http://onlinelibrary.wiley.com/rss/journal/10.1002/(ISSN)1521-4095

The study presents a novel ultrafast laser-driven synthesis technique for zeolites directly in liquid. Laser pulses create a microscopic reactor that controls reaction kinetics at femto- and picosecond timescales. Nonlinear light-matter interactions drive nucleation and growth, allowing the process to be paused at any stage of self-assembly.

Research demonstrates that zeolite nucleation and growth can be controlled by fine-tuning chemical composition, temperature, and pressure, resulting in structures with diverse porosities and functionalities. Nevertheless, current energy delivery methods lack the finesse required to operate on the femto- and picosecond timescales of silica polymerization and depolymerization, limiting their ability to direct synthesis with high precision. To overcome this limitation, an ultrafast laser synthesis technique is introduced, capable of delivering energy at these timescales with unprecedented spatiotemporal precision. Unlike conventional or emerging approaches, this method bypasses the need for specific temperature and pressure settings, as nucleation and growth are governed by dynamic phenomena arising from nonlinear light–matter interactions, such as convective flows, cavitation bubbles, plasma formation, and shock waves. These processes can be initiated, paused, and resumed within fractions of a second, effectively “freezing” structures at any stage of self-assembly. Using this approach, the entire nucleation and growth pathway of laser-synthesized TPA-silicate-1 zeolites is traced, from early oligomer formation to fully developed crystals. The unprecedented spatiotemporal control of this technique unlocks new avenues for manipulating reaction pathways and exploring the vast configurational space of zeolites.

Precisely manipulating the reconstruction process to generate specific active motifs remains challenging during the alkaline OER. NiCo2O4-Fn, structured with NiCo2O4 cores and (NH4)NixCo1−xF3 shells, facilitate the dual-metal NiCoOOH active phase with Ov forming at a lower voltage than the single-metal NiOOH in NiCo2O4, which is demonstrated by in situ Raman and XAFS. The NiCoOOH generation is attributed to the transformation of (NH4)NixCo1−xF3 into NixCo1−x(OH)2 hydroxide in electrolyte without bias. Consequently, NiCo2O4-Fn exhibits enhanced OER intrinsic activities compared to NiCo2O4.

Dynamic reconstruction of catalysts is key to active site formation in alkaline oxygen evolution reaction (OER), but precise control over this process remains challenging. Herein, F-doped NiCo2O4 (NiCo2O4-Fn), consisting of a NiCo2O4 core and a (NH4)NixCo1−xF3 shell is reported, which promotes the formation of a dual-metal NiCoOOH active phase. In situ Raman and X-ray absorption fine structure analyses reveal that the NiCoOOH, rich in oxygen vacancies (Ov), forms at 1.2 V versus the reversible hydrogen electrode (RHE) for NiCo2O4-F1, in contrast to the NiOOH phase formation at 1.4 V versus RHE for undoped NiCo2O4. This is facilitated by the transformation of (NH4)NixCo1−xF3 into amorphous NixCo1−x(OH)2 in the KOH electrolyte without bias. Electrochemical tests show that NiCo2O4-F1 exhibits a 14-fold increase in intrinsic activity compared to NiCo2O4. Theoretical calculations suggest that Ov-induced unsaturated Co and Ni sites enhance electroactivity by promoting *OH intermediates adsorption and conversion, lowering the OER energy barrier. The oriented control of NiCoOOH active motifs in NiCo2O4 spinel, achieved through fluorine engineering, paves a new avenue for designing efficient OER electrocatalysts.

A novel plasma strategy is reported to introduce N and F in Co3O4 (N, F-Co3O4) simultaneously as the heteroatoms, which enables the OER to occur via the lattice oxygen mechanism. The N, F-Co3O4 sample exhibits superior OER performance with a low overpotential and superior stability.

The oxygen evolution reaction (OER) is a pivotal process in numerous renewable energy conversion technologies. However, its sluggish intrinsic kinetics and intricate transfer process impede the efficient conversion of energy. Activating the lattice oxygen mechanism (LOM) is of paramount importance to break through the theoretical scaling relationship and boost the oxygen evolution catalytic activity. In this contribution, N and F are successfully introduced into Co3O4 simultaneously as heteroatoms via a controllable plasma strategy to modulate the covalency property of metal-oxygen. Theoretical simulations and experiment results demonstrated that the covalency of the cobalt-oxygen bond is significantly enhanced under the synergistic effect of N and F, successfully triggering the LOM pathway and facilitating the OER process. The N, F-Co3O4 composite displays an impressive OER performance, exhibiting a low overpotential of 254 mV at 10 mA cm−2 and remarkable stability at 20, 150, and 400 mA cm−2. In addition, The N, F-Co3O4 also exhibits a low overpotential of 285 mV at 20 mA cm−2 in 1 m KOH + 0.5 m NaCl solution, and remarkable performance on overall water splitting. This work offers profound insights into the OER mechanism and a crucial strategy for enhancing the electrocatalytic activity of spinel oxides.

