Molecular Simulation of CO2/H2 Mixture Separation in Metal-organic Frameworks： Effect of Catenation and Electrostatic Interactions

In this work grand canonical Monte Carlo simulations were performed to study gas separation in three pairs of isoreticular metal-organic frameworks (IRMOFs) with and without catenation at room temperature.Mixture composed of CO2 and H2 was selected as the model system to separate.The results show that CO2 selectivity in catenated MOFs with multi-porous frameworks is much higher than their non-catenated counterparts.The simulations also show that the electrostatic interactions are very important for the selectivity,and the contributions of different electrostatic interactions are different,depending on pore size,pressure and mixture composition.In fact,changing the electrostatic interactions can even qualitatively change the adsorption behavior.A general conclusion is that the electrostatic interactions between adsorbate molecules and the framework atoms play a dominant role at low pressures,and these interactions in catenated MOFs have much more pronounced effects than those in their non-catenated counterparts,while the electrostatic interactions between adsorbate molecules become evident with increasing pressure,and eventually dominant.

Minimizing electrostatic interactions from piezoresponse force microscopy via capacitive excitation

Piezoresponse force microscopy(PFM)has emerged as one of the most powerful techniques to probe ferroelectric materials at the nanoscale,yet it has been increasingly recognized that piezoresponse measured by PFM is often influenced by electrostatic interactions.In this letter,we report a capacitive excitation PFM(ce-PFM)to minimize the electrostatic interactions.The effectiveness of ce-PFM in minimizing electrostatic interactions is demonstrated by comparing the piezoresponse and the effective piezoelectric coefficient measured by ce-PFM and conventional PFM.The effectiveness is further confirmed through the ferroelectric domain pattern imaged via ce-PFM and conventional PFM in vertical modes,with the corresponding domain contrast obtained by ce-PFM is sharper than conventional PFM.These results demonstrate ce-PFM as an effective tool to minimize the interference from electrostatic interactions and to image ferroelectric domain pattern,and it can be easily implemented in conventional atomic force microscope(AFM)setup to probe true piezoelectricity at the nanoscale.

On electrostatic interactions of adenosine triphosphate-insulin-degrading enzyme revealed by quantum mechanics/molecular mechanics and molecular dynamics

The insulin-degrading enzyme(IDE)plays a significant role in the degradation of the amyloid beta(Aβ),a peptide found in the brain regions of the patients with early Alzheimer’s disease.Adenosine triphosphate(ATP)allosterically regulates the Aβ-degrading activity of IDE.The present study investigates the electrostatic interactions between ATP-IDE at the allosteric site of IDE,including thermostabilities/flexibilities of IDE residues,which have not yet been explored systematically.This study applies the quantum mechanics/molecular mechanics(QM/MM)to the proposed computational model for exploring electrostatic interactions between ATP and IDE.Molecular dynamic(MD)simulations are performed at different temperatures for identifying flexible and thermostable residues of IDE.The proposed computational model predicts QM/MM energy-minimised structures providing the IDE residues(Lys530 and Asp385)with high binding affinities.Considering root mean square fluctuation values during the MD simulations at 300.00 K including heat-shock temperatures(321.15 K and 315.15 K)indicates that Lys530 and Asp385 are also the thermostable residues of IDE,whereas Ser576 and Lys858 have high flexibilities with compromised thermostabilities.The present study sheds light on the phenomenon of biological recognition and interactions at the ATP-binding domain,which may have important implications for pharmacological drug design.The proposed computational model may facilitate the development of allosteric IDE activators/inhibitors,which mimic ATP interactions.

Electrostatic Interaction-directed Construction of Hierarchical Nanostructured Carbon Composite with Dual Electrical Conductive Networks for Zinc-ion Hybrid Capacitors with Ultrastability

