Evolution of humic substances in polymerization of polyphenol and amino acid based on non-destructive characterization

doi:10.1007/s11783-020-1297-y

Front. Environ. Sci. Eng.

2021, Vol. 15

Issue (1) : 5 https://doi.org/10.1007/s11783-020-1297-y

RESEARCH ARTICLE

Evolution of humic substances in polymerization of polyphenol and amino acid based on non-destructive characterization

Jianmei Zou^1,², Jianzhi Huang², Huichun Zhang², Dongbei Yue¹(

)

¹. School of Environment, Tsinghua University, Beijing 100084, China
². Department of Civil and Environmental Engineering, Case Western Reserve University, Cleveland, OH 44106, USA

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Abstract

• Humification evolution was identified with non-destructive characterization method.

• Humification process from precursors to fulvic and humic acid was confirmed.

• MnO₂ alone had limited oxidation ability to form HA.

• MnO₂ played a key role as a catalyst to transform FA to HA in the presence of O₂.

• MnO₂ could affect the structure of the humification products.

Abiotic humification is important in the formation and evolution of organic matter in soil and compost maturing processes. However, the roles of metal oxides in abiotic humification reactions under micro-aerobic remain ambiguous. The aim of this study was to use non-destructive measurement methods to investigate the role of MnO₂ in the evolution of humic substances (HSs) during oxidative polymerization of polyphenol-amino acid. Our results suggested a synergistic effect between MnO₂ and O₂ in promoting the polymerization reaction and identified that MnO₂ alone had a limited ability in accelerating the transformation of fulvic acid (FA) to humic acid (HA), whereas O₂ was the key factor in the process. Two-dimensional correlation spectroscopy (2D-COS) showed that the evolution in the UV-vis spectra followed the order of 475–525 nm>300–400 nm>240–280 nm in the humification process, indicating the formation of simple organic matter followed by FA and then HA. ¹³C nuclear magnetic resonance (¹³C NMR) analysis revealed that the products under both air and N₂ conditions in the presence of MnO₂ had greater amounts of aromatic-C than in the absence of MnO₂, demonstrating that MnO₂ affected the structure of the humification products. The results of this study provided new insights into the theory of abiotic humification.

Keywords Two-dimensional correlation spectroscopy (2D-COS) Humic substances (HSs) Humification Manganese dioxide Polyphenol

Corresponding Author(s): Dongbei Yue

Issue Date: 22 July 2020

Cite this article:

Jianmei Zou,Jianzhi Huang,Huichun Zhang, et al. Evolution of humic substances in polymerization of polyphenol and amino acid based on non-destructive characterization[J]. Front. Environ. Sci. Eng., 2021, 15(1): 5.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-020-1297-y
https://academic.hep.com.cn/fese/EN/Y2021/V15/I1/5

Fig.1 Time courses of pH in the catechin-glycine reaction systems (catechin 0.008 mol/L+ glycine 0.02 mol/L) in the presence of 2 g MnO₂ under ambient Air or N₂ conditions at 45℃ during a 90-h reaction period. Symbols and bars represent the mean values and standard deviations of duplicate measurements (some error bars are obscured by the symbols).

Fig.2 The catechin-glycine liquid UV–vis spectra in the 200–800 nm region in the four reaction systems: MnO₂(Air), MnO₂(N₂), Air, and N₂ at the reaction times of 3, 16, 26, 40, 60, and 90 h (the samples were all diluted 500 times).

Fig.3 Synchronous (S) and asynchronous (AS) 2D correlation maps generated from the UV-vis spectra of the reaction mixtures of catechin-glycine aliquots at 0, 3, 16, 26, 40, 60, and 90 h in the 200–800 nm region in the four reaction systems: MnO₂(Air) (a, e), MnO₂(N₂) (b, f), Air (c, g), and N₂ (d, h). Color changing from blue to red illustrates the change in the correlation intensity from negative to positive.

Tab.1 2D UV COS results on the assignment and sign of each cross-peak in the synchronous (Φ) and asynchronous (Ψ, in parentheses) maps for the reaction system of MnO₂ (Air)

Fig.4 (a) Effect of MnO₂ in the catechin-glycine reaction systems on the transformation of FA to HA under the air or N₂ atmosphere at 45℃ during the 90-h reaction period. (b) The concentration of humic acid and fulvic acid isolated from the four reaction systems at 90 h. The [HA]/[FA] ratios were calculated based on the obtained DOC concentrations in the samples. The data points are given as means with standard deviations.

Fig.5 ¹³C cross-polarization magic angle spinning nuclear magnetic resonance (CPMAS-NMR) spectra of humic acids (a) and fulvic acids (b) isolated from four catechin-glycine (catechin 0.008 mol/L, glycine 0.02 mol/L) reaction systems in the presence of 2 g MnO₂ under ambient O₂ or N₂ conditions at 45℃ at 90 h

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