Chemical Force Spectroscopy Evidence Supporting the Layer-by-Layer Model of Organic Matter Binding to Iron (oxy)Hydroxide Mineral Surfaces

Alexander W. Chassé; Tsutomu Ohno; Steven R. Higgins; Aria Amirbahman; Nadir Yildirim; Thomas B. Parr

doi:10.1021/acs.est.5b01877

Chemical Force Spectroscopy Evidence Supporting the Layer-by-Layer Model of Organic Matter Binding to Iron (oxy)Hydroxide Mineral Surfaces

Alexander W. Chassé, Tsutomu Ohno, Steven R. Higgins, Aria Amirbahman, Nadir Yildirim, Thomas B. Parr

Research output: Contribution to journal › Article › peer-review

71 Scopus citations

Abstract

© 2015 American Chemical Society. The adsorption of dissolved organic matter (DOM) to metal (oxy)hydroxide mineral surfaces is a critical step for C sequestration in soils. Although equilibrium studies have described some of the factors controlling this process, the molecular-scale description of the adsorption process has been more limited. Chemical force spectroscopy revealed differing adhesion strengths of DOM extracted from three soils and a reference peat soil material to an iron (oxy)hydroxide mineral surface. The DOM was characterized using ultrahigh-resolution negative ion mode electrospray ionization Fourier Transform ion cyclotron resonance mass spectrometry. The results indicate that carboxyl-rich aromatic and N-containing aliphatic molecules of DOM are correlated with high adhesion forces. Increasing molecular mass was shown to decrease the adhesion force between the mineral surface and the DOM. Kendrick mass defect analysis suggests that mechanisms involving two carboxyl groups result in the most stable bond to the mineral surface. We conceptualize these results using a layer-by-layer "onion" model of organic matter stabilization on soil mineral surfaces.

Original language	English (US)
Pages (from-to)	9733-9741
Number of pages	9
Journal	Environmental Science & Technology
Volume	49
Issue number	16
DOIs	https://doi.org/10.1021/acs.est.5b01877
State	Published - Aug 7 2015
Externally published	Yes

Bibliographical note

KAUST Repository Item: Exported on 2020-10-01
Acknowledgements: A.W.C. and T.O. extend our appreciation to Dr. Leonardo Gutierrez at the University of Illinois at Urbana–Champaign and Dr. Jean Philippe Croue at the King Abdullah University of Science and Technology for discussion and assistance with the preparation of the iron (oxy)hydroxide coated AFM probes. This project was supported by USDA-NIFA-AFRI 2013-67019-21368 and the Maine Agricultural and Forest Experiment Station Hatch Project ME0-H-1-00472-11. This is Maine Agricultural and Forest Experiment Station Journal no. 3432.
This publication acknowledges KAUST support, but has no KAUST affiliated authors.

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title = "Chemical Force Spectroscopy Evidence Supporting the Layer-by-Layer Model of Organic Matter Binding to Iron (oxy)Hydroxide Mineral Surfaces",

abstract = "{\textcopyright} 2015 American Chemical Society. The adsorption of dissolved organic matter (DOM) to metal (oxy)hydroxide mineral surfaces is a critical step for C sequestration in soils. Although equilibrium studies have described some of the factors controlling this process, the molecular-scale description of the adsorption process has been more limited. Chemical force spectroscopy revealed differing adhesion strengths of DOM extracted from three soils and a reference peat soil material to an iron (oxy)hydroxide mineral surface. The DOM was characterized using ultrahigh-resolution negative ion mode electrospray ionization Fourier Transform ion cyclotron resonance mass spectrometry. The results indicate that carboxyl-rich aromatic and N-containing aliphatic molecules of DOM are correlated with high adhesion forces. Increasing molecular mass was shown to decrease the adhesion force between the mineral surface and the DOM. Kendrick mass defect analysis suggests that mechanisms involving two carboxyl groups result in the most stable bond to the mineral surface. We conceptualize these results using a layer-by-layer {"}onion{"} model of organic matter stabilization on soil mineral surfaces.",

author = "Chass{\'e}, {Alexander W.} and Tsutomu Ohno and Higgins, {Steven R.} and Aria Amirbahman and Nadir Yildirim and Parr, {Thomas B.}",

