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Machine Learning Assisted Classification of Ca-Organic Matter Complexation Using X-ray Spectroscopies


EMSL Project ID
60173

Abstract

Soils and sediments host large stores of organic carbon, which can be released to the atmosphere upon mineralization. Ca has the potential to play a key role in preventing mineralization of
this organic carbon by enhancing mineral protection, as it has long been recognized that Ca forms cation bridges that link together negatively charged functional groups from organics and mineral surfaces. Ca bridging is thought to underlie the relationship between exchangeable Ca, increased soil organic matter (OM) content, and decreased OM mineralization. However, there is little experimental insight into the molecular-scale mechanisms and under what conditions they occur. This is in part due to the complexity of organic matter, which is a macromolecular assembly containing numerous functional groups capable of binding metals. Molecular insight into Ca-OM binding is essential to provide predictive knowledge on the conditions under which Ca stabilizes organic matter within sediments. Here, we propose to shed light on Ca binding in sediments and the role that it plays in OM sequestration by utilizing recently developed machine learning (ML) tools combined with X-ray spectroscopies. Specifically, we will use this approach to identify sensitive spectral fingerprints that can be used to distinguish which OM functional groups participate in Ca bridging. The structural and electronic structure information gained will be used to develop a comprehensive chemical and structural classification of Ca-organic matter complexation. We believe that this state-of-the-art approach can be used to aid the elucidation of the following hypotheses: a) Ca forms inner-sphere complexes with OM functional groups; and b) Ca is bound predominantly by carboxylate and catechol functional groups. Computational and experimental capabilities at EMSL and SSRL will be used to achieve this goal.

Project Details

Project type
Exploratory Research
Start Date
2021-12-01
End Date
2023-01-31
Status
Closed

Team

Principal Investigator

Niranjan Govind
Institution
Pacific Northwest National Laboratory

Co-Investigator(s)

Sharon Bone
Institution
Stanford Linear Accelerator Center

Team Members

Elisa Biasin
Institution
Pacific Northwest National Laboratory

Michael Sachs
Institution
Stanford Linear Accelerator Center

Jolina Alonzo
Institution
Pacific Northwest National Laboratory

Zhaoyuan Yang
Institution
University of Washington

Yeonsig Nam
Institution
University of California, Irvine

Soumen Ghosh
Institution
Indian Institute of Technology Indore

Gerald Seidler
Institution
University of Washington

Richard Cox
Institution
Pacific Northwest National Laboratory

Caroline Loe
Institution
University of Washington

Samantha Tetef
Institution
University of Washington

Benjamin Poulter
Institution
University of Washington