Charge Movement Research Articles

Enhancing solar-driven hydrogen production through photoelectrochemical methods via dual transition metal doping of titanium oxide to form an impurity energy band

Developing a photoanode that is stable, efficient, and cost-effective for photoelectrochemical water splitting poses a significant challenge. To address this, we have successfully synthesized cobalt and chromium-doped Titanium dioxide (CoCrTiO2) using the hydrothermal method. This innovative approach results in an efficient, stable, and economical material. The introduction of Co and Cr through doping creates an intermediate band energy within TiO2, thereby enhancing charge separation and movement. The performance of CoCrTiO2 in the photoelectrochemical water splitting process is noteworthy. At 0 V vs Ag/AgCl, CoCrTiO2 exhibits a photocurrent density of 3.45 mAcm−2, representing an impressive 8.5 times increase compared to bare TiO2. Furthermore, when employed as a photoanode, CoCrTiO2 demonstrates a significant increase in hydrogen production. The amount of hydrogen generated is measured at 67.8 μmolecm−2, surpassing bare TiO2 by a factor of 5.6. Analysis data strongly supports CoCrTiO2 as an excellent candidate for advancing the field of photoelectrochemical water splitting due to its exceptional performance characteristics.

Membrane potential stimulates ADP import and ATP export by the mitochondrial ADP/ATP carrier due to its positively charged binding site.

The mitochondrial adenosine 5'-diphosphate (ADP)/adenosine 5'-triphosphate (ATP) carrier imports ADP into the mitochondrion and exports ATP to the cell. Here, we demonstrate that 3.3 positive charges are translocated with the negatively charged substrate in each transport step. They can be assigned to three positively charged residues of the central substrate-binding site and two asparagine/arginine pairs. In this way, the membrane potential stimulates not only the ATP4- export step, as a net -0.7 charge is transported, but also the ADP3- import step, as a net +0.3 charge is transported with the electric field. These positive charge movements also inhibit the import of ATP and export of ADP in the presence of a membrane potential, allowing these nucleotides to be maintained at high concentrations in the cytosol and mitochondrial matrix to drive the hydrolysis and synthesis of ATP, respectively. Thus, this is the mechanism by which the membrane potential drives adenine nucleotide exchange with high directional fluxes to fuel the cellular processes.

Mechanism exploration of ion-implanted epoxy on surface trap distribution: An approach to augment the vacuum flashover voltages

Abstract The augmentation of the epoxy (EP) resin surface to advance flashover performance has become a pivotal point of global interest. This research introduces a novel surface modification method and its mechanism for insulation materials. The research follows an electron cyclotron resonance ion implantation system to subject the surface of EP insulation to ion beams with diverse energies, i.e., 6, 10, 20, 40, 50, and 60 keV for a consistent time of 300 s at an angle of 90°. The experimental phase includes the DC flashover examination under negative polarity. Besides, the simulation phase includes the Monte Carlo model constructed using SRIM software to examine the range and distribution of bombarded ions in the targeted insulation. Results reveal that the flashover properties are affected by the surface potential, surface conductivity, trap distribution, water contact angle, and elemental composition. Likewise, based on the outcomes and theoretical point of view, it is revealed that the bombardment of energetic ions enhances the trap depth, assisting in a reduction in surface conductivity, confining the surface charge movements, and extensively suppressing the secondary electron emission yield. Also, the enhanced trap depth induces homo-charge formation near triple junctions. Synergistically, the factors contribute to high flashover voltages.

Effects of charge motion on knock and thermal efficiency under high load condition of a heavy-duty natural gas engine

