Details
| Original language | English |
|---|---|
| Pages (from-to) | 2044-2053 |
| Number of pages | 10 |
| Journal | Environmental Science and Technology |
| Volume | 56 |
| Issue number | 3 |
| Publication status | Published - 11 Jan 2022 |
Abstract
Sorption of dissolved organic matter (DOM) is one major pathway in the formation of mineral-associated organic matter (MOM), but there is little information on how previous sorption events feedback to later ones by leaving their imprint on mineral surfaces and solutions (“legacy effect”). In order to conceptualize the role of legacy effects in MOM formation, we conducted sequential sorption experiments with kaolinite and gibbsite as minerals and DOM derived from forest floor materials. The MOM formation efficiency leveled off upon repeated addition of identical DOM solutions to minerals due to the retention of highly sorptive organic molecules (primarily aromatic, nitrogen-poor, hydrogen-poor, and oxygen-rich molecules), which decreased the sorption site availability and simultaneously modified the mineral surface charge. Organic–organic interactions as postulated in multilayer models played a negligible role in MOM formation. Continued exchange between DOM and MOM molecules upon repeated sorption altered the DOM composition but not the MOM formation efficiencies. Sorption-induced depletion of high-affinity compounds from solutions further decreased the MOM formation efficiencies to pristine minerals. Overall, the interplay between the differential sorptivities of DOM components and the mineral surface chemistry explains the legacy effects that contribute to the regulation of fluxes and the distribution of organic matter in the soil.
Keywords
- carbon sequestration, Fourier-transform ion cyclotron resonance mass spectrometry, legacy effects, mineral-associated organic matter, soil organic matter, sorption
ASJC Scopus subject areas
- Chemistry(all)
- General Chemistry
- Environmental Science(all)
- Environmental Chemistry
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In: Environmental Science and Technology, Vol. 56, No. 3, 11.01.2022, p. 2044-2053.
Research output: Contribution to journal › Article › Research › peer review
}
TY - JOUR
T1 - Legacy Effects of Sorption Determine the Formation Efficiency of Mineral-Associated Soil Organic Matter
AU - Chen, Shuling
AU - Klotzbücher, Thimo
AU - Lechtenfeld, Oliver J.
AU - Hong, Hanlie
AU - Liu, Chongxuan
AU - Kaiser, Klaus
AU - Mikutta, Christian
AU - Mikutta, Robert
N1 - Funding Information: This work was funded by the German Research Foundation (DFG, project “Formation and properties of mineral-organic soil interfaces as revealed by XPS,” MI 1377/13-1). Additional support was from the Program for Guangdong Introducing Innovative and Entrepreneurial Teams (2017ZT07Z479) and the Natural Science Foundation of China (nos. 41772032 and 42172045). We are grateful for the help of Anika Klotzbücher, Alexandra Boritzki, Christine Krenkewitz, and Gudrun von Koch during the laboratory work. We thank Jan Kaesler for the FT-ICR-MS measurements and Kai Franze for software development. The authors are grateful for using the analytical facilities of the Centre for Chemical Microscopy (ProVIS) at the Helmholtz Centre for Environmental Research, Leipzig, which is supported by the European Regional Development Funds (EFRE─Europe funds Saxony) and the Helmholtz Association.
PY - 2022/1/11
Y1 - 2022/1/11
N2 - Sorption of dissolved organic matter (DOM) is one major pathway in the formation of mineral-associated organic matter (MOM), but there is little information on how previous sorption events feedback to later ones by leaving their imprint on mineral surfaces and solutions (“legacy effect”). In order to conceptualize the role of legacy effects in MOM formation, we conducted sequential sorption experiments with kaolinite and gibbsite as minerals and DOM derived from forest floor materials. The MOM formation efficiency leveled off upon repeated addition of identical DOM solutions to minerals due to the retention of highly sorptive organic molecules (primarily aromatic, nitrogen-poor, hydrogen-poor, and oxygen-rich molecules), which decreased the sorption site availability and simultaneously modified the mineral surface charge. Organic–organic interactions as postulated in multilayer models played a negligible role in MOM formation. Continued exchange between DOM and MOM molecules upon repeated sorption altered the DOM composition but not the MOM formation efficiencies. Sorption-induced depletion of high-affinity compounds from solutions further decreased the MOM formation efficiencies to pristine minerals. Overall, the interplay between the differential sorptivities of DOM components and the mineral surface chemistry explains the legacy effects that contribute to the regulation of fluxes and the distribution of organic matter in the soil.
AB - Sorption of dissolved organic matter (DOM) is one major pathway in the formation of mineral-associated organic matter (MOM), but there is little information on how previous sorption events feedback to later ones by leaving their imprint on mineral surfaces and solutions (“legacy effect”). In order to conceptualize the role of legacy effects in MOM formation, we conducted sequential sorption experiments with kaolinite and gibbsite as minerals and DOM derived from forest floor materials. The MOM formation efficiency leveled off upon repeated addition of identical DOM solutions to minerals due to the retention of highly sorptive organic molecules (primarily aromatic, nitrogen-poor, hydrogen-poor, and oxygen-rich molecules), which decreased the sorption site availability and simultaneously modified the mineral surface charge. Organic–organic interactions as postulated in multilayer models played a negligible role in MOM formation. Continued exchange between DOM and MOM molecules upon repeated sorption altered the DOM composition but not the MOM formation efficiencies. Sorption-induced depletion of high-affinity compounds from solutions further decreased the MOM formation efficiencies to pristine minerals. Overall, the interplay between the differential sorptivities of DOM components and the mineral surface chemistry explains the legacy effects that contribute to the regulation of fluxes and the distribution of organic matter in the soil.
KW - carbon sequestration
KW - Fourier-transform ion cyclotron resonance mass spectrometry
KW - legacy effects
KW - mineral-associated organic matter
KW - soil organic matter
KW - sorption
UR - http://www.scopus.com/inward/record.url?scp=85123861034&partnerID=8YFLogxK
U2 - 10.1021/acs.est.1c06880
DO - 10.1021/acs.est.1c06880
M3 - Article
C2 - 35014800
AN - SCOPUS:85123861034
VL - 56
SP - 2044
EP - 2053
JO - Environmental Science and Technology
JF - Environmental Science and Technology
SN - 0013-936X
IS - 3
ER -