Electrostatic Interaction Energy Research Articles

Molecular Hydrogen Acts as a Hydrogen Bond Proton Acceptor: From Protonated Betaine Tagging to the Weakest Hydrogen Bond.

In an attempt to gain further insights into the intermolecular interactions implied by Rizzo's group's cautionary tale related to molecular tagging in infrared multiple photon dissociation (IRMPD) spectroscopy with molecular messengers [Masson, A. . J. Chem. Phys. 2015, 143, 104313], in the present study, we provide an in-depth analysis of the noncovalent interaction between the molecular hydrogen and protonated betaine molecule in the gas phase. We aim to shed some new light on the fundamental issues concerning the wide diapason of hydrogen-bonding-type intermolecular interactions, with a wide variety of proton acceptors. We demonstrate that in the course of tagging the protonated betaine with molecular hydrogen from the OH group side, it is the σ bond of molecular hydrogen that plays the role of hydrogen-bonding proton acceptor. The tagging thus induces a small yet significant red shift of the protonated betaine O-H stretching mode. We investigate the performance of a wide range of density functional theory (DFT) functionals for the calculation of anharmonic vibrational frequency shifts of the studied system, which are essential for the correct interpretation of the experimental IRMPD data. For an accurate prediction of the OH stretching frequency shifts, specifically designed functionals such as Handy's group HCTH/407 should be applied. The empirical dispersion correction enhances the systematic overestimation of the anharmonic frequency shift, characteristic of the most widely used DFT functionals. Combining the full-wave function approach with the charge field perturbation and natural bond orbital (NBO) deletion analyses, we demonstrate that the frequency shift in the OH-tagged structure is governed by the σHH → σ*OH intermolecular charge transfer. This interaction stabilizes the OH-tagged dimer as well, in contrast to the dipole-quadrupole electrostatic interaction energy term. Topological analysis of the electron density reveals the presence of an intermolecular bond critical point with a positive value of the density Laplacian very close to the lower limit for hydrogen bonds. NCI analyses demonstrate that the OH···H2 interaction is weaker than the intramolecular CH···O one within the protonated betaine molecule, with the through of reduced density gradient appearing at less negative sign(λ2)·ρ values. Analyzing the O-H stretching vibrational potential with the second-generation absolutely localized molecular orbitals energy decomposition analysis (ALMO-EDA 2) revealed that in the case of betaineH(+) tagged from the OH group side, the permanent electrostatics (ΔEelec), polarization (ΔEpol), and charge-transfer (ΔEct) contributions to the total intermolecular interaction energy contribute favorably to the weak hydrogen bond formation and to the red shift of the fundamental O-H stretching frequency, the ΔEct contribution being the most significant in the last context. The Pauli repulsion term, on the other hand, favors an O-H stretching frequency blue shift as a consequence of the vibrational confinement effects.

Two‐Way Regulation of MgFe‐LDH on ESC Cell Fate via Temporal Selective Activation of Different Cell Membrane Receptors

AbstractStem cell fate regulation by biomaterials has considerable therapeutic potential; however, the mechanisms whereby biomaterials instruct stem cells for accurate fate regulation still need to be elucidated. Layered double hydroxide (LDH) nanoparticles are widely used for tissue regeneration because of their excellent physicochemical properties and biocompatibility. This study reveals that MgFe‐LDH has bidirectional regulatory effects on the differentiation of mouse embryonic stem cells into neural progenitor cells, essentially suppressing cell differentiation on the 1st day and promoting cell differentiation on the 3rd day. Single‐cell transcriptome sequencing and simulated computation of structural analysis demonstrate that MgFe‐LDH interacts with the membrane receptors leukemia inhibitory factor receptor (LIFR, 15 nm above the cell membrane) and pached1 (PTCH1, 6 nm above the cell membrane) on the 1st and 3rd day of differentiation, respectively. LIFR has more contact with MgFe‐LDH than PTCH1 and relatively weaker electrostatic interaction energies (−11010.0 and −9829.3 kJ mol−1 for PTCH1 and LIFR, respectively). These factors determine receptor binding and activation priority, followed by cell fate regulation. The results indicate that MgFe‐LDH regulate the activity and fate of stem cells dually, thus creating possibilities for personalized therapy in neurodevelopment and regenerative medicine through an in‐depth study of cell membrane receptors.

