Realizing Outstanding Energy Storage Performance in KBT-Based Lead-Free Ceramics via Suppressing Space Charge Accumulation.

The great potential of K1/2Bi1/2TiO3 (KBT) for dielectric energy storage ceramics is impeded by its low dielectric breakdown strength, thereby limiting its utilization of high polarization. This study develops a novel composition, 0.83KBT-0.095Na1/2Bi1/2ZrO3-0.075 Bi0.85Nd0.15FeO3 (KNBNTF) ceramics, demonstrating outstanding energy storage performance under high electric fields up to 425 kV cm-1: a remarkable recoverable energy density of 7.03 J cm-3, and a high efficiency of 86.0%. The analysis reveals that the superior dielectric breakdown resistance arises from effective mitigation of space charge accumulation at the interface, influenced by differential dielectric and conductance behaviors between grains and grain boundaries. Electric impedance spectra confirm the significant suppression of space charge accumulation in KNBNTF, attributable to the co-introduction of Na1/2Bi1/2ZrO3 and Bi0.85Nd0.15FeO3. Phase-field simulations reveal the emergence of a trans-granular breakdown mode in KNBNTF resulting from the mitigated interfacial polarization, impeding breakdown propagation and increasing dielectric breakdown resistance. Furthermore, KNBNTF exhibits a complex local polarization and enhances the relaxor features, facilitating high field-induced polarization and establishing favorable conditions for exceptional energy storage performance. Therefore, the proposed strategy is a promising design pathway for tailoring dielectric ceramics in energy storage applications.

Time-Resolved Mechanistic Depiction of Photoinduced CO2 Reduction Catalysis on a Urea-Modified Iron Porphyrin.

The development of functional artificial photosynthetic devices relies on the understanding of mechanistic aspects involved in specialized photocatalysts. Modified iron porphyrins have long been explored as efficient catalysts for the light-induced reduction of carbon dioxide (CO2) towards solar fuels. In spite of the advancements in homogeneous catalysis, the development of the next generation of catalysts requires a complete understanding of the fundamental photoinduced processes taking place prior to and after activation of the substrate by the catalyst. In this work, we employ a state-of-the-art nanosecond optical transient absorption spectroscopic setup with a double excitation capability to induce charge accumulation and trigger the reduction of CO2 to carbon monoxide (CO). Our biomimetic system is composed of a urea-modified iron(III) tetraphenylporphyrin (UrFeIII) catalyst, the prototypical [Ru(bpy)3]2+ (bpy=2,2'-bipyridine) used as a photosensitizer, and sodium ascorbate as an electron donor. Under inert atmosphere, we show that two electrons can be successively accumulated on the catalyst as the fates of the photogenerated UrFeII and UrFeI reduced species are tracked. In the presence of CO2, the catalytic cycle is kick-started providing further evidence on CO2 activation by the UrFe catalyst in its formal FeI oxidation state.

Light-Induced Charge Separation in Covalently Linked BODIPY-Quinone-Alkyne Dyads.

Visible light-induced charge separation and directional charge transfer are cornerstones for artificial photosynthesis and the generation of solar fuels. Here, we report synthetic access to a series of noble metal-free donor-acceptor dyads based on bodipy light-absorbers and redox-active quinone/anthraquinone charge storage sites. Peripheral functionalization of the quinone/anthraquinone units with alkynes primes the dyads for integration into a range of light-harvesting systems, e. g., by Cu-catalyzed cycloadditions (CLICK chemistry) or Pd-catalyzed C-C cross-coupling reactions. Initial photophysical, electrochemical and theoretical analyses reveal the principal processes during the light-induced charge separation in the reported dyads.

Additive Manufacturing for Terahertz Metamaterials on the Dielectric Surface based on Optimized Electrohydrodynamic Drop-on-demand Printing Technology.

