[26] Noda I, Dowrey A E, Marcott C (1990). Two-dimensional infrared (2D IR) spectroscopy: Theory and applications. Applied Spectroscopy, 44(4): 550–561

[27] Palma D, Parlanti E, Sourzac M, Voldoire O, Beauger A, Sleiman M, Richard C (2021). Fluorescence analysis allows to predict the oxidative capacity of humic quinones in dissolved organic matter: implication for pollutant degradation. Environmental Chemistry Letters, 19(2): 1857–1863

[28] Pasalari H, Esrafili A, Rezaee A, Gholami M, Farzadkia M (2021). Electrochemical oxidation pretreatment for enhanced methane potential from landfill leachate in anaerobic co-digestion process: Performance, gompertz model, and energy assessment. Chemical Engineering Journal, 422: 130046

[29] Pérez M G, Martin-Neto L, Saab S C, Novotny E H, Milori D M B P, Bagnato V S, Colnago L A, Melo W J, Knicker H (2004). Characterization of humic acids from a brazilian oxisol under different tillage systems by EPR, ¹³C NMR, FTIR and fluorescence spectroscopy. Geoderma, 118(3–4): 181–190

[30] Qi H, Zhang A, Du Z, Wu J, Ye M (2021). δ-MnO₂ changed the structure of humic-like acid during co-composting of chicken manure and rice straw. Waste Management (New York, N.Y.), 128: 16–24

[31] Ren X, Wang Q, Li R, Chang C C, Pan J, Zhang Z (2020). Effect of clay on greenhouse gas emissions and humification during pig manure composting as supported by spectroscopic evidence. Science of the Total Environment, 737: 139712

[32] Romero E, Plaza C, Senesi N, Nogales R, Polo A (2007). Humic acid-like fractions in raw and vermicomposted winery and distillery wastes. Geoderma, 139(3–4): 397–406

[33] Seaux L, Van Houcke S, Dumoulin E, Fiers T, Lecocq E, Delanghe J R (2014). Dual-wavelength recording, a simple algorithm to eliminate interferences due to UV-absorbing substances in capillary electrophoresis. Electrophoresis, 35(16): 2248–2252

[34] Shindo H, Huang P (1982). Role of Mn (IV) oxide in abiotic formation of humic substances in the environment. Nature, 298(5872): 363–365

[35] Slepetiene A, Volungevicius J, Jurgutis L, Liaudanskiene I, Amaleviciute-Volunge K, Slepetys J, Ceseviciene J (2020). The potential of digestate as a biofertilizer in eroded soils of Lithuania. Waste Management (New York, N.Y.), 102: 441–451

[36] Souza S O, Silva M D M, Santos J C C, Oliveira L D, Carmo J D, Botero W G (2016). Evaluation of different fractions of the organic matter of peat on tetracycline retention in environmental conditions: in vitro studies. Journal of Soils and Sediments, 16(6): 1764–1775

[37] Stevenson F J (1983). Humus chemistry: Genesis, composition, reactions. Soil Science, 135(2): 129–130

[38] Ukalska-Jaruga A, Smreczak B (2020). The impact of organic matter on polycyclic aromatic hydrocarbon (PAH) availability and persistence in soils. Molecules, 25(11): 2470

[39] Valentinuzzi F, Cavani L, Porfido C, Terzano R, Pii Y, Cesco S, Marzadori C, Mimmo T (2020). The fertilising potential of manure-based biogas fermentation residues: Pelleted vs. liquid digestate. Heliyon, 6(2): e03325

[40] Wang R G, Wang T C, Qu G Z, Zhang Y, Guo X T, Jia H Z, Zhu L Y (2021). Insights into the underlying mechanisms for integrated inactivation of A. spiroides and depression of disinfection byproducts by plasma oxidation. Water Research, 196: 117027

[41] Wang X Q, Muhmood A, Dong R J, Wu S B (2020). Synthesis of humic-like acid from biomass pretreatment liquor: quantitative appraisal of electron transferring capacity and metal-binding potential. Journal of Cleaner Production, 255: 120243