Evaluation and improvement of Gay-Berne interaction potential to simulate 3D DLVO interaction of clay particles

This paper first presents a set of DLVO-based energy-separation functions for a pair of finite uniformly charged square platelets of infinitesimal thickness in three elementary configurations: face-to-face, edge-to-edge, and edge-to-face. The novel dataset was generated by summing the electrostatic interaction energy computed numerically by solving the non-linear 3D Poisson-Boltzmann equation and the van der Waals interaction energy calculated analytically. The dataset aims to inform qualitatively and quantitatively the energy/force separation functions used in the Discrete Element Method (DEM) and Coarse-Grained Molecular Dynamics (CGMD) modelling of clays. The same dataset was then used to calibrate and evaluate two Gay-Berne (GB)-type potentials: i) a DLVO-adapted Gay-Berne potential, where the Born-van der Waals branches of the underlying Lennard-Jones (LJ) potential are replaced with van der Waals-Columbic branches to represent DLVO interactions; ii) the Mie potential, where the exponents of the two energy terms are ‘unlocked’ instead of being set equal to 12 and 6 as per the original LJ potential. It is shown that the orientation parameter, µ, and the anisotropy parameter, ν, need to be different from µ = 2 and ν = 1 as adopted in CGMD clay modelling to capture the progression of the shape of the pair energy-separation function from face-to-face to edge-to-face and edge-to-edge configuration. It is also shown that the MIE potential (with exponents m = 3 and n = 1.5) better captures the slow decay of the electrostatic repulsive energy component of the DLVO potential energy Coulombic branch of the interaction potential compared to the DLVO-adapted GB potential, which embeds the Lennard-Jones (LJ) exponents m = 12 and n = 6.

Estimation of Electrostatic Interaction Energies on a Trapped-Ion Quantum Computer.

We present the first hardware implementation of electrostatic interaction energies by using a trapped-ion quantum computer. As test system for our computation, we focus on the reduction of NO to N2O catalyzed by a nitric oxide reductase (NOR). The quantum computer is used to generate an approximate ground state within the NOR active space. To efficiently measure the necessary one-particle density matrices, we incorporate fermionic basis rotations into the quantum circuit without extending the circuit length, laying the groundwork for further efficient measurement routines using factorizations. Measurements in the computational basis are then used as inputs for computing the electrostatic interaction energies on a classical computer. Our experimental results strongly agree with classical noise-less simulations of the same circuits, finding electrostatic interaction energies within chemical accuracy despite hardware noise. This work shows that algorithms tailored to specific observables of interest, such as interaction energies, may require significantly fewer quantum resources than individual ground state energies would require in the straightforward supermolecular approach.

Molecular basis for differential recognition of an allosteric inhibitor by receptor tyrosine kinases.

Understanding kinase-inhibitor selectivity continues to be a major objective in kinase drug discovery. We probe the molecular basis of selectivity of an allosteric inhibitor (MSC1609119A-1) of the insulin-like growth factor-I receptor kinase (IGF1RK), which has been shown to be ineffective for the homologous insulin receptor kinase (IRK). Specifically, we investigated the structural and energetic basis of the allosteric binding of this inhibitor to each kinase by combining molecular modeling, molecular dynamics (MD) simulations, and thermodynamic calculations. We predict the inhibitor conformation in the binding pocket of IRK and highlight that the charged residues in the histidine-arginine-aspartic acid (HRD) and aspartic acid-phenylalanine-glycine (DFG) motifs and the nonpolar residues in the binding pocket govern inhibitor interactions in the allosteric pocket of each kinase. We suggest that the conformational changes in the IGF1RK residues M1054 and M1079, movement of the ⍺C-helix, and the conformational stabilization of the DFG motif favor the selectivity of the inhibitor toward IGF1RK. Our thermodynamic calculations reveal that the observed selectivity can be rationalized through differences observed in the electrostatic interaction energy of the inhibitor in each inhibitor/kinase complex and the hydrogen bonding interactions of the inhibitor with the residue V1063 in IGF1RK that are not attained with the corresponding residue V1060 in IRK. Overall, our study provides a rationale for the molecular basis of recognition of this allosteric inhibitor by IGF1RK and IRK, which is potentially useful in developing novel inhibitors with improved affinity and selectivity.