The conventional techniques used to fabricate terahertz metamaterials, such as photolithography and etching, face hindrances in the form of high costs, lengthy processing cycles, and environmental pollution. In contrast, electrohydrodynamic (EHD) drop-on-demand (DOD) printing technology holds promise as an additive manufacturing method capable of producing micrometer- and nanometer-scale patterns rapidly and cost-effectively. However, achieving stable large-area printing proves challenging due to issues related to charge accumulation in insulated substrates and inconsistent meniscus vibration. In this paper, a smooth bipolar waveform driving method is proposed aimed at solving the problems of charge accumulation on insulated substrates and poor print consistency. The method involves utilizing driving waveforms with opposite polarities for neighboring droplets, allowing the charges carried by the printed droplets to neutralize each other. Moreover, extending the duration of the high voltage rise and fall times enhances the consistency of meniscus motion, thereby improving the stability of printing. Through optimization of the printing parameters, droplets with a diameter of 1.37 µm and straight lines with a width of 3 µm were printed. Furthermore, this approach was employed to print terahertz metamaterial surface devices, and the performance of the metamaterial is in good agreement with the simulation results. These findings demonstrate that the method greatly improves the stability of EHD DOD printing, thereby advancing the application of the technology in additive processing at the micro- and nanoscale.

Magnetocapacitance at the Ni/BiInO3 Schottky Interface.

We report the observation of a magnetocapacitance effect at the interface between Ni and epitaxial nonpolar BiInO3 thin films at room temperature. A detailed surface study using X-ray photoelectron spectroscopy (XPS) reveals the formation of an intermetallic Ni-Bi alloy at the Ni/BiInO3 interface and a shift in the Bi 4f and In 3d core levels to higher binding energies with increasing Ni thickness. The latter infers band bending in BiInO3, corresponding to the formation of a p-type Schottky barrier. The current-voltage characteristics of the Ni/BiInO3/(Ba,Sr)RuO3/NdScO3(110) heterostructure show a significant dependence on the applied magnetic field and voltage cycling, which can be attributed to voltage-controlled band bending and spin-polarized charge accumulation in the vicinity of the Ni/BiInO3 interface. The magnetocapacitance effect can be realized at room temperature without involving multiferroic materials.

Ionic Liquid Modified Polymer Intermediate Layer for Improved Charge Extraction toward Efficient and Stable Perovskite/Silicon Tandem Solar Cells.

Monolithic perovskite/silicon tandem solar cells have been attracted much attention in recent years. Despite their high performances, the stability issue of perovskite-based devices is recognized as one of the key challenges to realize industrial application. When comes to the perovskite top subcell, the interface between perovskite and electron transporting layers (usually C60) significantly affects the device efficiency as well as the stability due to their poor adhesion. Here, different from the conventional interfacial passivation using metal fluorides, a hybrid intermediate layer is proposed-PMMA functionalized with ionic liquid (IL)-is introduced at the perovskite/C60 interface. The application of PMMA essentially improves the interfacial stability due to its strong hydrophobicity, while adding IL relieves the charge accumulation between PMMA and the perovskite. Thus, an optimal wide-bandgap perovskite solar cells achieves power conversion efficiency of 20.62%. These cells are further integrated as top subcells with silicon bottom cells in a monolithic tandem structure, presenting an optimized PCE up to 27.51%. More importantly, such monolithic perovskite/silicon cells exhibit superior stability by maintaining 90% of initial efficiency after 1200 h under continuous illumination.

Investigation of the Charge Accumulation Based on Stiffness Variation of the Micro-Shell Resonator Gyroscope.

In capacitive microelectromechanical system (MEMS) devices, the application of dielectric materials causes long-term charging problems in the dielectric layers or substrates, which especially affect the repeatability and stability of high-performance devices. Due to the difficulties of observation and characterization of charge accumulation, an accurate characterization method is needed to study the effect of charge and propose suppression methods. In this paper, we analyze the influence of charge accumulation on the MSRG and propose a characterization method for charge accumulation based on stiffness variation. Experiments are carried out to characterize the charge accumulation in MSRG, and the effect of temperature on the process is also investigated. In the experiment, the charge accumulation is characterized accurately by the variation of the frequency split and stiffness axes. Furthermore, the acceleration of the charge accumulation is observed at high temperatures, as is the higher additional voltage from the charge accumulation.

