Homogeneous water vapor condensation with a deep neural network potential model.

Molecular-level nucleation has not been clearly understood due to the complexity of multi-body potentials and the stochastic, rare nature of the process. This work utilizes molecular dynamics (MD) simulations, incorporating a first-principles-based deep neural network (DNN) potential model, to investigate homogeneous water vapor condensation. The nucleation rates and critical nucleus sizes predicted by the DNN model are compared against commonly used semi-empirical models, namely extended simple point charge (SPC/E), TIP4P, and OPC, in addition to classical nucleation theory (CNT). The nucleation rates from the DNN model are comparable with those from the OPC model yet surpass the rates from the SPC/E and TIP4P models, a discrepancy that could mainly arise from the overestimated bulk free energy by SPC/E and TIP4P. The surface free energy predicted by CNT is lower than that in MD simulations, while its bulk free energy is higher than that in MD simulations, irrespective of the potential model used. Further analysis of cluster properties with the DNN model unveils pronounced variations of O-H bond length and H-O-H bond angle, along with averaged bond lengths and angles that are enlarged during embryonic cluster formation. Properties such as cluster surface free energy and liquid-to-vapor density transition profiles exhibit significant deviations from CNT assumptions.

The dynamics of chemically propelled dimer motors on a pinning substrate.

The dynamics of self-propelled micro-motors, in a thin fluid film containing an attractive substrate, is investigated by means of a particle-based simulation. A chemically powered sphere dimer, consisting of a catalytic and a noncatalytic sphere, may be captured by a trap on the substrate and consequently rotates around the trap center. A pair of trapped dimers spontaneously forms various configurations, including anti-parallel aligned doublets and head-to-tail rotating doublets. Small traps randomly distributed on the substrate are capable of pinning the dimers. The diffusion coefficient decreases with increasing pinning force or the pinning density, and it falls quickly at a certain critical pinning force beyond which the dimer motor is pinned completely. It is found that the pin array on the substrate gives rise to the formation of clusters of dimers and the underlying mechanism is discussed.

DFT study on the effect of functional groups of carbonaceous surface on ammonium adsorption from water.

Density functional theory (DFT) was used to study the adsorption of ammonium ion on carbon materials. The effects of single and multiple adjacent functional groups of carbon structures on ammonium ion adsorption were emphasized. The electrostatic potential, adsorption energy, charge transfer, molecular orbital, and dipole moment of different configurations were analyzed. Results showed that the carbonyl group was more likely to adsorb ammonium ion than lactone, carboxyl, and hydroxyl. When the carbon material contained multiple adjacent functional groups at the same time, the adsorption of ammonium ion can be promoted or inhibited due to the interaction among functional groups. The effect of functional groups on the adsorption of π bond in carbon materials was related to the electronegativity of functional groups, i.e., greater electronegativity led to smaller adsorption energy of π bond. Carbon material itself is nonpolar and hydrophobic, so adding oxygen-containing functional groups can increase the dipole moment of carbon material molecules, thereby enhancing its polarity and adsorption capacity.

Computational study of phosphate adsorption on Mg/Ca modified biochar structure in aqueous solution.

Phosphate removal in water using biochar is widely investigated. Density functional theory was used to study the adsorption of phosphate (H2PO4-) on biochar in water after metal modification. Two types of metals, Mg and Ca, were used to modify the biochar structure, and the edge and metal adsorptions of H2PO4- were investigated on the modified biochar structure. Results were analyzed from the aspects of structural stability, adsorption energy, change in dipole moment, density of electronic states, and atoms in molecules analysis. The overall effect of metal-modified biochar materials on phosphate adsorption was stronger than that of unmodified biochar materials in terms of molecular level. The stability of the metal-modified structure by adding metal was low, and adsorption was prone to occur in this situation. The Ca-modified biochar showed better phosphate adsorption than the Mg-modified structure. Metal adsorption performed better than edge adsorption, proving that the modified metal in the biochar structure played a leading role in H2PO4- adsorption. Metal adsorption was mainly caused by electrostatic attraction, and edge adsorption was mainly caused by covalent bonding.

Quantum chemistry study on the destruction mechanism of 2,3,7,8-TCDD by OH and O(3) radicals.

Due to its fundamental importance, the destruction mechanism of the dioxins, as exemplified by 2,3,7,8-TCDD, by OH and O3 radicals was investigated in detail employing Quantum Chemical Calculations in this paper. Theoretical results showed that, OH radical degraded 2,3,7,8-TCDD via substituting chlorine at the 2,3,7,8 positions, while O3 radical degraded 2,3,7,8-TCDD via destructing CC bonds and aromatic ring. Based on the mechanism study, the kinetic parameters of the reactions were also calculated by Transition State Theory. By comparing, the rate constant of the 2,3,7,8-TCDD destruction by OH was found to be much higher than that by O3, which indicated that OH radical have much stronger ability to degrade 2,3,7,8-TCDD than O3 radical. This finding was consistent with the standard electrode potential of OH and O3 radical. The theoretical results in this paper can be believed to supply important theory basis for the further investigation on dioxins removal by using the catalytic oxidation technology.