Molecular Insights into Water-Chloride and Water-Water Interactions in the Supramolecular Architecture of Aconine Hydrochloride Dihydrate.

Despite the previous preparation of aconine hydrochloride monohydrate (AHM), accurate determination of the crystal's composition was hindered by severely disordered water molecules within the crystal. In this study, we successfully prepared a new dihydrate form of the aconine hydrochloride [C25H42NO9+Cl-·2(H2O), aconine hydrochloride dihydrate (AHD)] and accurately refined all water molecules within the AHD crystal. Our objective is to elucidate both water-chloride and water-water interactions in the AHD crystal. The crystal structure of AHD was determined at 136 K using X-ray diffraction and a multipolar atom model was constructed by transferring charge-density parameters to explore the topological features of key short contacts. By comparing the crystal structures of dihydrate and monohydrate forms, we have observed that both AHD and AHM exhibit identical aconine cations, except for variations in the number of water molecules present. In the AHD crystal, chloride anions and water molecules serve as pivotal connecting hubs to establish three-dimensional hydrogen bonding networks and one-dimensional hydrogen bonding chain; both water-chloride and water-water interactions assemble supramolecular architectures. The crystal packing of AHD exhibits a complete reversal in the stacking order compared to AHM, thereby emphasizing distinct disparities between them. Hirshfeld surface analysis reveals that H···Cl- and H···O contacts play a significant role in constructing the hydrogen bonding network and chain within these supramolecular architectures. Furthermore, topological analysis and electrostatic interaction energy confirm that both water-chloride and water-water interactions stabilize supramolecular architectures through electrostatic attraction facilitated by H···Cl- and H···O contacts. Importantly, these findings are strongly supported by the existing literature evidence. Consequently, navigating these water-chloride and water-water interactions is imperative for ensuring storage and safe processing of this pharmaceutical compound.

Probing the selective interaction mechanisms of propyl gallate with diaspore and kaolinite from a microscopic force view

The microscopic force between collector and mineral is the fundamental mechanism for selective adsorption of collector on mineral surface. Propyl gallate (PG) is a highly selective collector for the separation of diaspore and kaolinite, and its selective collection performance is better than that of traditional collector sodium oleate (NaOL). The selective interaction mechanisms of PG with diaspore were analyzed using EDLVO theory and AFM analysis in this study. EDLVO calculation results indicate that the electrostatic interaction energy and hydrophobic interaction energy of diaspore particles treated by PG were higher than that of NaOL. AFM results also show that the interaction force between PG and diaspore is greater than that between NaOL and diaspore, confirming the fact that PG had better collection and selectivity than NaOL for diaspore. This work revealed the selective interaction mechanism of PG collector with diaspore other than kaolinite at a molecular level, which would deepen the understanding of the selective flotation of PG for diaspore from kaolinite.