Metal-organic framework(MOF)-derived carbon composites have been considered as the promising materials for energy storage.However,the construction of MOF-based composites with highly controllable mode via the liquid-liquid synthesis method has a great challenge because of the simultaneous heterogeneous nucleation on substrates and the self-nucleation of individual MOF nanocrystals in the liquid phase.Herein,we report a bidirectional electrostatic generated self-assembly strategy to achieve the precisely controlled coatings of single-layer nanoscale MOFs on a range of substrates,including carbon nanotubes(CNTs),graphene oxide(GO),MXene,layered double hydroxides(LDHs),MOFs,and SiO_(2).The obtained MOF-based nanostructured carbon composite exhibits the hierarchical porosity(V_(meso)/V_(micro)∶2.4),ultrahigh N content of 12.4 at.%and"dual electrical conductive networks."The assembled aqueous zinc-ion hybrid capacitor(ZIC)with the prepared nanocarbon composite as a cathode shows a high specific capacitance of 236 F g^(-1)at 0.5 A g^(-1),great rate performance of 98 F g^(-1)at 100 A g^(-1),and especially,an ultralong cycling stability up to 230000 cycles with the capacitance retention of 90.1%.This work develops a repeatable and general method for the controlled construction of MOF coatings on various functional substrates and further fabricates carbon composites for ZICs with ultrastability.

Resolution enhancement in hydrophobic interaction chromatography via electrostatic interactions

In this work,a new type of hydrophobic stationary phase that provide electrostatic interactions with analytes was developed by bondingβ-phenylethylamine as a functional ligand to silica.This stationary phase can separate proteins with similar hydrophobicity that traditional hydrophobic resins cannot.Hen egg white was separated to examine the selectivity.The results show that the introduced electrostatic interactions are an important factor for the resolution enhancement and the new resin could have important applications in separation and purification of biological macromolecules.

Hybrid Hydrogels Toughened by Chemical Covalent Bonding and Physical Electrostatic Interactions

Polystyrene nanoparticles with negative charges（n-PSs） were synthesized using styrene（St） and sodium styrene sulfonate（NaSS） as initial materials by surfactant-free emulsion polymerization. Subsequently, a hybrid hydrogel was prepared using acrylamide（AAm） and methacryloyloxyethyltrimethyl ammonium chloride（DMC） as co-monomers with N,N＇-methylenebisacrylmnide（MBA） as a chemical crosslinker and n-PSs as a physical electrostatic interaction agent. The resulting hybrid hydrogels exhibited excellent tensile strength and elongation at break. The tensile stress of hybrid hydrogels was seven times greater than that ofhydrogels without n-PSs. The elongation at break of hydrogels reached 700%, which was much higher compared to those of the hydrogels without n-PSs. Furthermore, swelling measurements of the hydrogels indicate that there is an overshoot in the swelling process and the extent of overshoot decreases with the increasing n-PSs. Therefore, the work presented here provides a method for improving the mechanical properties of hydrogels via the introduction of polymeric nanoparticles.

Nerve conduction models in myelinated and unmyelinated nerves based on three-dimensional electrostatic interaction

Until now, nerve conduction has been described on the basis of equivalent circuit model and cable theory, both of which supposed closed electric circuits spreading inside and outside the axoplasm. With these conventional models, we can simulate the propagating pattern of action potential along the axonal membrane based on Ohm＇s law and Kirchhoff＇s law. However, we could not fully explain the different conductive patterns in unmyelinated and myelinated nerves with these theories. Also, whether we can really suppose closed electrical circuits in the actual site of the nerves or not has not been fully discussed yet. In this report, a recently introduced new theoretical model of nerve conduction based on electrostatic molecular interactions within the axoplasm will be reviewed. With this new approach, we can explain the different conductive patterns in unmyelinated and myelinated nerves. This new mathematical conductive model based on electrostatic compressional wave in the intracellular fluid may also be able to explain the signal integration in the neuronal cell body and the back-propagation mechanism from the axons to the dendrites. With this new mathematical nerve conduction model based on electrostatic molecular interactions within the intracellular fluid, we may be able to achieve an integrated explanation for the physiological phenomena taking place in the nervous system.

Effects of anions on the structural regulation of Zn‑salen‑modified metal‑organic cage

By virtue of a 3∶1 complementary coordination strategy,a chiral heteroleptic metal-organic cage that con-tains divergent functional units,Pd‑R(Zn),was precisely constructed via self-assembly of monodentate variational Zn-salen ligands RZn and NADH(reduced nicotinamide adenine dinucleotide)mimic modified tridentate ligands with square-planar Pd ions.UV-Vis and luminescence spectra experiments reveal that different anions could selec-tively interact with different sites of Zn-salen modified metal-organic cages to achieve the structural regulation of cage compound,by using the differentiated host-guest electrostatic interactions of counter ions with metal-organic hosts.Compared to other anions,the presence of chloride ions caused the most significant fluorescence emission enhancement of Pd‑R(Zn),meanwhile,the UV-Vis absorption band attributed to the salen aromatic backbone showed an absorption decrease,and the metal-to-ligand induced peak displayed a blue shift effect.Circular dichro-ism and ^(1)H NMR spectra further demonstrate that the introduction of chloride anions is beneficial to keeping a more rigid scaffold.