High-Precision Inertial Sensor Charge Management Based on Ultraviolet Discharge: A Comprehensive Review.

The charge accumulation caused by cosmic rays and solar energetic particles poses a significant challenge as a source of noise for inertial sensors used in space gravitational wave detection. To address this issue, the implementation of charge management systems based on ultraviolet discharge becomes crucial. This paper focuses on elucidating the principles and methods of using ultraviolet discharge for charge management in high-precision inertial sensors. Furthermore, it presents the design and implementation of relevant payloads. Through an analysis of the charge accumulation effect and its impact on noise, key considerations regarding coatings, light sources, and optical paths are explored, and some current and valuable insights into the future development of charge management systems are also summarized. The conclusions drawn from this research also provide guidance for the advancement of higher precision ultraviolet discharge technology and the design of charge management systems.

The Time, Electric Field, and Temperature Dependence of Charging and Discharging Currents in Polypropylene Films.

The insulating properties of polypropylene (PP) film play a very important role in the operating status of direct current (DC) support capacitors. Charging and discharging currents in PP film under high DC electric fields and temperatures correspond to charge transportation and accumulation, which significantly influence the electrical insulating properties of PP. In this paper, we have comprehensively studied the dependence of charging/discharging currents in PP film on time, electric field (150-670 kV/mm), and temperature (40-120 °C). The results showed that the charging current increased by almost an order of magnitude from 150 kV/mm to 670 kV/mm and exhibits a steep increase with temperature above 80 °C. The discharging currents are about 10 times less than the corresponding charging currents. Carrier mobility varies little with the electric field and becomes slightly larger with an increase in temperature. The quantity of the accumulated charges was calculated by the integral of the charging and discharging current differentials and showed a significant increase with the electric field and temperature. The corresponding electric field distortion becomes larger above 80 °C compared to 20-60 °C. Both electric field and temperature have an important effect on PP film and capacitors based on charge transport and accumulation and their electric field distortion. This study is innovative in that it combines the operating status of DC support capacitors with traditional methods to research synthetically charged transport mechanisms of PP film. The findings are meaningful for understanding the insulation failure mechanisms of PP film and capacitors under complex stresses.

Amplified Performance of Charge Accumulation and Trapping Induced by Enhancing the Dielectric Constant via the Cyano Group of 3D-Structured Textile for a Triboelectric Multi-Modal Sensor.

To further improve the output performance of triboelectric devices, reducing charge attenuation and loss has become a hot research topic. Particularly, textiles have emerged as one of the promising research directions for triboelectric devices owing to their special internal structure and large specific surface area. In the present work, polyacrylonitrile fibers are fabricated with two distinct structures to provide a higher dielectric constant due to the strong polar properties brought about by higher dipole moment of the CN group. In addition, the complex and closely connected structure of the textile increases specific internal surface area. As a friction layer, the output voltage is shown to increase to 625% of the initial value (from 8 to 60 V) after the application of friction for a short time due to accumulation property. When acting as a trapping layer, the charge loss after injection is effectively prevented due to excellent charge trapping effect. After 24 h, the triboelectric output performance remains at ≈70% of the initial value (decreasing from 320 to 220 V), which is more than 20 times that of the polytetrafluoroethylene film, which decreases from 125 to 19 V. The device is realized for the advanced application of multi-modal sensors.

Charge Concentration Limits the Hydrogen Evolution Rate in Organic Nanoparticle Photocatalysts.