note = "KAUST Repository Item: Exported on 2020-10-01 Acknowledgements: A.W.C. and T.O. extend our appreciation to Dr. Leonardo Gutierrez at the University of Illinois at Urbana–Champaign and Dr. Jean Philippe Croue at the King Abdullah University of Science and Technology for discussion and assistance with the preparation of the iron (oxy)hydroxide coated AFM probes. This project was supported by USDA-NIFA-AFRI 2013-67019-21368 and the Maine Agricultural and Forest Experiment Station Hatch Project ME0-H-1-00472-11. This is Maine Agricultural and Forest Experiment Station Journal no. 3432. This publication acknowledges KAUST support, but has no KAUST affiliated authors.",

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T1 - Chemical Force Spectroscopy Evidence Supporting the Layer-by-Layer Model of Organic Matter Binding to Iron (oxy)Hydroxide Mineral Surfaces

AU - Chassé, Alexander W.

AU - Ohno, Tsutomu

AU - Higgins, Steven R.

AU - Amirbahman, Aria

AU - Yildirim, Nadir

AU - Parr, Thomas B.

N1 - KAUST Repository Item: Exported on 2020-10-01 Acknowledgements: A.W.C. and T.O. extend our appreciation to Dr. Leonardo Gutierrez at the University of Illinois at Urbana–Champaign and Dr. Jean Philippe Croue at the King Abdullah University of Science and Technology for discussion and assistance with the preparation of the iron (oxy)hydroxide coated AFM probes. This project was supported by USDA-NIFA-AFRI 2013-67019-21368 and the Maine Agricultural and Forest Experiment Station Hatch Project ME0-H-1-00472-11. This is Maine Agricultural and Forest Experiment Station Journal no. 3432. This publication acknowledges KAUST support, but has no KAUST affiliated authors.

PY - 2015/8/7

Y1 - 2015/8/7

N2 - © 2015 American Chemical Society. The adsorption of dissolved organic matter (DOM) to metal (oxy)hydroxide mineral surfaces is a critical step for C sequestration in soils. Although equilibrium studies have described some of the factors controlling this process, the molecular-scale description of the adsorption process has been more limited. Chemical force spectroscopy revealed differing adhesion strengths of DOM extracted from three soils and a reference peat soil material to an iron (oxy)hydroxide mineral surface. The DOM was characterized using ultrahigh-resolution negative ion mode electrospray ionization Fourier Transform ion cyclotron resonance mass spectrometry. The results indicate that carboxyl-rich aromatic and N-containing aliphatic molecules of DOM are correlated with high adhesion forces. Increasing molecular mass was shown to decrease the adhesion force between the mineral surface and the DOM. Kendrick mass defect analysis suggests that mechanisms involving two carboxyl groups result in the most stable bond to the mineral surface. We conceptualize these results using a layer-by-layer "onion" model of organic matter stabilization on soil mineral surfaces.

AB - © 2015 American Chemical Society. The adsorption of dissolved organic matter (DOM) to metal (oxy)hydroxide mineral surfaces is a critical step for C sequestration in soils. Although equilibrium studies have described some of the factors controlling this process, the molecular-scale description of the adsorption process has been more limited. Chemical force spectroscopy revealed differing adhesion strengths of DOM extracted from three soils and a reference peat soil material to an iron (oxy)hydroxide mineral surface. The DOM was characterized using ultrahigh-resolution negative ion mode electrospray ionization Fourier Transform ion cyclotron resonance mass spectrometry. The results indicate that carboxyl-rich aromatic and N-containing aliphatic molecules of DOM are correlated with high adhesion forces. Increasing molecular mass was shown to decrease the adhesion force between the mineral surface and the DOM. Kendrick mass defect analysis suggests that mechanisms involving two carboxyl groups result in the most stable bond to the mineral surface. We conceptualize these results using a layer-by-layer "onion" model of organic matter stabilization on soil mineral surfaces.

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Chemical Force Spectroscopy Evidence Supporting the Layer-by-Layer Model of Organic Matter Binding to Iron (oxy)Hydroxide Mineral Surfaces

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