Electrostatic interaction energy between the electrodes of a concentric coplanar sensor

The capacitive testing method using coplanar capacitive sensors represents a relatively new technique for non-destructive evaluation of the properties of a given material. The most conventional design of a coplanar capacitive sensor is that of two oppositely charged coplanar electrodes located at some separation distance from each other. The electrodes can have any shape including designs with circular symmetry. The concentric coplanar sensor is a special case of a device with circular symmetry. It comprises a disk as the inner electrode and an annulus as the outer one. In this work we analyze the features of the electrostatic interaction energy between the two electrodes of a concentric coplanar sensor by considering a model consisting of a uniformly charged disk and a uniformly charged annulus that is concentric and coplanar to the disk. For the sake of generality, we assume that the two objects carry an arbitrary amount of net charge and their dimensions are arbitrary. We obtain an exact expression for the electrostatic interaction energy of the system as a function of three important length scales, radius of disk and inner/outer radii of the annulus. The interplay between these parameters determines the features of the electrostatic interaction energy between the electrodes as well as the overall performance of the sensor.

Regulating interfacial ion migration with pillar effect in layer-by-layer inter-embedded MoS2/Ti3C2 for high-performance zinc-ion batteries

Two-dimensional (2D) layered materials have promising prospects for Zn-storage due to their flexible and adjustable interlayer architecture. The strong electrostatic interaction and high diffusion energy barrier, however, lead to slow diffusion kinetics of Zn-ions between the 2D interfaces, limiting its widespread application. Herein, Ti3C2 MXene is introduced into the MoS2 interlayer by the “pillar effect” to assemble a layer-by-layer inter-embedded structure (L-MoS2/Ti3C2), which provides sufficient diffusion channels for Zn-ions. DFT computations and GITT confirm that the L-MoS2/Ti3C2 exhibits superior Zn-ions migration kinetics. Therefore, L-MoS2/Ti3C2 shows excellent long-term cycling stability (75.6% capacity retention after 7000 cycles at 15 A g-1) and glorious high-rate capability (107 mAh g-1 at 20 A g-1). In addition, the practical application of this material is demonstrated by evaluating the performance of L-MoS2/Ti3C2 in flexible quasi-solid-state aqueous zinc ion batteries under various extreme bending conditions, which exhibits good stability under 180° during the 4000 cycles with a capacity retention of 80.5% at 2.0 A g-1.

Docosahexaenoic acid promotes vesicle clustering mediated by alpha-Synuclein via electrostatic interaction.

α-Synuclein (α-Syn) is an intrinsically disordered protein whose aggregation is associated with Parkinson's disease, dementia, and other neurodegenerative diseases known as synucleinopathies. However, the functional role of α-Syn is still unclear, although it has been shown to be involved in the regulation of neurotransmitter release via the interaction with synaptic vesicles (SVs), vesicle clustering, and SNARE complex assembly. Fatty acids have significant occupancy in synaptic vesicles; and recent studies suggest the interaction of fatty acids with α-Syn affect the formation of (pathological) aggregates, but it is less clear how fatty acids affects the functional role of α-Syn including α-Syn-membrane interactions, in particular with (SV-like) vesicles. Here, we report the concentration dependent effect of docosahexaenoic acid (DHA) in synaptic-like vesicle clustering via α-Syn interaction. Through molecular dynamics simulation, we revealed that DHA promoted vesicle clustering is due to the electrostatic interaction between DHA in the membrane and the N-terminal region of α-Syn. Moreover, this increased electrostatic interaction arises from a change in the macroscopic properties of the protein-membrane interface induced by (preferential solvation of) DHA. Our results provide insight as to how DHA regulates vesicle clustering mediated by α-Syn and may further be useful to understand its physiological as well as pathological role. Description: In physiological environments, α-Synuclein (α-Syn) localizes at nerve termini and synaptic vesicles and interacts with anionic phospholipid membranes to promote vesicle clustering. Docosahexaenoic acid (DHA) increases binding affinity between α-Syn and lipid membranes by increasing electrostatic interaction energy through modulating the local and global membrane environment and conformational properties of α-Syn.