Time-resolved microwave conductivity is used to compare aqueous-soluble organic nanoparticle photocatalysts and bulk thin films composed of the same mixture of semiconducting polymer and non-fullerene acceptor molecule and the relationship between composition, interfacial surface area, charge-carrier dynamics, and photocatalytic activity is examined. The rate of hydrogen evolution reaction by nanoparticles composed of various donor:acceptor blend ratio compositions is quantitatively measured, and it is found that the most active blend ratio displays a hydrogen quantum yield of 0.83% per photon. Moreover, it is found that nanoparticle photocatalytic activity corresponds directly to charge generation, and that nanoparticles have 3× more long-lived accumulated charges relative to bulk samples of the same material composition. These results suggest that, under the current reaction conditions, with ≈3× solar flux, catalytic activity by the nanoparticles is limited by the concentration of electrons and holes in operando and not a finite number of active surface sites or the catalytic rate at the interface. This provides a clear design goal for the next generation of efficient photocatalytic nanoparticles.

Spatial Control of the Hole Accumulation Zone for Hole-Dominated Perovskite Light-Emitting Diodes by Inserting a CsAc Layer.

Perovskites show efficient electroluminescence and are expected to have wide applications in light-emitting diodes (LEDs). However, owing to the unbalanced electron-hole transport properties of some highly luminescent perovskites, a fundamental challenge is that the exciton recombination zone of perovskite LEDs (PeLEDs) typically overlaps with an accumulation of the major carrier. It is known to reduce the performances of PeLEDs, leading to a reduction of efficiency and operation stability due to Auger recombination. To address this issue in a hole-dominated blue PeLED, we propose to insert a cesium acetate (CsAc) layer between the hole transport layer (HTL) and the hole-dominant perovskite layer. Electronic properties indicate that the hole accumulation zone of the device with the CsAc layer shifts away from the perovskite/ETL interface, i.e., the recombination zone, to the HTL/CsAc interface. Separation of the hole accumulation region and the exciton recombination zones substantially suppresses exciton quenching. Moreover, the CsAc layer can also improve the photophysical properties of the perovskite film by providing an extra Cs source to interact with the defect site of unreacted PbBr2 in the perovskite film and enhance the crystallinity of the perovskite with an enlarged crystal grain size. As a result, the external quantum efficiency (EQE) of the sky-blue PeLEDs shows considerable improvement from 5.3 to 9.2% upon inserting the CsAc layer.

Ferromagnetic-Based Charge-Accumulation Triboelectric Nanogenerator With Ultrahigh Surface Charge Density.

An encouraging micro-energy harvesting technology, the triboelectric nanogenerator (TENG), has been proven to transfer ambient environmental micro-energy into electricity, but a low surface charge density results in low performance and limits the practical application of TENG. Here, a ferromagnetic-based charge-accumulation TENG (FC-TENG) is proposed with ultrahigh surface charge density and performances. The FC-TENG introduces a ferromagnetic media to enhance the output charge by magnetization effect. Meanwhile, the charge can also be continuously accumulated by the charge pump effects. Based on these two effects, an ultra-high surface charge density of 2.85 mC m-2 is obtained under ambient atmospheric conditions using an ultra-thin PET film (3 µm) and deposited Permalloy ferromagnetic electrodes. Meanwhile, the surface charge density of the FC-TENG can always maintain more than 1.5 mC m-2 , even if the relative humidity arrives at 90%. This work provides a prospective technical mode to enhance the surface charge density of TENG, which would shed a new insight and guidance on the high-performance TENG for various environmental conditions such as the ocean, industrial manufacturing, aerospace, and rail traffic.

Study on the Method of Charge Accumulation Suppression of Electrostatic Suspended Accelerometer.

