Cross-Linked Polyvinylimidazole Complexed with Heteropolyacid Clusters for Deep Oxidative Desulfurization.

The combustion of fuel with high sulfur concentrations produces a large number of sulfur oxides (SOx), which have a range of negative effects on human health and life. The preparation of catalysts with excellent performance in the oxidative desulfurization (ODS) process is highly effective for reducing SOx production. In this paper, cross-linked polyvinylimidazole (VE) was successfully created using a simple ontology aggregation method, after which a catalyst of polyvinylimidazolyl heteropolyacid clusters (VE-HPA) was prepared by adding heteropolyacid clusters. Polyvinylimidazolyl-phosphotungstic acid (VE-HPW) showed an outstanding desulfurization performance, and the desulfurization efficiency reached 99.68% in 60 min at 50 °C with H2O2 as an oxidant. Additionally, the catalyst exhibited recyclability nine consecutive times and remained stable, with a removal rate of 98.60%. The reaction mechanism was eventually proposed with the assistance of the free radical capture experiment and GC-MS analysis.

Synergistically enhanced discharged energy density and efficiency achieved in designed polyetherimide-based composites via asymmetrical interlayer structure induced optimized interface effectiveness.

The continuous advancement in energy storage technologies necessitates the iteration of energy storage dielectrics urgently. However, the current state-of-the-art composite films fail to meet the application requirements of energy storage devices, which demand a combination of high discharged energy density (Ue), high energy storage efficiency (η), and excellent high-temperature performance. To address this challenge, we present an innovative interlayer composed of pure BN nanosheets in polyetherimide (PEI)-based asymmetrical multilayered composites doped with Na0.5Bi0.5TiO3 ceramic fibers. This innovative structure confers the PEI-based composites upon synergistic optimization of polarization intensity, breakdown strength and energy loss by designed interface effectiveness adopting tailored filler and interface configuration as modulation means, which can be further confirmed by finite element simulations and comparative experiments. The resultant composite film achieves an excellent Ue of 22.95 J cm-3 and an ultra-high η of 96.81% at ambient temperature, along with high-temperature performances of 12.88 J cm-3 and 79.26% at 150 °C, surpassing all previously reported polymer films in terms of both metrics. This study provides new insights for developing high-performance energy storage dielectrics suitable for practical applications.

Experimental and Theoretical Density Functional Theory Approaches for Desulfurization of Dibenzothiophene from Diesel Fuel with Imidazole-Based Heteropolyacid Catalysts.

Oxidative desulfurization (ODS) has been proved to be an efficient strategy for the removal of aromatic sulfur compounds from diesel oils, which are one of the main sources of air pollution. Heteropolyacid catalysts are highly active species for ODS, but the promotion of their catalytic activity and clarification of their catalytic mechanism remain an important issue. Herein, a series of novel imidazole-based heteropolyacid catalysts are prepared by a one-pot method for multiphase deep ODS of fuel with hydrogen peroxide as an oxidant. The experimental results show that the desulfurization performance of the prepared imidazole-based heteropolyacid catalysts is high up to 99.9% under mild conditions. The catalyst also possesses excellent recovery performance, and the desulfurization activity remains at 97.7% after being recycled seven times. Furthermore, density functional theory calculation is first employed to clarify the origin of the high desulfurization activity, and the results show that with the imidazole-based heteropolyacid (HPW-VIM) as the catalyst, the energy barrier is much lower than that with phosphotungstic acid (HPW) as the catalyst.

Deciphering the phase transition-induced ultrahigh piezoresponse in (K,Na)NbO3-based piezoceramics.

Here, we introduce phase change mechanisms in lead-free piezoceramics as a strategy to utilize attendant volume change for harvesting large electrostrain. In the newly developed (K,Na)NbO3 solid-solution at the polymorphic phase boundary we combine atomic mapping of the local polar vector with in situ synchrotron X-ray diffraction and density functional theory to uncover the phase change and interpret its underlying nature. We demonstrate that an electric field-induced phase transition between orthorhombic and tetragonal phases triggers a dramatic volume change and contributes to a huge effective piezoelectric coefficient of 1250 pm V-1 along specific crystallographic directions. The existence of the phase transition is validated by a significant volume change evidenced by the simultaneous recording of macroscopic longitudinal and transverse strain. The principle of using phase transition to promote electrostrain provides broader design flexibility in the development of high-performance piezoelectric materials and opens the door for the discovery of high-performance future functional oxides.