Nowadays, the carbon-neutral trend and the crude oil crisis have brought natural gas into increasing focus. However, heavy-duty engines fueled by natural gas have been plagued by thermal efficiency and knocking limitation problems. Well-structured charge motions can enhance thermal efficiency and concurrently mitigate knock, however, there is a lack of comprehensive work involving charge motions. In this paper, numerical simulation is employed to investigate the impact of charge motion on knock and thermal efficiency under high load conditions for a heavy-duty spark-ignition natural gas engine. The findings indicate that in the configuration with intense swirl, the diminished turbulent kinetic energy (TKE) at the combustion chamber’s base lessens the convective heat exchange between the fresh charge and the heated exhaust gases, resulting in a noticeable high-temperature zone and triggering hot spots. In configurations with inclined swirl and strong tumble motion, the extensive tumble motion near the spark plug region close to top dead center leads to an asymmetric flame front shape, determining the location of hotspots. The research also revealed that excessive tumbling motion and TKE can increase the likelihood of engine knock, while appropriate cylinder charge motion can improve the knock resistance of the engine to some extent, the maximum reduction in knocking intensity can reach 92.5%. The optimized combustion systems can significantly improve the initial combustion rate, shorten the ignition delay period, and advance the combustion center. With the combined effects of ignition timing and charge motion, the total indicated specific power per unit of fuel mass is increased in the optimized systems. Compared to the original combustion system, the indicated thermal efficiency within the knocking boundary can be improved by 1.11%.

Electron Migratory Polarization of Interfacial Electric Fields Facilitates Efficient Microwave Absorption

AbstractHigh‐performance microwave absorption materials (MAM) are often accompanied by synergistic effects of multiple loss mechanisms, but the contribution share of various loss mechanisms has been neglected to provide a template and reference for the design of MAM. Here, a highly conductive 2D structure is designed through a functional group‐induced structure modulation strategy, composite L‐Ni@C can reach an effective absorption bandwidth of 6.45 GHz at 15% fill rate, with a maximum absorption efficiency of 99.9999%. Through the layer‐by‐layer analysis of the loss mechanism, it is found that the strong loss originates from the polarization loss at the heterogeneous interface. The movement of space charge between the two‐phase interface forms an interfacial electric field, and the in situ doping of nitrogen is cleverly achieved by the introduction of amino functional groups, which significantly enhances the rate of space charge transfer between the two‐phase interface and greatly facilitates the electron migration polarization. The space charge motion law of the interfacial electric field is also simulated using COMSOL simulation software to illustrate the electron migration polarization mechanism at heterogeneous interfaces. This work fills the gap of functional group‐induced structural modulation and presents new theories into the mechanism of space charge movement at heterogeneous interfaces.

Effect of transition metal ions on the dielectric properties of chromium potassium phosphates

Potassium ions are important for developing electrode materials because they have similar properties to lithium and sodium ions. Mixed chromium phosphates (KMIICr(PO4)2) with substituted MII sites using divalent elements (M = Ni, Co, Cu) were synthesized using a solid-state reaction method. The samples were analyzed using various techniques such as powder X-ray diffraction, Fourier transform infrared, Raman, and electron paramagnetic resonance spectroscopy. The proposed phosphates had a monoclinic phase structure with a P21/n space group, and they contained large tunnels occupied by K+ cations. The dielectric properties showed that the Ni-based phosphates had slower dielectric relaxation, while the Co and Cu-based phosphates had quicker polarization and depolarization processes. Additionally, the resistance of the grains decreased from Ni to Co to Cu-based phosphates, indicating easier charge movement in each material, consistent with the increase in conductive losses and a.c. conductivity when changing the MII ions.

ZnSnS Nanoparticles Synthesized by Simple SMI Technique for Photocatalytic Application

Photocatalysis, driven by semiconductor nanoparticles under visible or ultraviolet light, has emerged as a powerful and sustainable approach for environmental remediation and clean energy production. In this study, we investigate the photocatalytic potential of tin (0, 2, 4, 6, 8, 10) mole % alloyed with zinc sulfide (ZnSnS) nanoparticles as efficient catalysts for various environment and energy-related applications. ZnSnS nanoparticles were produced via a simple microwave irradiation technique. Comprehensive structural characterization through X-ray diffraction (XRD), FESEM, EDAX and HRTEM confirmed the successful incorporation of tin atoms into the ZnS crystal lattice. Optical study indicated significant blue shifts in the absorption edge, extending the light absorption into the visible region, a key advantage for photocatalytic applications. Photocatalytic experiments were conducted to evaluate the performance of Zn-alloyed SnS nanoparticles in degrading organic pollutants and hydrogen evolution from water splitting reactions. Our results revealed remarkable enhancements in photocatalytic activity. The enhanced efficiency can be credited to the creation of fresh energy levels within the bandgap, aiding in the separation and movement of charges, and also to the heightened light absorption caused by the reduced bandgap. Furthermore, stability tests indicated the durability of (ZnSnS) nanoparticles, making them suitable candidates for long-term applications in real-world environments. The observed photocatalytic activity enhancements hold promise for addressing environmental issues, including wastewater treatment, air purification, and hydrogen production for clean energy.

