Molecular heterogeneity in pyrogenic dissolved organic matter from a thermal series of oak and grass chars

被引:39
作者
Wozniak, Andrew S. [1 ]
Goranov, Aleksandar, I [2 ]
Mitra, Siddhartha [3 ]
Bostick, Kyle W. [4 ]
Zimmerman, Andrew R. [4 ]
Schlesinger, Danielle R. [5 ]
Myneni, Satish [5 ]
Hatcher, Patrick G. [2 ]
机构
[1] Univ Delaware, Sch Marine Sci & Policy, 1044 Coll Dr, Lewes, DE 19958 USA
[2] Old Dominion Univ, Dept Chem & Biochem, Norfolk, VA USA
[3] East Carolina Univ, Dept Geol Sci, Greenville, NC USA
[4] Univ Florida, Dept Geol Sci, Gainesville, FL USA
[5] Princeton Univ, Dept Geosci, Princeton, NJ USA
基金
美国国家科学基金会;
关键词
Black carbon; Pyrogenic organic matter; Biochar; FTICR-MS; H-1; NMR; Dissolved organic matter (DOM); STATE C-13 NMR; BLACK CARBON; BIOCHAR; MASS; PYROLYSIS; BIOMASS; LIGNIN; SOIL; DEGRADATION; CHARCOAL;
D O I
10.1016/j.orggeochem.2020.104065
中图分类号
P3 [地球物理学]; P59 [地球化学];
学科分类号
0708 ; 070902 ;
摘要
Pyrogenic organic matter (Py-OM), generated via the incomplete combustion of biomass, is well studied due to the presence of slow-cycling, condensed aromatic compounds (ConAC) known to sequester in soils and sediments. Recently, dissolved Py-OM (Py-DOM) has received interest, due to its higher mobility and potential to be transferred through watersheds to aquatic systems. Py-DOM quantities, molecular identities and importance to global carbon budgets and cycles are only beginning to be understood. Fourier transform ion cyclotron resonance mass spectrometry (FTICR-MS) analyses were performed on PyDOM isolated from oak and grass biochars produced over a range of temperatures (250-650 degrees C), and the data are compared to complementary H-1 NMR spectroscopic and benzenepolycarboxylic acid biomarker (BPCAs) analyses. Py-DOM is revealed to be a heterogeneous mixture of compounds ranging in relative aromaticity and oxygenation. FTICR-MS analyses demonstrate a decrease in Py-DOM relative oxygen content and a concurrent increase in aliphatic character and heteroatomic (N, Cl) content. H-1 NMR and BPCAs analyses detail low O/C dissolved ConAC not observed by FTICR-MS, demonstrating the necessity for a multiple proxy approach to Py-DOM characterization. Heterogeneous Py-DOM is explained as resulting from pyrolysis-initiated and radical-mediated functional group cleavage, aromatic condensation and aromatic ring-opening reactions. Oak biomass progresses faster along a char maturity continuum for a given pyrolysis temperature, perhaps due to its greater lignin content or radical quenching by grass cuticular material. Biomass species and pyrolysis temperature likely result in different PyDOM compositions and fates and must be considered when evaluating the impacts of wildfires and biochar applications. (C) 2020 Elsevier Ltd. All rights reserved.
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页数:18
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共 76 条
  • [1] Pyrogenic carbon soluble fraction is larger and more aromatic in aged charcoal than in fresh charcoal
    Abiven, Samuel
    Hengartner, Pascal
    Schneider, Maximilian P. W.
    Singh, Nimisha
    Schmidt, Michael W. I.
    [J]. SOIL BIOLOGY & BIOCHEMISTRY, 2011, 43 (07) : 1615 - 1617
  • [2] Aerosols as a source of dissolved black carbon to the ocean
    Bao, Hongyan
    Niggemann, Jutta
    Luo, Li
    Dittmar, Thorsten
    Kao, Shuh-Ji
    [J]. NATURE COMMUNICATIONS, 2017, 8
  • [3] CONTROLLING THE FALSE DISCOVERY RATE - A PRACTICAL AND POWERFUL APPROACH TO MULTIPLE TESTING
    BENJAMINI, Y
    HOCHBERG, Y
    [J]. JOURNAL OF THE ROYAL STATISTICAL SOCIETY SERIES B-STATISTICAL METHODOLOGY, 1995, 57 (01) : 289 - 300
  • [4] Bianchi TS, 2011, CHEMICAL BIOMARKERS IN AQUATIC ECOSYSTEMS, P1
  • [5] Release of chlorine from biomass at pyrolysis and gasification conditions
    Bjorkman, E
    Stromberg, B
    [J]. ENERGY & FUELS, 1997, 11 (05) : 1026 - 1032
  • [6] Bostick K.W., 2018, FRONT EARTH SC-SWITZ, V6, P1
  • [7] The effect of the biomass components lignin, cellulose and hemicellulose on TGA and fixed bed pyrolysis
    Burhenne, Luisa
    Messmer, Jonas
    Aicher, Thomas
    Laborie, Marie-Pierre
    [J]. JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS, 2013, 101 : 177 - 184
  • [8] Selected dark sides of biomass-derived biochars as environmental amendments
    Chen, Zien
    Luo, Lei
    Xiao, Diyi
    Lv, Jitao
    Wen, Bei
    Ma, Yibing
    Zhang, Shuzhen
    [J]. JOURNAL OF ENVIRONMENTAL SCIENCES, 2017, 54 : 13 - 20
  • [9] Aged black carbon in marine sediments and sinking particles
    Coppola, Alysha I.
    Ziolkowski, Lori A.
    Masiello, Caroline A.
    Druffel, Ellen R. M.
    [J]. GEOPHYSICAL RESEARCH LETTERS, 2014, 41 (07) : 2427 - 2433
  • [10] Effects of charring on mass, organic carbon, and stable carbon isotope composition of wood
    Czimczik, CI
    Preston, CM
    Schmidt, MWI
    Werner, RA
    Schulze, ED
    [J]. ORGANIC GEOCHEMISTRY, 2002, 33 (11) : 1207 - 1223