Multiscale structural engineering of dielectric ceramics for energy storage applications: from bulk to thin films.

Dielectric capacitors with the prominent features of ultrafast charging-discharging rates and ultrahigh power densities are ubiquitous components in modern electronics. To meet the growing demand for electronics miniaturization, dielectric capacitors with high energy storage properties are extensively researched. Here we present an overview of the recent progress in the engineering of multiscale structures of dielectric ceramics ranging from bulk to thin films. This article commences with a brief introduction of the fundamentals of dielectric ceramics, including primary parameters, a library of dielectric ceramics, and multiscale structures. Emphases are placed on the relationship between multiscale structures and energy storage properties and the rational structure design principles in dielectric ceramics. Also included are currently available multilayer ceramic capacitors based on multiscale engineered ceramic structures. Finally, challenges along with opportunities for further research and development of high-performance dielectric ceramics for electrostatic energy storage are highlighted.

Multilayer Structured Poly(vinylidene fluoride)-Based Composite Film with Ultrahigh Breakdown Strength and Discharged Energy Density.

Poly(vinylidene fluoride)-based (PVDF) composites with high discharged energy density (Ue) have been considered as advanced dielectric materials for pulsed power systems and electrical weapon systems. However, further improvement of the Ue of PVDF-based composites with higher breakdown strength (Eb) is of utmost importance. Based on the principle of voltage distribution in the multilayer structure, the multilayer structure (five-layer structure) ceramic/polymer composite films consisting of pristine PVDF layers with high breakdown strength and PVDF layers doped with one-dimensional 0.15SrTiO3-0.85Na0.5Bi0.5TiO3 (1D SNBT) fibers where the two kinds of layers stacked alternately has been designed and fabricated. Accordingly, a series of analyses of the dielectric properties and energy storage performances are presented, and the related results are tentatively explained by finite element simulation. The energy storage characteristics of the composite films are greatly improved due to the newly designed structure. An excellent Ue of 20.82 J cm-3 is achieved at an ultrahigh electric field of 640 MV m-1 with the PVDF layers containing 6 vol % SNBT fibers. Therefore, this work provides a new strategy to design and fabricate advanced polymer-based energy storage materials.

Excellent Energy-Storage Properties Achieved in BaTiO3-Based Lead-Free Relaxor Ferroelectric Ceramics via Domain Engineering on the Nanoscale.

Barium titanate-based energy-storage dielectric ceramics have attracted great attention due to their environmental friendliness and outstanding ferroelectric properties. Here, we demonstrate that a recoverable energy density of 2.51 J cm-3 and a giant energy efficiency of 86.89% can be simultaneously achieved in 0.92BaTiO3-0.08K0.73Bi0.09NbO3 ceramics. In addition, excellent thermal stability (25-100 °C) and superior frequency stability (1-100 Hz) have been obtained under 180 kV cm-1. The first-order reversal curve method and transmission electron microscopy measurement show that the introduction of K0.73Bi0.09NbO3 makes ferroelectric domains to transform into highly dynamic polar nanoregions (PNRs), leading to the concurrently enhanced energy-storage properties by the transition from ferroelectric to relaxor ferroelectric (RFE). Furthermore, it is confirmed by piezoresponse force microscopy that the appearance of PNRs breaks the long-range order to some extent and reduces the stability of the microstructure, which explains the excellent energy-storage performance of RFE ceramics. Therefore, this work has promoted the practical application ability of BaTiO3-based energy-storage dielectric ceramics.

Significantly Enhanced Breakdown Strength and Energy Density in Sandwich-Structured Barium Titanate/Poly(vinylidene fluoride) Nanocomposites.

Sandwich-structured BaTiO3 /poly(vinylidene fluoride) (PVDF) nanocomposites are successfully prepared by the solution-casting method layer by layer. They possess both high breakdown strength and large dielectric polarization simultaneously. An ultra-high energy-storage density of 18.8 J cm(-3) can be achieved by adjusting the volume fraction of ceramic fillers: this is almost three times larger than that of pure PVDF.