[42] Wei M J, Gao C, Zhou Y J, Duan P F, Li M (2019). Variation in spectral characteristics of dissolved organic matter in inland rivers in various trophic states, and their relationship with phytoplankton. Ecological Indicators, 104: 321–332

[43] Xia A, Murphy J D (2016). Microalgal cultivation in treating liquid digestate from biogas systems. Trends in Biotechnology, 34(4): 264–275

[44] Yang C M, Sun J L, Chen Y Y, Wu J, Wang Y L (2020). Linkage between water soluble organic matter and bacterial community in sediment from a shallow, eutrophic lake, Lake Chaohu, China. Journal of Environmental Sciences-China, 98: 39–46

[45] Yang F, Antonietti M (2020). The sleeping giant: A polymer view on humic matter in synthesis and applications. Progress in Polymer Science, 100: 101182

[46] Yang X F, Zheng X, Wu L, Cao X, Li Y, Niu J, Meng F (2018). Interactions between algal (AOM) and natural organic matter (NOM): Impacts on their photodegradation in surface waters. Environmental Pollution, 242(Pt B): 1185–1197

[47] Zhang J, Lv B Y, Xing M Y, Yang J (2015a). Tracking the composition and transformation of humic and fulvic acids during vermicomposting of sewage sludge by elemental analysis and fluorescence excitation-emission matrix. Waste Management (New York, N.Y.), 39: 111–118

[48] Zhang W, Dai X H, Dong B, Dai L L (2020a). New insights into the effect of sludge proteins on the hydrophilic/hydrophobic properties that improve sludge dewaterability during anaerobic digestion. Water Research, 173: 115503

[49] Zhang Y C, Yue D B, Fang D, Dong X W, Li W L (2020b). Enhanced darkening effect from the interaction of MnO₂ and oxygen on the component evolution of amino-phenolic humic-like substances. Chemosphere, 263: 127956

[50] Zhang Y C, Yue D B, Ma H (2015b). Darkening mechanism and kinetics of humification process in catechol-Maillard system. Chemosphere, 130: 40–45

[51] Zhou L, Zhou Y, Hu Y, Cai J, Liu X, Bai C, Tang X, Zhang Y, Jang K S, Spencer R G M, Jeppesen E (2019). Microbial production and consumption of dissolved organic matter in glacial ecosystems on the Tibetan Plateau. Water Research, 160: 18–28

[52] Zhou Y, Yao X, Zhang Y, Shi K, Zhang Y, Jeppesen E, Gao G, Zhu G, Qin B (2017). Potential rainfall-intensity and pH-driven shifts in the apparent fluorescent composition of dissolved organic matter in rainwater. Environmental Pollution, 224: 638–648

[53] Zilio M, Orzi V, Chiodini M E, Riva C, Acutis M, Boccasile G, Adani F (2020). Evaluation of ammonia and odour emissions from animal slurry and digestate storage in the Po Valley (Italy). Waste Management (New York, N.Y.), 103: 296–304

[54] Zou J M, Huang J Z, Zhang H C, Yue D B (2021). Evolution of humic substances in polymerization of polyphenol and amino acid based on non-destructive characterization. Frontiers of Environmental Science & Engineering, 15(1): 5

Acknowledgements

The authors are grateful for the financial support from the National Key Technology Research and Development Programs, China (No. 2018YFC1901405), the National Natural Science Foundation of China (Grant No. 52100167), the Natural Science Foundation of Hebei Province, China (No. B2020203024), the Key Research and Development Plan of Hebei Province, China (No. 21327312D), the Young and Middle-Aged Science and Technology Innovation Leadership Talents Project of Xinjiang Production and Construction Corps, China (No. 2019CB028) and the Science and Technology Public Relations Projects in Key Fields of Xinjiang Production and Construction Corps, China (No. 2019AB028).

Electronic Supplementary Material

Supplementary material is available in the online version of this article at https://doi.org/10.1007/s11783-022-1520-0 and is accessible for authorized users.

RIGHTS & PERMISSIONS

2022 Higher Education Press