Electrostatic Interaction Tailored Anion-Rich Solvation Sheath Stabilizing High-Voltage Lithium Metal Batteries

Through tailoring interfacial chemistry,electrolyte engineering is a facile yet effective strategy for highperformance lithium(Li)metal batteries,where the solvation structure is critical for interfacial chemistry.Herein,the effect of electrostatic interaction on regulating an anion-rich solvation is firstly proposed.The moderate electrostatic interaction between anion and solvent promotes anion to enter the solvation sheath,inducing stable solid electrolyte interphase with fast Li+transport kinetics on the anode.This asdesigned electrolyte exhibits excellent compatibility with Li metal anode(a Li deposition/stripping Coulombic efficiency of 99.3%)and high-voltage LiCoO_(2) cathode.Consequently,the 50μm-thin Li||high-loading LiCoO_(2) cells achieve significantly improved cycling performance under stringent conditions of high voltage over 4.5 V,lean electrolyte,and wide temperature range(-20 to 60℃).This work inspires a groundbreaking strategy to manipulate the solvation structure through regulating the interactions of solvent and anion for highperformance Li metal batteries.

Defect passivation through electrostatic interaction for high performance flexible perovskite solar cells

The light weight,good bending resistance and low production cost make flexible perovskite solar cells(PSCs)good candidates in wearable electronics,portable charger,remote power,and flying objects.High power conversion efficiency(PCE)plays a crucial role on obtaining the high mass specific power of flexible devices.However,the performance for flexible PSCs is still having a large room to be improved.Here,we added the 2-amino-5-cyanopyridine(ACP)molecule with a polar electron density distribution in the perovskite precursor solution to improve the performance of flexible PSCs.The cyano groups with electron-withdrawing ability are expected to passivate positively charged point defects,while amines with electron donating ability are expected to passivate negatively charged point defects in perovskite films.Thanks to the effective passivation of defects at the grain boundary and surface of perovskite films,the PCE of flexible PSCs is obviously increased from 16.9%to 18.0%.These results provide a universal approach to improve performance of flexible PSCs by healing the defects in perovskite films through electrostatic interactions.

Characterization of Au/CdTe nanocomposites prepared by electrostatic interaction

Au/CdTe nanocomposites were prepared by electrostatic interaction between oppositely-charged gold （Au） and cadmium telluride （CdTe） nanoparticles. Au and CdTe nanoparticles were stabilized by 4-（dimethylamino）pyridine （DMAP） and 3-mercaptopropionic acid to develop positive and negative charges on their surfaces in aqueous solutions, respectively. The red shifts of the surface plasmon absorptions with the increase of Au content indicate that the sizes of the nanocomposites expanded due to the complex formation. Mixing ratio of Au and CdTe nanoparticles controls the structure of the resulting composites effectively. Moreover, the sizes and shapes of the mixed nanoparticles are important parameters for the formation of metal/semiconductor nanocomposites. The Au/CdTe nanocomposites were characterized by small angle X-ray scattering technique （SAXS）, transmission electron microscopy （TEM）, cyclic voltammetry （CV） and X-ray photoelectron spectroscopy （XPS）.

Electrostatic interaction of a spherical particle in the vicinity of a circular orifice

The electrostatic interaction of a charged spherical particle in the vicinity of an orifice plane has been investigated in this paper. The particle can creep along the axis of the orifice and is immersed in a bulk electrolyte. By solving the Poisson-Boltzmann problem, we have obtained the effective electrostatic interaction for several values of reduced orifice radius h, including the cases of h ~ 1, h = i and h 〈 1. Two kinds of boundary conditions of the orifice plane are considered. One is the constant potential model corresponding to a conducting plane, the other is the constant charge model. In the constant potential model, there is an electrostatic attraction between the particle and the orifice plane when they get close to each other, while there is a pure electrostatic repulsion in the constant charge model. The interactions in both boundary models are sensitive to the parameters of the reduced orifice radius, the reduced particle-rifice distance, surface charge densities of the particle and orifice plane, and the reduced Debye screen constant corresponding to the salt-ion concentration and ion valence.