Completely Multipolar Model as a General Framework for Many-Body Interactions as Illustrated for Water.

We introduce a general framework for many-body force fields, the Completely Multipolar Model (CMM), that utilizes multipolar electrical moments modulated by exponential decay of electron density as a common functional form for all terms of an energy decomposition analysis of intermolecular interactions. With this common functional form, the CMM model establishes well-formulated damped tensors that reach the correct asymptotes at both long- and short-range while formally ensuring no short-range catastrophes. CMM describes the separable EDA terms of dispersion, exchange polarization, and Pauli repulsion with short-ranged anisotropy, polarization as intramolecular charge fluctuations and induced dipoles, while charge transfer describes explicit movement of charge between molecules, and naturally describes many-body charge transfer by coupling into the polarization equations. We also utilize a new one-body potential that accounts for intramolecular polarization by including an electric field-dependent correction to the Morse potential to ensure that CMM reproduces all physically relevant monomer properties including the dipole moment, molecular polarizability, and dipole and polarizability derivatives. The quality of CMM is illustrated through agreement of individual terms of the EDA and excellent extrapolation to energies and geometries of an extensive validation set of water cluster data.

Preparation of porous composite coatings to suppress surface charge movement and reduce electrical resistivity

In this work, Cr2O3/TiO2 composite coatings were prepared on α-Al2O3 insulating ceramic matrix surface by screen printing and solid phase sintering methods to yield an average film thickness of about 14.10 μm. Scanning electron microscopy (SEM) revealed changes in the pore structures of the coatings at different TiO2 contents. The atomic force microscopy (AFM) analysis of the coating surface roughness suggested a TiO2 content of 0.025 mol to yield the best surface roughness and pore structure of the coating. The calculation showed an increase in the energy level of the deep trap center on the surface from 1.506 eV to 1.547 eV, reaching a maximum. The surface resistivity of insulating ceramics decreased from 1016 Ω to 1012 Ω. The formation of deep surface traps and the decrease in surface resistivity promoted charge dispersion and suppressed the formation of flashover channels, effectively improving the surface flashover voltage of the ceramics.

Surface-Integrating Oxygen Vacancy and CuxO Nanodots Enabling Synergistic Electric Field and Dual Catalytic Sites Boosting CO2 Photoreduction.

High carrier separation efficiency and rapid surface catalytic reaction are crucial for enhancing catalytic CO2 photoreduction reaction. Herein, integrated surface decoration strategy with oxygen vacancies (Ov) and anchoring CuxO (1 < x < 2) nanodots below 10nm is realized on Bi2MoO6 for promoting CO2 photoreduction performance. The charge interaction between Ov and anchored CuxO enables the formation of enhanced internal electric field, which provides a strong driving force for accelerating the separation of photocharge carriers on the surface of Bi2MoO6 (ηsurf ≈71%). They can also cooperatively reduce the surface work function of Bi2MoO6, facilitating the migration of carrier to the surface. Meanwhile, surface-integrated Ov and CuxO nanodots allowing dual catalytic sites strengthens the adsorption and activation CO2 into *CO2 over Bi2MoO6, considerably boosting the progression of CO2 conversion process. In the absence of co-catalyst or sacrificial agent, Bi2MoO6 with Ov and CuxO nanodots achieves a photocatalytic CO generation rate of 12.75µmol g-1 h-1, a remarkable increase of over ≈15 times that of the original counterpart. This work provides a new idea for governing charge movement behaviors and catalytic reaction thermodynamics on the basis of synergistic improvement of electric field and active sites by coupling of the internal defects and external species.

