Interdisciplinary Materials最新文献

The critical challenges of the energy crisis and environmental degradation promote innovative approaches for energy conversion. Semiconductor-based photocatalytic technology, which transforms solar energy into chemical energy, emerges as a promising solution. However, the practical application of this technology faces several challenges, such as the rapid recombination of photogenerated electrons and holes, significantly limiting photocatalytic efficiency. In this review, we provide a detailed discussion, an insightful perspective, and a critical evaluation of recent advances, challenges, and opportunities in the field of photocatalysis using polar materials. We present a comprehensive examination of the photocatalytic mechanisms, activity, and diverse applications of photocatalysts based on polar materials. We also briefly discuss the engineering design of polar photocatalysis in experiments and its scalability in the industry. This review outlines future trends and potential breakthroughs in the photocatalytic field using polar materials, projecting their transformative impact on environmental chemistry and energy engineering.

Electrocatalysis, which involves oxidation and reduction reactions with direct electron transfer, is essential for a variety of clean energy conversion devices. Currently, the vast majority of studies regarding electrocatalysis reactions focus on strong acidic or alkaline media because of the higher catalytic activity. Nevertheless, some inherent drawbacks, including the corrosive environment, expensive proton exchange membranes, and side effects, are still hard to break through. A sustainably promising way to overcome these shortcomings is to deploy neutral/near-neutral electrolytes for electrocatalysis reactions. Unfortunately, insufficient research in this area due to the lack of attention to related issues has slowed down the development process. In this review, we systematically review the catalytic reaction mechanisms, neutral electrolytes, electrocatalysts, and modification strategies carried out in neutral media on the three most common electrocatalytic reactions, that is, hydrogen evolution reaction, oxygen reduction reaction, and oxygen evolution reaction. Furthermore, the advanced characterization tools for guiding catalyst synthesis and mechanistic studies are also summarized. Eventually, we propose some challenges and perspectives on electrocatalysis reactions in neutral media and hope it will attract more research interest and provide guidance in neutral electrocatalysis.

Poly(vinylidene fluoride) (PVDF) is the most attractive piezoelectric polymer for application in flexible sensors. To attain excellent piezoelectric properties, a substantial amount of spontaneous polar β-phase content is highly desired. Nevertheless, the current reported manufacturing methods to increase β-phase contents are inconvenient and complex, hindering progress in PVDF's application. This work proposes a folding-hot-pressing method to fabricate high β-phase-content PVDF films. Structural characterization indicates that the films have α and β phases and the folding-hot-pressing process transforms the α phase into the β phase. Due to the 97.5% β-phase content and aligned structure, a piezoelectric constant of 20 pC/N is achieved in the three-times folded film. Furthermore, the process method enhances the tensile strength (126.2 MPa) of the films, with a low Young's modulus (0.87 GPa) remaining, making the films applicable for flexible piezoelectric sensors. Additionally, sensors based on the achieved films were assembled and applied for human physiological activity monitoring. This work offers a scalable new melt-processing strategy for developing high-performance PVDF-based piezoelectric composite films for wearable electronic devices.

Along with the constantly evolving functional microsystems toward more diversification, the more rigorous design deliberation of pursuing higher mass-loading of electrode materials and low-temperature fabrication compatibility have imposed unprecedented demand on integrable all-solid-state thin-film microbatteries. While the classic thin-film intercalation cathode prepared by vacuum-based techniques inevitably encountered a post-annealing process, tape-casting technologies hold great merits both in terms of high-mass loading and low-temperature processing. In this work, a novel microbattery configuration is developed by the combination of traditional tape-casting thick electrodes and sputtered inorganic thin-film solid electrolytes (~3 μm lithium phosphorus oxynitride). Enabled by physically pressed or vapor-deposited Li as an anode, solid-state batteries with tape-casted LiFePO₄ electrodes exhibit outstanding cyclability and stability. To meet integration requirements, LiFePO₄/LiPON/Si microbatteries were successfully fabricated at low temperatures and found to achieve a wide operating temperature range. This novel configuration has good prospects in promoting the thin-film microbattery enabling a paradigm shift and satisfying diversified requirements.

In recent years, the precisely controlled synthesis of chiral twisted molecular carbons has emerged as a forefront topic in the research of carbon materials. Molecular carbons refer to carbon nanomaterials synthesized with precision at the atomic level. Through rational design, rigid and stable chiral twisted structures can be synthesized. The exploration in the field of chiral twisted molecular carbons is key to fully understanding the various twisted configurations of carbon materials and delving into the relationship between structure design and functionality. This review explores chiral twisted configurations of carbon nanomaterials such as nanographene, carbon nanobelts, carbon nanosheets, graphdiyne, etc. It emphasizes the role of photocyclization, Scholl reaction, and Diels–Alder reactions in achieving precise chiral control and discusses a range of innovative design strategies. These strategies have led to the development of various twisted structures, such as helical, propeller, and Möbius strip configurations. The introduction of chirality, combined with the inherent exceptional optical properties of nanocarbon materials, has facilitated the creation of materials with superior chiroptical performances. This advancement is driving applications in fields such as optoelectronics and chiral optics.

