A set-up for simultaneous measurement of second harmonic generation and streaming potential and some test applications.
We present a measurement cell that allows simultaneous measurement of second harmonic generation (SHG) and streaming potential (SP) at mineral-water interfaces with flat specimen that are suitable for non-linear optical (NLO) studies. The set-up directly yields SHG data for the interface of interest and can also be used to obtain information concerning the influence of flow on NLO signals from that interface. The streaming potential is at present measured against a reference substrate (PTFE). The properties of this inert reference can be independently determined for the same conditions. With the new cell, for the first time the SHG signal and the SP for flat surfaces have been simultaneousl…
Modeling plutonium sorption to kaolinite: Accounting for redox equilibria and the stability of surface species
Abstract Plutonium with its particularly complex redox chemistry may be thermodynamically stable in the states + III to + VI depending on the redox conditions in the environment. Mineral surfaces can also affect Pu redox speciation. Therefore, the interpretation of Pu sorption data becomes particularly challenging, even for simplified laboratory experiments. The present study focuses on Pu sorption to kaolinite. Am(III), Th(IV), Np(V) and U(VI) literature sorption data are used as analogues for the corresponding Pu redox states to calibrate a simple surface complexation model, and the Nernst formalism is applied. Two independent pH–pe diagrams, one for the kaolinite surface and another for …
Atypical titration curves for GaAl12Keggin-ions explained by a joint experimental and simulation approach
Although they have been widely used as models for oxide surfaces, the deprotonation behaviors of the Keggin-ions (MeAl127+) and typical oxide surfaces are very different. On Keggin-ions, the deprotonation occurs over a very narrow pH range at odds with the broad charging curve of larger oxide surfaces. Depending on the Me concentration, the deprotonation curve levels off sooner (high Me concentration) or later (for low Me concentration). The leveling off shows the onset of aggregation before which the Keggin-ions are present as individual units. We show that the atypical titration data previously observed for some GaAl12 solutions in comparison to the originally reported data can be explain…