This review examines the crucial role of materials in heart disease interventions, focusing on strategies for monitoring, managing, and repairing heart conditions. It discusses the material requirements for medical devices, highlighting recent innovations and their impact on cardiovascular health. It aims to provide insights into the challenges in cardiovascular interventions and the essential role of materials in developing effective solutions.

Heart disease encompasses a range of conditions that affect the heart, including coronary artery disease, arrhythmias, congenital heart defects, heart valve disease, and conditions that affect the heart muscle. Intervention strategies can be categorized according to when they are administered and include: 1) Monitoring cardiac function using sensor technology to inform diagnosis and treatment, 2) Managing symptoms by restoring cardiac output, electrophysiology, and hemodynamics, and often serving as bridge-to-recovery or bridge-to-transplantation strategies, and 3) Repairing damaged tissue, including myocardium and heart valves, when management strategies are insufficient. Each intervention approach and technology require specific material properties to function optimally, relying on materials that support their action and interface with the body, with new technologies increasingly depending on advances in materials science and engineering. This review explores material properties and requirements driving innovation in advanced intervention strategies for heart disease and highlights key examples of recent progress in the field driven by advances in materials research.

An iodine-mediated electrochemical strategy recycles spent LiFePO4 cathodes, extracting lithium as carbonate and producing metallic zinc. Delithiated LiFePO4 is transformed into an efficient oxygen evolution catalyst. This scalable, sustainable approach reduces energy use and emissions while offering economic benefits for clean energy applications.

With the widespread application of lithium-ion batteries, the recycling of spent batteries, especially those involving LiFePO4 (LFP) cathodes for their low-cost and high safety, has become an urgent environmental and resource challenge. Traditional recycling methods (hydrometallurgy and pyrometallurgy) struggle to achieve green and efficient recycling. Herein, this study proposes an iodine-mediated electrochemical strategy to utilize a recyclable I3 −/I− redox system and efficiently extract Li+ from spent LFP through liquid-phase reactions on one side (achieving a 93% leaching rate and recovery as lithium carbonate), while simultaneously producing metallic zinc through electrodeposition, which can be directly used in Zn-air batteries or hydrogen production. Furthermore, the delithiated LFP is upcycled into an oxygen evolution reaction (OER) catalyst, achieving an overpotential of only 250 mV at 10 mA cm−2, superior to commercial RuO2 catalysts. Eventually, this system reduces energy consumption by 32% (9.2 MJ kg−1) compared to traditional hydrometallurgical processes, decreases greenhouse gas emissions by 35% compared to traditional pyrometallurgical processes, while achieving a net profit of ≈$0.44 per kg. This work establishes a novel, scalable recycling system, providing a robust sustainable solution for spent LFP cathodes recycling and clean energy storage.

Phononic devices offer unique advantages in RF applications due to their shorter wavelengths compared to photons. This perspective explores functional phononic devices that can enable integrated phononic circuits. These circuits promise to enable miniaturized communication systems with improved SWaP-C characteristics, while also finding applications in quantum information science, sensing, and biomedical engineering.

The phonon wavelength, being much shorter than that of photons at the same frequency, offers phononic devices a unique niche in radio frequency (RF) applications. However, the current limitations of these devices, particularly their restricted functionality, hinder their broader integration and application. Currently, many functions are achieved using alternative signal forms like electric and photonic signals, requiring bulky converters to transform between phonon signals and other forms. The development of functional phononic devices paves the way for integrated phononic circuits, which aim to minimize the need for signal conversion while accomplishing all necessary functions. In this perspective, a brief overview of several types of functional phononic devices is provided that hold promise for integration, such as phononic modulators, amplifiers, lasers, nonreciprocal devices, and those inspired by topological physics. It is envisioned that through continued developments in materials, fabrication techniques, and designs, it's possible to realize integrated phononic circuits which will be applied in miniaturized communication devices with reduced size, weight, power consumption, and cost (SWaP-C), as well as in other fields including quantum information science, sensing, biomedical engineering, and beyond.

Metal@Cu2O composites are developed as platforms to investigate the localized surface plasmon resonance (LSPR) induced enhancement on photoelectrocatalysis. The contributions of two LSPR mechanisms, plasmon-induced resonance energy transfer (PIRET) and hot electron transfer (HET), to the photocurrent are quantified using different bands of incident light, providing a quantitative understanding of the role of PIRET and HET in boosting photoelectrocatalysis.