To unveil the nature of amorphous states, single-element amorphous metals have been the perfect research subject due to the simplest composition. However, the extreme crystal nucleation and growth rate in single-element metal make the synthesis of single-element amorphous metals seemingly impossible in the past. Fortunately, benefited by several delicate synthetic strategies developed recently, the single-element amorphous metals have been successfully demonstrated. This review aims to provide a systematic overview of the synthesis of single-element amorphous metals covering the challenges in physics and recent achievements. In addition, current understanding of the atomic and electronic structures of single-element amorphous metal has also been included. Finally, the challenges that worth further investigation are discussed. By identifying the potential avenues for further exploration, this review aims to contribute valuable insights that will propel the cognition of single-element amorphous metals.

Alkaline hydrogen evolution reaction (HER) for scalable hydrogen production largely hinges on addressing the sluggish bubble-involved kinetics on the traditional Ni-based electrode, especially for ampere-level current densities and beyond. Herein, 3D-printed Ni-based sulfide (3DPNS) electrodes with varying scaffolds are designed and fabricated. In situ observations at microscopic levels demonstrate that the bubble escape velocity increases with the number of hole sides (HS) in the scaffolds. Subsequently, we conduct multiphysics field simulations to illustrate that as the hole shapes transition from square, pentagon, and hexagon to circle, where a noticeable reduction in the bubble-attached HS length and the pressure balance time around the bubbles results in a decrease in bubble size and an acceleration in the rate of bubble escape. Ultimately, the 3DPNS electrode with circular hole configurations exhibits the most favorable HER performance with an overpotential of 297 mV at the current density of up to 1000 mA cm⁻² for 120 h. The present study highlights a scalable and effective electrode scaffold design that promotes low-cost and low-energy green hydrogen production through the ampere-level alkaline HER.

Exploration of metastable phases holds profound implications for functional materials. Herein, we engineer the metastable phase to enhance the thermoelectric performance of germanium selenide (GeSe) through tailoring the chemical bonding mechanism. Initially, AgInTe₂ alloying fosters a transition from stable orthorhombic to metastable rhombohedral phase in GeSe by substantially promoting p-state electron bonding to form metavalent bonding (MVB). Besides, extra Pb is employed to prevent a transition into a stable hexagonal phase at elevated temperatures by moderately enhancing the degree of MVB. The stabilization of the metastable rhombohedral phase generates an optimized bandgap, sharpened valence band edge, and stimulative band convergence compared to stable phases. This leads to decent carrier concentration, improved carrier mobility, and enhanced density-of-state effective mass, culminating in a superior power factor. Moreover, lattice thermal conductivity is suppressed by pronounced lattice anharmonicity, low sound velocity, and strong phonon scattering induced by multiple defects. Consequently, a maximum zT of 1.0 at 773 K is achieved in (Ge_0.98Pb_0.02Se)_0.875(AgInTe₂)_0.125, resulting in a maximum energy conversion efficiency of 4.90% under the temperature difference of 500 K. This work underscores the significance of regulating MVB to stabilize metastable phases in chalcogenides.

Sodium (Na) metal is a competitive anode for next-generation energy storage applications in view of its low cost and high-energy density. However, the uncontrolled side reactions, unstable solid electrolyte interphase (SEI) and dendrite growth at the electrode/electrolyte interfaces impede the practical application of Na metal as anode. Herein, a heterogeneous Na-based alloys interfacial protective layer is constructed in situ on the surface of Na foil by self-diffusion of liquid metal at room temperature, named “HAIP Na.” The interfacial Na-based alloys layer with good electrolyte wettability and strong sodiophilicity, and assisted in the construction of NaF-rich SEI. By means of direct visualization and theoretical simulation, we verify that the interfacial Na-based alloys layer enabling uniform Na⁺ flux deposition and suppressing the dendrite growth. As a result, in the carbonate-based electrolyte, the HAIP Na||HAIP Na symmetric cells exhibit a remarkably enhanced cycling life for more than 650 h with a capacity of 1 mAh cm⁻² at a current density of 1 mA cm⁻². When the HAIP Na anode is paired with sulfurized polyacrylonitrile (SPAN) cathode, the SPAN||HAIP Na full cells demonstrate excellent rate performance and cycling stability.

Low efficiency and spectral instability caused by the surface defects have been considerable issues for the mixed-halogen blue emitting perovskite quantum dots light-emitting diodes (PeQLEDs). Here, an in situ surface passivation to perovskite quantum dots (PeQDs) is realized by introducing the metal cations competitive lattice occupancy assisted with acid-etching, in which the long-chain, insulating and weakly bond surface ligands are removed by addition of octanoic acid (OTAC). Meanwhile, the dissolved A-site cations (Na⁺) compete with the protonated oleyl amine and are subsequently anchored to the surface vacancies. The preadded lead bromide, acting as inorganic ligands, demonstrates strong bonding to the uncoordinated surface ions. The as-synthesized PeQDs show the boosted photoluminescence quantum yield (PLQY) and superior stability with longer lifetime. As a result, the PeQLEDs (470 nm) based on the OTAC-Na PeQDs exhibit an external quantum efficiency of 8.42% in the mixed halogen PeQDs (CsPb(Br_xCl_1−x)₃). Moreover, the device exhibits superior spectra stability with negligible shift. Our competition mechanism in combination with in situ passivation strategy paves a new way for improving the performance of blue PeQLEDs.