Molecular Dynamics Investigation on the Diffusion of POSS in Insulating Oil Under External Electric Field

In this study, the interaction energy and migration characteristics of caged octaphenylpropyl Polysilsesquioxane (POSS) molecules in vegetable insulating oil and mineral insulating oil under external electric field is investigated. The results show that POSS molecules have stronger migration ability in mineral oil, but the electric field has no obvious effect on the migration ability of POSS molecules in mineral oil. In addition, the electric field can promote the diffusion of POSS molecules in vegetable oil, which is caused by the increase of electrostatic interaction energy between POSS molecules and vegetable oil molecules under the electric field. Furthermore, mineral oil molecules and vegetable oil molecules have strong interaction with the Si-O structure and peripheral branches of POSS molecules, which limits the diffusion of POSS molecules in vegetable oil, and further explain the reason for the large displacement of POSS molecules in mineral oil system. This work is of great significance to the application research of nano-additives in dielectrics.

Investigation on high performance and stabilized surface of AlF3-coated V2O5 micro-flower for zinc energy storage

Vanadium oxide (V2O5) cathode material, possessing abundant reserves and high theoretical capacity, has been extensively researched in aqueous zinc ion batteries (ZIBs). However, its electrochemical performance is significantly hindered by insufficient electronic conductivity, vanadium dissolution into electrolyte, and slow diffusion kinetics. In this study, the V2O5 micro-flower was first synthesized by a solvothermal method, and then modified by coating with AlF3 passivation layer, forming AlF3@V2O5 hybrid material. Impressively, AlF3@V2O5 exhibits excellent electrochemical and kinetic properties due to the special structure of V2O5 and the interfacial protection of AlF3. An exceptional rate property (325 mAh g−1 at 0.1 A g−1, 188 mAh g−1 at 15 A g−1) as well as extraordinary cycling stability with 89.3% capacity retention after 6000 cycles at 10 A g−1 can be attained with 2 wt% AlF3 addition (that is AF-2@V2O5). The computation based on density functional theory (DFT) suggests that AlF3 coating can reduce the interlayer electrostatic interaction and adsorption energy barrier between the intercalated Zn2+ and V2O5 host, thereby enabling fast redox kinetics. This study showcases the efficacy of interfacial modification of passivated coatings and presents an influential approach for material design in ZIBs.

Computer-assisted drug discovery of potential natural inhibitors of the SARS-CoV-2 RNA-dependent RNA polymerase through a multi-phase in silico approach.

The COVID-19 pandemic has led to significant loss of life and economic disruption worldwide. Currently, there are limited effective treatments available for this disease. SARS-CoV-2 RNA-dependent RNA polymerase (SARS-CoV-2 RdRp) has been identified as a potential target for drug development against COVID-19. Natural products have been shown to possess antiviral properties, making them a promising source for developing drugs against SARS-CoV-2. The objective of this study is to identify the most effective natural inhibitors of SARS-CoV-2 RdRp among a set of 4924 African natural products using a multi-phase in silico approach. The study utilized remdesivir (RTP), the co-crystallized ligand of RdRp, as a starting point to select compounds that have the most similar chemical structures among the examined set of compounds. Molecular fingerprints and structure similarity studies were carried out in the first part of the study. The second part of the study included molecular docking against SARS-CoV-2 RdRp (PDB ID: 7BV2) and Molecular Dynamics (MD) simulations including the calculation of RMSD, RMSF, Rg, SASA, hydrogen bonding, and PLIP. Moreover, the calculations of Molecular mechanics with generalised Born and surface area solvation (MM-GBSA) Lennard-Jones and Columbic electrostatic interaction energies have been conducted. Additionally, in silico ADMET and toxicity studies were performed to examine the drug likeness degrees of the selected compounds. Eight compounds were identified as the most effective natural inhibitors of SARS-CoV-2 RdRp. These compounds are kaempferol 3-galactoside, kaempferol 3-O-β-D-glucopyranoside, mangiferin methyl ether, luteolin 7-O-β-D-glucopyranoside, quercetin-O-β-D-3-glucopyranoside, 1-methoxy-3-indolylmethyl glucosinolate, naringenin, and asphodelin A 4'-O-β-D-glucopyranoside. The results of this study provide valuable information for the development of natural product-based drugs against COVID-19. However, the elected compounds should be further studied in vitro and in vivo to confirm their efficacy in treating COVID-19.

