Water chemistry alteration induced strength weakening of natural sediment, which leads to the differential settlement of infrastructures in coastal areas, has caused numerous disasters and engineering failures. To thoroughly understand the underlying mechanisms of how water chemistry influences the microfabric and mechanical properties evolution of coastal sediments, herein, the authors adopted centrifuge test, X-ray diffraction (XRD), and atomic force microscope (AFM) to quantitatively study the structure anisotropy index (i.e., orientation index (OI)), micromorphological property (i.e., root mean square height (Sq)), and micromechanics (i.e., microscale apparent modulus) of clay sediments in different water chemistry conditions and gravity gradients. The results show that the change rule of OI is: OIsaline > OIalkaline > OIwater > OIacid, along the vertical sedimentary depth. Randomly distributed clay flocs and loose flocculated soil skeleton (mainly consisted by edge-to-face (EF) and edge-to-edge (EE) contact of the kaolinite platelets) are associated with the acidic water chemical conditions. The action of supergravity and face-to-face (FF) repulsive contact mode lead to high degree of anisotropy of kaolinite sediments in alkaline environment. Clay platelets are compacted closely under the synergetic effect of centrifugal pressure and prevailing van der Waals attraction (reduction of electric double layer repulsion) in saline environment. The change of 1/Sq is highly consistent with the change of OI at different depths in different water chemical environments. Along the sedimentary depth (i.e., transition from the normal gravity (1 g) to supergravity (8000 g)), the microscale apparent modulus of kaolinite sediment was found to be the highest in alkaline environment. As the water chemistry changes from alkaline to acidic, however, the microscale apparent modulus of kaolinite aggregate decreased, and it showed the smallest in the saline environment.
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