The localized surface plasmon resonance (LSPR) of metal nanoparticles can substantially enhance the activity of photoelectrocatalytic (PEC) reactions. However, quantifying the respective contributions of different LSPR mechanisms to the enhancement of PEC performance remains an urgent challenge. In this work, Cu@Cu2O composites prepared by annealing Cu2O under an inert atmosphere and electrodeposited metal@Cu2O composites (MED@Cu2O, MED = CuED, AuED, AgED, PdED, PtED) are employed as platform materials to investigate the LSPR effect on the PEC hydrogen evolution reaction (HER). All the composites exhibited remarkably LSPR-enhanced activity toward PEC HER. The contributions of two LSPR mechanisms, plasmon induced resonance energy transfer (PIRET) and hot electron transfer (HET), to the photocurrent on Cu@Cu2O and CuED@Cu2O are quantified by using different bands of incident light. Moreover, using MED@Cu2O composites, the effects of both the metal species and the applied potential on HET are quantitatively investigated. The results reveal that a pronounced HET enhancement occurs only when the LSPR peak energy is lower than the semiconductor bandgap energy (E g) and that HET strengthens as the applied potential becomes more negative for PEC HER. This work therefore provides a quantitative understanding of the roles of PIRET and HET in boosting PEC activity.

Emulating skin-texturing capabilities of cephalopods, a magnetic shape-morphing platform (MMP) is developed to enable systems that reversibly modulate their morphology and stiffness. The MMP, consisting of polymer composites embedded with liquid metal droplets and ferromagnetic particles, achieves complex and sophisticated 3D configurations through thermo-magnetic stimuli under programmed magnetization profiles. Proof-of-concept demonstrations suggest potential applications in 3D displays and soft robotics.

Shape-morphing systems capable of actively achieving diverse three-dimensional (3D) configurations are essential for advancements in 3D electronics and soft robotics. However, current shape-morphing technologies encounter challenges such as iterative shape reconfiguration with high geometrical complexity, mechanical stability, and slow response times. Inspired by the 3D skin texturing abilities of cephalopods, 3D magnetic shape-morphing systems are introduced, enabling reversible and continuous transformation with a broad range of complex reconfigurable shapes. This is achieved through thermo-magnetoactive actuation, guided by magnetization profiles created via a 3D magnetic encoding strategy. The system leverages magnetic shape-morphing platforms (MMPs) built with a composite containing elastomer mixed with low melting point alloy (LMPA) particles comprising ferromagnetic particles. The MMP can produce intricate, robust 3D configurations using multimodal magnetic actuation facilitated by tunable stiffness and magnetoactive reconfigurability. Proof-of-concept demonstrations of 3D visio-tactile displays and light-responsive flower robots highlight the potential of bioinspired 3D magnetic shape-morphing systems, suggesting promising applications in 3D electronics, soft robotics, and visio-haptic human interfacing.

A composite hydrogel electrolyte is prepared by constructing a 3D supramolecular network. The hydrogel electrolyte possesses good mechanical properties, superior ionic conductivity, and high zinc ion transference number, which can inhibit dendrite growth, enable uniform zinc deposition, achieve long cycle life, and realize high capacity retention.

Hydrogel electrolytes have garnered extensive attention in zinc ion batteries due to their excellent flexibility and good safety. However, their limited mechanical properties, low ionic conductivity, and poor Zn2+ transference number pose significant challenges for developing high-performance zinc ion batteries. Herein, this work constructs a 3D supramolecular network capable of locking anions and active water molecules through the abundant hydrogen bonding interactions between aramid nanofibers, polyvinyl alcohol, and anions. This network synergistically enhances the mechanical properties (with a mechanical strength of 0.88 MPa and a toughness of 3.28 MJ m−3), ionic conductivity (4.22 S m−1), and Zn2+ transference number (0.78). As a result, the supramolecular composite hydrogel electrolyte can effectively inhibit dendrite growth and side reactions, facilitate interface regulation, and enable uniform zinc deposition. The Zn anode exhibits a cycle life of 1500 h at 5 mA cm−2 and 5 mAh cm−2, with an average coulombic efficiency of 99.1% over 600 cycles. Additionally, the Zn||polyaniline full cell maintains a high capacity retention of 78% after 9100 cycles at 1 A g−1. The assembled pouch cells demonstrate good flexibility, deformability, and compression resistance. This work provides valuable insights into the design of high-performance hydrogel electrolytes for zinc ion batteries.

Magnetotactic bacteria (MTB) are living microorganisms that produce magnetosomes for navigation using the Earth's geomagnetic field. Their built-in magnetic components, along with their intrinsic and/or modified biological functions, make them one of the most promising platforms for making future living and programmable microrobots. This review highlights recent advances in MTB-based microrobotics, detailing their interactions with magnetic fields, propulsion mechanisms, motion control, and emerging strategies for engineering and functionalizing MTB for biomedical applications.