Electrostatic suspended accelerometers (ESAs) are widely used in high accuracy acceleration measurement. However, there exist accumulated charges on the isolated mass which damage the accuracy and the stability of ESAs. In this paper, we propose to apply actuation voltage with a combined waveform to suppress the acceleration noise due to deposited charge. A model of the electrostatic force on the mass is established and the deviation voltage is found to be the dominant source of charge noise. Based on the analysis of disturbance electrostatic force under DC and AC signals, actuation combined with DC and AC voltage is designed and the disturbance force due to charge can be suppressed through adjustment towards the duty cycle of different compositions. Simulations and experiments are carried out and the results indicate that the disturbance due to charge can be suppressed up to 40%, which validates the efficiency of the scheme.

Charge Accumulation in the Homo-Crosslinked-Polyethylene Bilayer.

The homo-crosslinked-polyethylene (H-XLPE) bilayer simplifies the returned insulation structure of the factory joint in submarine cables, and its dielectric property is key to the reliability of the power transmission system. In this paper, we investigated the charge accumulation phenomenon in a secondary thermocompression H-XLPE bilayer using the pulse electro-acoustic method. The charge accumulation reduces its overall breakdown strength when compared with XLPE. According to X-ray diffraction measurement and thermal analysis results, the specimen forms a homo-junction region between the bilayers, which has overlapping spherulites with a thick lamella, high crystallinity, and high surface free energy. The charge accumulation can be ascribed to fused lamellas and the crystal imperfection of the homo-junction region, which restricts the charge transport process and exhibits a higher number of deep traps. This study emphasizes the importance of the homo-junction region in the H-XLPE bilayer, which should be considered in the design and operation of factory joint insulation.

Evaluating the Capacitive Response in Metal Halide Perovskite Solar Cells.

The perovskites solar cells (PSCs) is composed of multifaceted device architecture and involve complex charge extraction (both electronic and ionic), this makes the task demanding to unlock the origin of the different physical process that occurs in a PSC. The capacitance in PSCs depends on several external perturbations including frequency, illumination, temperature, applied bias, and importantly on the interface modification of perovskites/charge selective contact. Arguably, different features including interfacial and bulk; ionic, and electronic charge transport in PSCs occur at different time scales. Capacitance spectroscopy is a prevailing technique to unravel the various physical phenomenon that occurs in a PSC at different time scales. A deeper knowledge of the capacitive response of a PSCs is essential to understand the charge carrier kinetics and unlock the device physics. This work highlights the capacitive response of PSCs and its application to unlock the device physics which is essential for the further optimization and improvement of the device performance.

Boosting Nitrogen Reduction to Ammonia on FeN4 Sites by Atomic Spin Regulation.

Understanding the relationship between the electronic state of active sites and N2 reduction reaction (NRR) performance is essential to explore efficient electrocatalysts. Herein, atomically dispersed Fe and Mo sites are designed and achieved in the form of well-defined FeN4 and MoN4 coordination in polyphthalocyanine (PPc) organic framework to investigate the influence of the spin state of FeN4 on NRR behavior. The neighboring MoN4 can regulate the spin state of Fe center in FeN4 from high-spin (dxy 2 dyz 1 dxz 1 d z 2 1 d x 2 - y 2 1 ) to medium-spin (dxy 2 dyz 2 dxz 1 d z 2 1 ), where the empty d orbitals and separate d electron favor the overlap of Fe 3d with the N 2p orbitals, more effectively activating N≡N triple bond. Theoretical modeling suggests that the NRR preferably takes place on FeN4 instead of MoN4 , and the transition of Fe spin state significantly lowers the energy barrier of the potential determining step, which is conducive to the first hydrogenation of N2 . As a result, FeMoPPc with medium-spin FeN4 exhibits 2.0 and 9.0 times higher Faradaic efficiency and 2.0 and 17.2 times higher NH3 yields for NRR than FePPc with high-spin FeN4 and MoPPc with MoN4 , respectively. These new insights may open up opportunities for exploiting efficient NRR electrocatalysts by atomically regulating the spin state of metal centers.

A review on factors that affect surface charge accumulation and charge-induced surface flashover.