Stability of a point charge for the repulsive Vlasov–Poisson system

We consider solutions of the repulsive Vlasov–Poisson system which are a combination of a point charge and a small gas, i.e., measures of the form \delta_{(\mathcal{X}(t),\mathcal{V}(t))}+\mu^{2}d\mathbf{x}d\mathbf{v} for some (\mathcal{X}, \mathcal{V})\colon \mathbb{R}\to\mathbb{R}^{6} and a small gas distribution \mu\colon \mathbb{R}\to L^{2}_{\mathbf{x},\mathbf{v}} , and study asymptotic dynamics in the associated initial value problem. If initially suitable moments on \mu_{0}=\mu(t=0) are small, we obtain a global solution of the above form, and the electric field generated by the gas distribution \mu decays at an almost optimal rate. Assuming in addition boundedness of suitable derivatives of \mu_{0} , the electric field decays at an optimal rate, and we derive modified scattering dynamics for the motion of the point charge and the gas distribution. Our proof makes crucial use of the Hamiltonian structure. The linearized system is transport by the Kepler ODE, which we integrate exactly through an asymptotic action-angle transformation. Thanks to a precise understanding of the associated kinematics, moment and derivative control is achieved via a bootstrap analysis that relies on the decay of the electric field associated to \mu . The asymptotic behavior can then be deduced from the properties of Poisson brackets in asymptotic action coordinates.

Improving the suppression of charge movement by porous chromium oxide coating

A chromium trioxide coating was prepared on the surface of electronic ceramics by screen printing, and solid-phase sintering was carried out at 1350 °C. The surface roughness and surface resistance characteristics of composite coatings with different chromium trioxide contents were studied. The analysis results indicate that the average thickness of Cr2O3 coating is about 19.89 μm. The main crystal phase is (Al0.9Cr0.1)2O3. SEM shows that the surface "pores" and surface roughness of the coating change with the content of Cr2O3. AFM shows that when the Cr2O3 content in the coating is 0.0921 mol, the surface roughness changes the most, and the corresponding surface resistivity of Al2O3 insulating ceramics decreases to the lowest, from 1016 Ω to 1012 Ω. An increase in surface roughness can lead to changes in the incidence angle of electrons, reducing the probability of electron surface collision. The lower the surface resistivity, the better the high-voltage breakdown resistance of vacuum ceramic devices, thereby improving the surface flashover performance of ceramics.

Dissecting the charge movements during adenine nucleotide exchange by mitochondrial ADP/ATP carrier

Dissecting the charge movements during adenine nucleotide exchange by mitochondrial ADP/ATP carrier

Improved high temperature energy storage density and efficiency of polyimide nanocomposites via hindering charge and molecular motions

Electric vehicles and renewable energy consumption have huge demands for high-performance polymer dielectric capacitors. However, the resistivity and breakdown strength of existing polymer dielectrics deteriorate significantly at high temperatures, reducing the energy storage density and charge-discharge efficiency of capacitors below service requirements. The charge transport and molecular chain motion characteristics in linear polymers determine their conductivity, breakdown, and energy storage properties, but the quantitative relationship between them is not clear. An in-situ polymerization method was used to prepare polyimide/Al2O3 nanocomposites (PI/Al2O3 PNCs). Experimental results show that the resistivity, breakdown strength, energy storage density, and charge-discharge efficiency of PNCs increase initially and then decrease with increasing doping content, peaking at 3 wt%. The discharged energy density of PI/Al2O3-3 wt% PNCs at 180°C is 207.52 % higher than pure PI. A conductance-breakdown-energy storage co-simulation model based on charge transport and molecular chain displacement was used to simulate the voltage-current, breakdown, and energy storage characteristics of PNCs. The simulation results are consistent with the experiments. Comparative studies between simulation and experiments show that the independent interface zone between nanofillers and PI hinders charge transport and molecular chain movement, reducing electric field distortion and molecular chain spacing, thereby improving high-temperature breakdown and energy storage performance of PNCs.

Role of charge injection/de-trapping in imprint behavior of ferroelectric Hf0.5Zr0.5O2 thin film

Ferroelectric HfO2-based thin films have attracted increasing interest due to their potential applications in nonvolatile memory areas. However, their unique properties, such as imprint, lead to serious reliability issues. In this study, the origin of imprint behavior is investigated by using TiN/Hf0.5Zr0.5O2 (10 nm)/TiN MFM capacitors. By modulating the internal electric field during imprint, we discover that charge injection/de-trapping in metal–ferroelectric interfaces plays an essential role in imprint behavior rather than charge movement inside the FE layer. The asymmetric shift of the coercive field is also discussed, which is attributed to nonlinear interaction between polarization's bound charges and the electrode's screening charges. This suggests that controlling interface quality should effectively suppress imprint in HfO2-based thin films.