ELECTROSTATIC INTERACTION HYBRIDS FROM WATER-BORNE CONDUCTIVE POLYANILINE AND INORGANIC PRECURSOR CONTAINING CARBOXYL GROUP

Electrostatic interaction conductive hybrids were prepared in water/ethanol solution by the sol-gel process from inorganic sol containing carboxyl group and water-borne conductive polyaniline （cPANI）. The electrostatic interaction hybrids film displayed 1-2 orders of magnitude higher electrical conductivity in comparison with common hybrids film, showing remarkable conductivity stability against water soaking. Most strikingly, it displayed ideal electrochemical activity even in a solution with pH = 14, which enlarged the conducting polyaniline application window to strong alkaline media.

Electrostatic interaction between a rod-like macromolecule and a circular orifice/disk in an electrolyte solution

We present the solutions of the interaction energy for a colloid system with a charged rod-like macromolecule immersed in a bulk electrolyte and moving along the axis of a circular orifice or disk （orifice/disk）. The calculation requires a numerical computation of the surface charge profiles, which result from a constant surface potential on the macromolecule and the orifice/disk. In the calculation, remarkable divergences of the surface charge emerge on the edges of the macromolecule and the orifice/disk, which are well-known edge effects. The anisotropic distribution of the surface charge （effective dipole） results in an attraction between these two charged objects. This attraction is enhanced with the increase of the screening length of the system for both the orifice and the disk systems. However, the sizes of the orifice and the disk reduce to different effects on the interaction energy.

Effect of ionic strength and mixing ratio on complex coacervation of soy protein isolate/Flammulina velutipes polysaccharide

Soy protein isolate(SPI)is a commercial protein with balanced amino acids,while the poor solubility impedes its use in traditional foods.To overcome the problem,the complex coacervation of SPI/Flammulina velutipes polysaccharide(FVP)were investigated.Initial results revealed that the suitable amounts of FVP contributed to reducing the turbidity of SPI solution.Under electrostatic interaction,the formation of SPI/FVP coacervates were spontaneous and went through a nucleation and growth process.Low salt concentration(C_(NaCl)=10,50 mmol/L)led to an increase in the critical pH values(pHc,pHφ1)while the critical pH values decreased when C_(NaCl)≥100 mmol/L.The concentration of NaCl ions increased the content ofα-helix.With the increase of FVP,the critical pH values decreased and the content ofβ-sheet increased through electrostatic interaction.At SPI/FVP ratio of 10:1 and 15:1,the complex coacervation of SPI/FVP were saturated,and the coacervates had the same storage modulus value.SPI/FVP coacervates exhibited solid-like properties and presented the strongest storage modulus at C_(NaCl)=50 mmol/L.The optimal pH,SPI/FVP ratio and NaCl concentration of complex coacervation were collected,and the coacervates demonstrated a valuable application potential to protect and deliver bioactives and food ingredients.

Fabrication of graphene oxide-keratin-chitosan nanocomposite as an adsorbent to remove turbidity from tannery wastewater

Excessive turbidity in water is aesthetically unappealing and severely malfunctions the photosynthesis process of aquatic ecosystems. This study aimed to evaluate the effectiveness of a nanocomposite adsorbent made of graphene oxide-keratin-chitosan for removing turbidity from tannery influent. The nanocomposite was fabricated with simple solution casting methods. Material dispersibility, bonding between composite materials (amide linkage), and the surface morphology of the nanocomposite were analyzed with the ultraviolet-visible spectroscopy, Fourier transform infrared spectroscopy, X-ray diffraction, transmission electron microscopy, and scanning electron microscopy. At pH of 6, 2 g/L of adsorbent and a 25-min contact time resulted in about 88% of turbidity elimination. After the adsorption process, the total suspended solids, total dissolved solids, salinity, biochemical oxygen demand, and chemical oxygen demand of the tannery wastewater were reduced by 55%, 29%, 12%, 58%, and 75%, respectively. The optimum dosage of the nanocomposite with the maximum turbidity removal capacity was 12.62 mg/g. According the adsorption kinetic and isotherm models, the graphene oxide-keratin-chitosan nanocomposite played a key role in the turbidity removal process with chemisorption and electrostatic multilayer adsorption. This study provided methodological and mechanistic insights into the procedures of investigating the removal of turbidity from tannery wastewater with a novel composite material.