The surface charge accumulation is very likely to trigger the surface flashover, which limits the large-scale application of DC GIL/GIS. This article comprehensively reviews the effect of six factors, including insulator-electrode shape, surface roughness of the insulator and conductor, metal particles, temperature, humidity, and gas type, on the insulator surface charging property. Furthermore, three models i.e. 'analogous ineffective region' expansion model, charge cluster triggered surface flashover model, and synergistic model of adsorbed gas, revealing the mechanism of charge triggered surface flashover phenomenon are reviewed and discussed. Future work from the perspective of theoretical analysis and engineering application are suggested in this field.

Synthesis of a Novel Semi-Conductive Composites Doping with La0.8Sr0.2MnO3 for Excellent Electric Performance for HVDC Cable.

The semi-conductive layer located between the wire core and the insulation layer in high voltage direct current (HVDC) cable plays a vital role in uniform electric field and affecting space charges behaviors. In this work, the research idea of adding ionic conductive particles to semi-conductive materials to improve the conductive network and reduce the energy of the moving charge inside it and to suppress charge injection was proposed. Semi-conductive composites doped with different La0.8Sr0.2MnO3 (LSM) contents were prepared. Resistivity at different temperatures was measured to investigate the positive temperature coefficient (PTC) effect. Pulse electro-acoustic (PEA) method and thermal-stimulation depolarization currents (TSDC) tests of the insulation layers were carried out. From the results, space charge distribution and TSDC currents in the insulation samples were analyzed to evaluate the inhibitory effect on space charge injection. When LSM content is 6 wt. %, the experimental results show that the PTC effect of the specimen and charge injection are both being suppressed significantly. The maximum resistivity of it is decreased by 53.3% and the insulation sample has the smallest charge amount, 1.85 × 10-7 C under 10 kV/mm-decreased by 40%, 3.6 × 10-7 C under 20 kV/mm-decreased by 45%, and 6.42 × 10-7 C under 30 kV/mm-decreased by 26%. When the LSM content reaches 10 wt. %, the suppression effect on the PTC effect and the charge injection are both weakened, owing to the agglomeration of the conductive particles inside the composites which leads to the interface electric field distortion and results in charge injection enhancement.

Improved DC Dielectric Performance of Photon-Initiated Crosslinking Polyethylene with TMPTMA Auxiliary Agent.

To achieve high direct current (DC) dielectric performance of crosslinked polyethylene (XLPE) applied for insulated cable, the auxiliary crosslinking agent of trimethylolpropane trimethacrylate (TMPTMA) is employed in photon-initiated crosslinking process to the present polar-molecular group which will introduce deep traps for charge carriers. The space-charge accumulation and electrical conductance of XLPE are observably suppressed due to the deep traps deriving from the TMPTMA crosslinkers that are chemically connecting (grafted onto) polyethylene molecules. Thermally stimulated depolarization current tests and first-principles calculations consistently demonstrate a trapping mechanism of impeding charge injection and carrier transport in XLPE with TMPTMA crosslinkers. The characteristic cyclic anhydrides with coupled carbonyl groups are used as auxiliary crosslinkers to promote crosslinking efficiency and provide polar groups to polyethylene molecules which can be effectively fulfilled in industrial cable production. The results of infrared spectroscopy show that the auxiliary crosslinkers have been successfully grated to polyethylene molecules through the UV-initiation process. The space-charge characteristics achieve a significant improvement consistent with the theoretical estimation that deeper electronic traps can be introduced by auxiliary crosslinker and will consequently suppress space-charge accumulation through a trapping mechanism. Meanwhile, the conductivity of XLPE observably increases after using TMPTMA auxiliary crosslinkers at various temperatures of cable operation. The first-principles calculations also demonstrate that substantial electronic bound states have been introduced at the band edge of polyethylene molecules crosslinked by TMPTMA, leading to reduction in electrical conductivity. On the advantage of ameliorating DC dielectric performance by way of UV-initiated crosslinking process, the present research suggests a substantial strategy in XLPE cable industrial productions.