Metallophthalocyanines as Outstanding Hole Transporting Materials in Perovskite Solar Cells

Perovskite solar cells (PSCs) are promising candidates to reach the market to complement the current offer of photovoltaic cells although for such a thing they still have to overcome some challenges such as long-term stability. The hole transporting layer (HTL) is a crucial component in n-i-p PSC, since it must favor an adequate movement of charges and protect the perovskite layer from environmental conditions. In this sense, the commonly used HTL, spiro-OMeTAD, does not provide PSCs with sufficient stability and is too expensive. Cheaper molecular materials such as metallophthalocyanines are proving to be a good alternative, as they provide greater stability.[1]In this communication, we will present novel ZnPcs and CuPcs monomers[2] (see as examples Figure 1), among others, as efficient, stable, and low cost HTMs in PSCs. The MPcs are substituted with functional groups that possesses a very good solubility in a wide range of organic solvents, adequate HOMO LUMO levels and their photovoltaics performance as high stable solution processing in a wide range of perovskite solar cell devices.

Integrating Electrochemical Analysis and Machine Learning for Enhanced Discovery of Conductive MOFs: A Database-Driven Approach

Metal-organic frameworks (MOFs) are highly versatile structures composed of metal ions linked by organic molecules. They offer a broad range of applications in electronics and light-based technologies due to their flexibility. However, the connection between metal ions and organic components often hinders efficient charge movement, which is essential for electrical conduction. To address this challenge, researchers have been innovatively designing MOFs to enhance their conductivity, which is typically low. This process is complex and time-consuming. To overcome these barriers, and to save both time and costs, we integrated machine learning (ML) with electrochemical testing. Our aim was to pinpoint ion and electron conductive MOFs from the Computation-Ready, Experimental Metal–Organic Framework (CoREMOF) Database, which contains over 14,000 MOFs. The ML approach predicted 84 intrinsically conductive MOFs, which were then subjected to rigorous experimental validation through synthesis and conductivity performance testing. Further experimental data confirmed that only two conductive MOFs, containing copper and pyrazole structures with carbonyl groups, exhibited both proton and electron conductivity. The differences between them lie solely in the preparation techniques and solvents used. Sample 1 was prepared using hydrothermal methods and alcohol as the solvent, and NH4@1 was prepared with an ammonium solution at room temperature. To understand deeper their intrinsic conductivity and semiconductor properties, we employed temperature-dependent conductivity and electrochemical measurements, including Cyclic Voltammetry (CV), Electrochemical Impedance Spectroscopy (EIS), Linear Sweep Voltammetry (I-V), and Mott-Schottky analysis. The EIS data showed a smaller semicircular arc for synthesized NH4@1, indicating its lower charge transfer resistance due to the presence of two different positive charge carriers on its surface. We investigated the effect of increasing positive charge carriers by raising the humidity up to 98% RH. EIS data showed that increasing positive charge has a significantly reduced charge transfer resistance of sample 1 compared to NH4@1. Because NH4@1 consists of ammonium and H3O+ simultaneously, causing saturation of positive charges and increasing charge transfer resistance. Mott-Schottky analysis further elucidated the electrical properties of compounds 1 and NH4@1, revealing their p-type behavior with negative slopes and flat band potentials of 0.61 V and 0.9 V, respectively. The CV analysis of pyrazole carboxylic acid in a 0.1 M KOH solution, using three reference electrodes, revealed reduction and oxidation peaks vs. Ag/AgCl. These peaks highlight the redox behavior of the linker, generating a stable carboxylate anion (-COO−) that facilitates charge hopping. This reversible redox activity is crucial for the charge transport mechanism within the MOFs. CV analyses confirmed the presence of different copper oxidation states in both compounds, with cathodic peaks indicating the reduction from Cu(II) to Cu(I), suggesting active charge transfer. Extensive electrochemical studies, encompassing both Mott-Schottky and EIS analyses, provided deeper insights into charge carriers and transfer resistance, areas not extensively explored in previous research on intrinsically conductive MOFs. Our results underscore the critical role of experimental validation of ML predictions in accelerating the discovery and characterization of conductive MOFs for potential applications in batteries.