The diffusion characteristics of POSS under electric field and non-uniform temperature field in natural ester insulating oil

The natural ester insulating oil is a green and environmentally friendly liquid dielectric, and nano additives can effectively improve its dielectric and heat transfer performance. However, nano additives are prone to agglomeration, especially under the influence of electric and temperature fields, which can impact the prolonged stable operation of power transformers. In this paper, the diffusion properties of caged Polysilsesquioxane (POSS) molecules in natural ester insulating oil under external electric field and non-uniform temperature field were investigated via simulation, and the effects of temperature and electric field on POSS molecules were expounded from the perspective of interaction. The results show that the high temperature difference and strong electric field can effectively improve the mobility of POSS molecules, and the temperature difference has a greater impact on the diffusion. The decrease of interaction energy is mainly due to the negative positive interaction between Si-O molecules in POSS molecules and insulating oil at high temperature, which counteracts the attraction of branch chains. At the same time, POSS molecules in the electric field will also show obvious polarization due to temperature changes, which further reduces the interaction between POSS molecules and insulating oil molecules. In addition, the electrostatic interaction energy decreases most obviously, which is the main reason that affects the migration characteristics of POSS molecules in natural ester insulating oil. This study provides a theoretical explanation for the migration mechanism of insulating oil in the microenvironment.

Deciphering the driving forces in crystal packing by analysis of electrostatic energies and contact enrichment ratios.

Hirshfeld surface analysis is a widely used tool for identifying the types of intermolecular contacts that contribute most significantly to crystal packing stabilization. One useful metric for analyzing these contacts is the contact enrichment descriptor, which indicates the types of contacts that are over- or under-represented. In this statistical study, enrichment ratios were combined with electrostatic energy (Eelec) data for a variety of compound families. To compute the electrostatic interaction energy between atoms, charge density models from the ELMAM2 database of multipolar atoms were used. As expected, strong hydrogen bonds such as O/N-H...N and O/N-H...O typically display large enrichment values and have the most negative (i.e. favorable) electrostatic energies. Conversely, contacts that are repulsive from an electrostatic perspective are usually the most under-represented. Analyzing the enrichment ratio and electrostatic energy indicators was shown to help identify which favorable contacts are the most competitive with each other. For weaker interactions, such as hydrophobic contacts, the behavior is less clear cut and can depend on other factors such as the chemical content of the molecule. The anticorrelation between contact enrichment and Eelec is generally lost for weaker contacts. However, we observed that C...C contacts are often enriched in crystal structures containing heterocycles, despite the low electrostatic attraction. For molecules with only weak hydrogen bond donors/acceptors and hydrophobic groups, the correlation between contact enrichment and Eelec is still evident for the strongest of these interactions. However, there are some exceptions where the most favorable contacts from an electrostatic perspective are not the most over-represented. This can occur in cases where the shape of the molecule is complex or elongated, favoring dispersion forces and shape complementarity in the packing.

Nitric acid oxidation and urea modification of carbon fibres as biofilm carriers

ABSTRACT Carbon fibres (CF) are commonly used as carriers in biofilm-based wastewater treatment. The surface properties of the CF are herein modified using a combination of nitric acid oxidation and urea to optimise the carrier to immobilise bacterial cells. The capacity of the CF carriers to immobilise bacterial cells and activated sludge is evaluated using bacterial cell adhesion and sludge immobilisation tests. The total interaction energy profiles between the CF supports and bacterial cells were calculated according to the Derjaguin–Landau–Verwey–Overbeek (DLVO) theory to explain the mechanism by which these modifications enhance this immobilisation capacity. CF-U has a high capacity for immobilising bacterial cells and activated sludge (3.7 g-sludge/g-CF supports) owing to its low total interaction energy. Nitric acid oxidation reduced the diiodomethane contact angle of CF from 55.1° to 38.5°, which reduced the Lifshitz-van der Waals interaction energy, while urea modification further increased the zeta potential of CF from 12.8 mV to −0.7 mV, thereby reducing the electrostatic interaction energy. Experiments and DLVO theory both determined that a combination of nitric acid oxidation and urea modification significantly enhanced the ability of CF to immobilise microorganisms.