Effect of carboxymethyl konjac glucomannan coating on curcumin-loaded multilayered emulsion:stability evaluation

The stability against various environmental stresses of the curcumin-loaded secondary and tertiary emulsions that was emulsified by whey protein isolate(WPI)and coated by chitosan(CHI),carboxymethyl konjac glucomannan(CMKGM),or their combination through layer-by-layer assembly was investigated.Generally,the multilayered emulsions were destabilized in high Na Cl concentrations or medium p H that could interrupt the electrostatic interaction between the three polyelectrolytes or deprotonate CHI,indicating that electrostatic interaction played an important role in the stability of emulsions.Compared with the primary emulsion that was solely stabilized by WPI,extra coating with CHI and CMKGM generally increased the stability of the emulsion against repeated freezing-thawing,improved the retention of curcumin against heating,UV irradiation,and long-term storage,and the effects were more remarkable in the tertiary emulsion with CMKGM locating in the outmost layer.Since CMKGM has shown the colon-targeted delivery potency,the multilayered emulsions assembled by layer-by-layer deposition,especially the tertiary emulsion,could be used as an effective carrier for the targeted delivery of curcumin.

Electrostatic interaction-mediated 1:1 complexes for high-contrast mitochondrial-targeted phosphorescence bioimaging

Organelle-targeted imaging can provide information on cellular functions and intracellular interactions,being significant for disease diagnosis.The use of room-temperature phosphorescence(RTP)in organelle-targeted imaging can fully utilize its unique characteristics of long wavelength and deep penetration.However,this technology has long been plagued by insufficient probe targeting and limited luminous intensity.In this work,we prepared a series of complexes composed of multicationic persulfurated arenes and biomacromolecules via electrostatic interactions in 1:1 stoichiometry for high-contrast mitochondrial-targeted RTP imaging.Such an electrostatic interaction design effectively prevented the self-aggregation of the probes,which is not conducive to mitochondrial targeting.Simultaneously,it suppressed the non-radiative decay to the maximum extent,enabling the probes to exhibit strong RTP signals both in aqueous solution and at the cellular level.Furthermore,the biomacromolecules can serve as carriers for an electrostatic interaction transfer of the persulfurated arenes to mitochondria.This leads to high mitochondrial targeting Pearson's correlation coefficients of the probes and high-contrast RTP imaging effects,as well as the independence of the co-incubated probe concentration.These results provide new insights for the development of targeted imaging technologies.

An innovative inertial parameters identification method for non-cooperative space targets based on electrostatic interaction

Inertial characteristics of non-cooperative targets are crucial for space capture and sub-sequent on-orbit servicing.Previous methods for identifying inertial parameters involve proximity operations,which are associated with the risk of collision with non-cooperative targets.This paper introduces a long-range,contactless method for identifying the inertial parameters of a non-cooperative target during the pre-capture phase.Specifically,electrostatic interaction is used as an external excitation to alter the target's motion.A force estimation algorithm that uses measure-ments from visual and potential sensors is proposed to estimate the electrostatic interaction and eliminate the need for force sensors.Furthermore,a recursive estimation-identification framework is presented to concurrently estimate the coupled motion state,weak electrostatic interaction,and inertial parameters of the target.The simulation results show that the proposed method extends the identification distance to 170 times that of the previous method while maintaining high identifica-tion precision forall parameters.

A novel aminated polymeric adsorbent for removing refractory dissolved organic matter from landfill leachate treatment plant

Refractory dissolved organic matter （DOM） from landfill leachate treatment plant was with high dissolved organic carbon （DOC） content. An aminated polymeric adsorbent NDA-8 with tertiary amino groups and sufficient mesopore was synthesized, which exhibited high adsorption capacity to the DOM （raw water after coagulation）. Resin NDA-8 performed better in the uptake of the DOM than resin DAX-8 and A100. Electrostatic attraction was considered as the decisive interaction between the adsorbent and adsorbate. Special attention was paid to the correlation between porous structure and adsorption capacity. The mesopore of NDA-8 played a crucial role during uptake of the DOM. In general, resin in chloride form performed a higher removal rate of DOC. According to the colunm adsorption test, total adsorption capacity of NDA-8 was calculated to 52.28 mg DOC/mL wet resin. 0.2 mol/L sodium hydroxide solution could regenerate the adsorbent efficiently.