Itaconic anhydride functionalized cyanoethyl cellulose with crosslinked structure enabled improved dielectric properties

AbstractAs a type of cellulose ether, cyanoethyl cellulose (CEC) is considered to be a promising candidate for polymer dielectrics due to its sustainable nature and high dielectric constant induced by the cyano groups. However, the relatively high conduction loss of CEC arising from the charge motion across the polymer degrades its dielectric properties. In this work, we designed and synthesized an all‐organic polymer composite of CEC/itaconic anhydride (ITA) to improve dielectric properties. The CEC matrix was graft functionalized by ITA via an esterification reaction between the anhydride groups of ITA and hydroxyl groups of CEC. Meanwhile, crosslinking structure was also established in the composite by the generation of diester. Significantly improved dielectric constant (εr), elevated breakdown strength (Eb), restrained dielectric loss (tan δ) and decreased conductivity (σ) were observed in the composites compared with unmodified CEC. The εr increased from 17 for pure CEC to 32 for CEC/ITA at 1 kHz, and Eb also soared from 145 MV m−1 for CEC to 226 MV m−1 for the composite. The tan δ reduced from 0.24 for pure CEC to about 0.05 for the composite at 100 Hz. This should be attributed to the molecule trapping centers arising from the high electron affinity ITA and the formation of crosslinked networks as well as hydrogen bonding, which impeded the electric conduction. It also provided additional advantages of better dielectric properties for the CEC/ITA composites than pure CEC at high temperatures, which may offer inspiration for the design and preparation of bio‐based dielectrics for high temperatures. © 2024 Society of Chemical Industry.

Hollow g-C3N4@Ag3PO4 Core-Shell Nanoreactor Loaded with Au Nanoparticles: Boosting Photothermal Catalysis in Confined Space.

Low solar energy utilization efficiency and serious charge recombination remain major challenges for photocatalytic systems. Herein, a hollow core-shell Au/g-C3N4@Ag3PO4 photothermal nanoreactor is successfully prepared by a two-step deposition method. Benefit from efficient spectral utilization and fast charge separation induced by the unique hollow core-shell heterostructure, the H2 evolution rate of Au/g-C3N4@Ag3PO4 is 16.9 times that of the pristine g-C3N4, and the degradation efficiency of tetracycline is increased by 88.1%. The enhanced catalytic performance can be attributed to the ordered charge movement on the hollow core-shell structure and a local high-temperature environment, which effectively accelerates the carrier separation and chemical reaction kinetics. This work highlights the important role of the space confinement effect in photothermal catalysis and provides a promising strategy for the development of the next generation of highly efficient photothermal catalysts.

Single crystal, conformational, quantum reactivity, hirshfeld surface, molecular interactions, ADMET, and molecular docking investigations on HIV-1 site of 3-isopropyldiphenyl-1-(2-(thiophen-2yl)acetyl)piperidin-4-one

The 3-isopropyl-2,6-diphenyl-1-(2-(thiophen-2yl)acetyl)piperidin-4-one (IPTP) single crystals were grown by slow evaporation method and the structure is confirmed through FT-IR, 1H NMR, and 13C NMR spectral analyses. Single crystal X-ray diffraction revealed that the title compound having chair conformation of the piperidine ring, with an axial orientation of phenyl rings at C-2 and C-6 positions and an isopropyl group at C-3. Hirshfeld surface analysis was employed to examine intermolecular contacts and strong and weak attractive, repulsive, and van der Waals interactions in the molecule were determined using the reduced density gradient method (RDG). The geometrical parameters obtained through Density Functional Theory are compared with experimental values and also conducted to optimize structural parameters, frontier molecular orbitals (FMOs), and molecular electrostatic potential surface analysis (MEPS). NBO calculations were employed to investigate intermolecular and intramolecular charge movement, as well as the molecule's stability. Vibrational Energy Distribution Analysis (VEDA) software facilitated potential energy decomposition (PED) analysis using FT-IR wave numbers. The title compound molecular docking data were compared with the markedly available FDA-approved anti-HIV drug of Nelfinavir and their results were discussed, ADME analysis studies were discussed concerning FDA-approved anti-HIV drugs, including Nelfinavir, Betulinic Acid, Haloperidol, and Donepezil.