Morphology control by tuning electrostatic interactions for efficient polythiophene-based all-polymer solar cells

•Correlations between electrostatic force and interaction energy are established •Domain purity of the film can be modulated by tuning the donor:acceptor ESP difference •A high PCE of 15.3% is demonstrated in a PT-based all-polymer solar cell Polythiophenes are one of the most classical donors for organic solar cells, which have simple chemical structures and thus low production costs. However, their photovoltaic performance is lagging far behind the donor-acceptor-type polymers, especially when blending with polymer acceptors, where morphology control is a huge challenge. Here, we systematically study the intermolecular interaction in polythiophene:polymer acceptor (PY-IT) combinations and establish a rational relationship between chemical structure and blend miscibility. Our results suggest that the electrostatic force plays a key role in determining the donor:acceptor intermolecular interaction energy. Introducing electron-withdrawing functional groups into the backbone of P3HT can increase the electrostatic potential (ESP) and suppress the intermolecular interaction with PY-IT. Due to the proper miscibility and improved domain purity, the corresponding polymer PDCBT records a high-power conversion efficiency (PCE) of 15.3%, which is the highest value in polythiophene-based all-polymer solar cells (all-PSCs) and crucial for advancing their practical applications. Polythiophenes are one of the most classical donors for organic solar cells, which have simple chemical structures and thus low production costs. However, their photovoltaic performance is lagging far behind the donor-acceptor-type polymers, especially when blending with polymer acceptors, where morphology control is a huge challenge. Here, we systematically study the intermolecular interaction in polythiophene:polymer acceptor (PY-IT) combinations and establish a rational relationship between chemical structure and blend miscibility. Our results suggest that the electrostatic force plays a key role in determining the donor:acceptor intermolecular interaction energy. Introducing electron-withdrawing functional groups into the backbone of P3HT can increase the electrostatic potential (ESP) and suppress the intermolecular interaction with PY-IT. Due to the proper miscibility and improved domain purity, the corresponding polymer PDCBT records a high-power conversion efficiency (PCE) of 15.3%, which is the highest value in polythiophene-based all-polymer solar cells (all-PSCs) and crucial for advancing their practical applications.

Subclass Effects on Self-Association and Viscosity of Monoclonal Antibodies at High Concentrations.

The effects of a subclass of monoclonal antibodies (mAbs) on protein-protein interactions, formation of reversible oligomers (clusters), and viscosity (η) are not well understood at high concentrations. Herein, we quantify a short-range anisotropic attraction between the complementarity-determining region (CDR) and CH3 domains (KCDR-CH3) for vedolizumab IgG1, IgG2, or IgG4 subclasses by fitting small-angle X-ray scattering (SAXS) structure factor Seff(q) data with an extensive library of 12-bead coarse-grained (CG) molecular dynamics simulations. The KCDR-CH3 bead attraction strength was isolated from the strength of long-range electrostatic repulsion for the full mAb, which was determined from the theoretical net charge and a scaling parameter ψ to account for solvent accessibility and ion pairing. At low ionic strength (IS), the strongest short-range attraction (KCDR-CH3) and consequently the largest clusters and highest η were observed with IgG1, the subclass with the most positively charged CH3 domain. Furthermore, the trend in KCDR-CH3 with the subclass followed the electrostatic interaction energy between the CDR and CH3 regions calculated with the BioLuminate software using the 3D mAb structure and molecular interaction potentials. Whereas the equilibrium cluster size distributions and fractal dimensions were determined from fits of SAXS with the MD simulations, the degree of cluster rigidity under flow was estimated from the experimental η with a phenomenological model. For the systems with the largest clusters, especially IgG1, the inefficient packing of mAbs in the clusters played the largest role in increasing η, whereas for other systems, the relative contribution from stress produced by the clusters was more significant. The ability to relate η to short-range attraction from SAXS measurements at high concentrations and to theoretical characterization of electrostatic patches on the 3D surface is not only of fundamental interest but also of practical value for mAb discovery, processing, formulation, and subcutaneous delivery.

