Nanodiamonds exhibit exceptional
colloidal properties in aqueous
media that lead to a wide range of applications in nanomedicine and
other fields. Nevertheless, the role of surface chemistry on the hydration
of nanodiamonds remains poorly understood. Here, we probed the water
hydrogen bond network in aqueous dispersions of nanodiamonds by infrared,
Raman, and X-ray absorption spectroscopies applied in situ in aqueous
environment. Aqueous dispersions of nanodiamonds with hydrogenated,
carboxylated, hydroxylated, and polyfunctional surface terminations
were compared. A different hydrogen bond network was found in hydrogenated
nanodiamonds dispersions compared to dispersions of nanodiamonds with
other surface terminations. Although no hydrogen bonds are formed
between water and hydrogenated surface groups, a long-range disruption
of the water hydrogen bond network is evidenced in hydrogenated nanodiamonds
dispersion. We propose that this unusual hydration structure results
from electron accumulation at the diamond–water interface.
The structure of aqueous alcohol solutions at the molecular level for many decades has remained an intriguing topic in numerous theoretical and practical investigations. The aberrant thermodynamic properties of water-alcohol mixtures are believed to be caused by the differences in energy of hydrogen bonding between water-water, alcohol-alcohol, and alcohol-water molecules. We present the Raman scattering spectra of water, ethanol, and water-ethanol solutions with 20 and 70 vol % of ethanol thoroughly measured and analyzed at temperatures varying from -10 to +70 °C. Application of the MCR-ALS method allowed for each spectrum to extract contributions of molecules with different strengths of hydrogen bonding. The energy (enthalpy) of formation/weakening of hydrogen bonds was calculated using the slope of Van't Hoff plot. The energy of hydrogen bonding in 20 vol % of ethanol was found the highest among all the samples. This finding further supports appearance of clathrate-like structures in water-ethanol solutions with concentrations around 20 vol % of ethanol.
Although vodka is a reasonably pure mixture of alcohol and water, beverage drinks typically show differences in appeal among brands. The question immediately arises as to the molecular basis, if any, of vodka taste perception. This study shows that commercial vodkas differ measurably from ethanol-water solutions. Specifically, differences in hydrogen-bonding strength among vodkas are observed by (1)H NMR, FT-IR, and Raman spectroscopy. Component analysis of the FT-IR and Raman data reveals a water-rich hydrate of composition E x (5.3 +/- 0.1)H(2)O prevalent in both vodka and water-ethanol solutions. This composition is close to that of a clathrate-hydrate observed at low temperature, implying a cage-like morphology. A structurability parameter (SP) is defined by the concentration of the E x (5.3 +/- 0.1)H(2)O hydrate compared to pure ethanol-water at the same alcohol content. SP thus measures the deviation of vodka from "clean" ethanol-water solutions. SP quantifies the effect of a variety of trace compounds present in vodka. It is argued that the hydrate structure E x (5.3 +/- 0.1)H(2)O and its content are related to the perception of vodka.
The interaction of nanodiamond (ND) particles produced by detonation synthesis with water molecules in ND water suspensions was studied using Raman and photoluminescence spectroscopy. To address the role of the surface chemistry of ND particles, NDs with heterogeneous surface groups as well as ND particles enriched with carboxyl-, hydroxyl-, and fluorine-containing surface groups were investigated. The influence of the nanodiamond particles on the shape and position of the water valence band in the Raman spectra of ND water suspensions was demonstrated for the first time. Changes in the water band parameters take place up to 1.5 mg/mL of NDs in all studied suspensions and are most pronounced for the ND functionalized with COOH groups. A correlation between increasing ND luminescence intensity and strengthening of hydrogen bonds formed at the interface of ND and water molecules in water suspensions of variously functionalized NDs was found. The most intense ND luminescence was detected for the ND functionalized with OH groups, forming the strongest hydrogen bonds among the studied samples.
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