Varvec{J}-, M- and varvec{L}-integrals of line charges and line forces

In this work, the varvec{J}-, M- and varvec{L}-integrals of two line charges and two line forces in generalized plane strain are derived in the framework of three-dimensional (3D) electrostatics and three-dimensional compatible linear elasticity, respectively, in order to study the interaction between them. The key point in this derivation is achieved by expressing the varvec{J}-, M- and varvec{L}-integrals of point charges and point forces in three dimensions in terms of the corresponding three-dimensional Green functions, that is, the three-dimensional Green function of the Laplace operator and the three-dimensional Green tensor of the Navier operator, respectively. The major mathematical tool used in deriving the varvec{J}-, M- and L_3-integrals of line charges and line forces from the corresponding varvec{J}-, M- and varvec{L}-integrals of point charges and point forces is the method of embedding or method of descent of Green functions to two dimensions (2D) from the corresponding Green functions in 3D. The analytical expressions of varvec{J}-, M- and L_3-integrals of line charges and line forces in antiplane and plane strain are derived and discussed. The varvec{J}-integral is the electrostatic part of the Lorentz force (electrostatic interaction force) between two line charges in electrostatics and the Cherepanov force between two line forces in elasticity. The M-integral of two line sources (charges or forces) equals half the electrostatic interaction energy in electrostatics and half the elastic interaction energy in elasticity of these two line sources, respectively. The L_3-integral of two line sources (charges or forces) is the z-component of the configurational vector moment or the rotational moment representing the total torque about the z-axis caused by the interaction of the two line sources. An important outcome is that the varvec{J}-integral is twice the negative gradient of the M-integral, leading to the result that the {varvec{J}}-integral for line charges and line forces is a conservative force (with the corresponding interaction energy playing the role of the potential energy) and consequently an irrotational vector field. Finally, the obtained varvec{J}-, M- and L_3-integrals being functions of the distance and of the angle, are able to describe the physical behaviour of the interaction of two line sources (charges and forces), since they represent the fundamental and necessary quantities, that is, the interaction force, interaction energy and total torque produced by the interaction of these two line sources.

Competitive adsorption characteristics of gasoline evaporated VOCs in microporous activated carbon by molecular simulation

The activated carbon in the vehicle's carbon canister needs to adsorb a variety of VOCs (Volatile Organic Compounds) emitted by gasoline evaporation, while the difference in gas adsorption capacity can lead to adsorption competition phenomena. In this study, three typical VOCs (toluene, cyclohexane, and ethanol) were selected to study the adsorption competition characteristics between multi-component gases at different pressures by molecular simulation method. In addition, the effect of temperature on adsorption competition was also investigated. The results show that the selectivity of activated carbon to toluene is negatively correlated with the adsorption pressure, but the opposite is true for ethanol, and the change of cyclohexane is not significant. The competitive order of the three VOCs is toluene > cyclohexane > ethanol at low pressure, which becomes ethanol > toluene > cyclohexane at high pressure. With increasing pressure, the interaction energy decreases from 12.87 kcal/mol to 11.87 kcal/mol, where the electrostatic interaction energy increases from 1.97 kcal/mol to 2.54 kcal/mol. In microporous activated carbon, the competition is mainly manifested in that ethanol preempts the low-energy adsorption sites of toluene in the pore size of 10 Å to 18 Å, while gas molecules near the surface of activated carbon or in smaller pore sizes are stably adsorbed without competition. Despite the fact that high temperature decreases the total adsorption capacity, activated carbon selectivity for toluene increases instead, while the competitiveness of polar ethanol decreases significantly.