Nature's ability to create complex and functionalized organisms has long inspired engineers and scientists to develop increasingly advanced machines. Magnetotactic bacteria (MTB), a group of Gram-negative prokaryotes that biomineralize iron and thrive in aquatic environments, have garnered significant attention from the bioengineering community. These bacteria possess chains of magnetic nanocrystals known as magnetosomes, which allow them to align with Earth's geomagnetic field and navigate through aquatic environments via magnetotaxis, enabling localization to areas rich in nutrients and optimal oxygen concentration. Their built-in magnetic components, along with their intrinsic and/or modified biological functions, make them one of the most promising platforms for future medical microrobots. Leveraging an externally applied magnetic field, the motion of MTBs can be precisely controlled, rendering them suitable for use as a new type of biohybrid microrobotics with great promise in medicine for bioimaging, drug delivery, cancer therapy, antimicrobial treatment, and detoxification. This mini-review provides an up-to-date overview of recent advancements in MTB microrobots, delineates the interaction between MTB microrobots and magnetic fields, elucidates propulsion mechanisms and motion control, and reports state-of-the-art strategies for modifying and functionalizing MTB for medical applications.

This work reports the precise recognition of gas molecules with similar kinetic sizes while maintaining high gas diffusivity through the modification of the 1D channels of micrometer-sized mordenite. The weak acid salt-modified mordenite NaAlO2@MOR(0.5) exhibits remarkable carbon dioxide/acetylene kinetic selectivity (534.3), and high carbon dioxide capacity and diffusion constant.

The design of physical adsorbents for a precise recognition of gas molecules with similar kinetic sizes is of importance as adsorptive separation can serve as an alternative to energy-intensive distillation processes. However, it is challenging to balance the selectivity, capacity, and adsorption kinetics of the adsorbents. Herein, an efficient kinetic separation of acetylene and carbon dioxide is reported, which have nearly identical kinetic sizes, achieved through modification of the one-dimensional (1D) channels of a micrometer-sized mordenite. Under ambient conditions, the weak acid salt-modified mordenite denoted as NaAlO2@MOR(0.5), exhibits a remarkable kinetic separation selectivity of 534.3 while retaining an excellent diffusivity for CO2. Compared to other adsorbent materials, its dynamic column performance for carbon dioxide significantly exceeds those of molecular sieve materials. In terms of separation selectivity, it is superior to thermodynamic separation adsorbents. The high efficiency of NaAlO2@MOR(0.5) in CO2/C2H2 kinetic separation is validated by column breakthrough experiments. Furthermore, NaAlO2@MOR(0.5) has a low cost and high thermal stability. This study can guide the design of adsorbents that balance selectivity, capacity, and gas diffusivity, to provide a highly efficient kinetic separation of gas molecules with similar kinetic diameters.

Recreating Silk's Fibrillar Nanostructure

In article number 2413786, Martin Zaki, Benjamin James Allardyce, and co-workers present a new method to solubilise silk without degumming and use it to successfully wet spin fibres with a nanofibrillar structure akin to natural silk, but twice as tough. This new spinning dope, which contains both undegraded fibroin and sericin, spontaneously exhibited naturally-occurring liquid-liquid phase separation behaviour, which is likely to be a crucial step in replicating native silk spinning. Cover art by Ella Maru Studios.

Mechanical Metamaterials

Simple changes in the local topology of a mechanical metamaterial can induce dramatic global deformations, potentially driving advances in future shape-morphing materials and deployable structures, such as those used in space settlement or medical devices. More details can be found in article number 2415962 by Johan Christensen and co-workers.

Directly Printed Soft 3D Plasmonic Resonators

Conventional 2D plasmonic resonators face limitations in their application to soft electronic platforms due to signal attenuation induced by lossy media. In article number 2418182, Seungjun Chung and co-workers developed directly printed 3D plasmonic resonators with highly conductive elastomeric composites. Diverse soft 3D resonators demonstrated structural and signal integrities under repetitive strain cycles, highlighting higher Q-factor resonances even on lossy media.

Organic Redox Mediators

In article number 2415805, Hyun-Wook Lee, Ji-Won Hwang, Ja-Yeong Kim, Shuming Chen, Sung-Eun Suh, Won-Jin Kwak, and co-workers present reactive oxygen-resistive redox mediator (RM) by rational design strategies based on Bredt's rule. Unlike other bi-cyclic RMs, the as-designed RM shows exceptional chemical stability against reactive oxygens and consequently delivers improved electrochemical reversibility with high oxygen yield during cycles.

Rapid Drying

Rapid drying is a key principle for scalable, high-speed, uniform, and pinhole-less deposition of 2D materials. Using hot dipping and air knife sweeping (AKS), deposition speeds up to 0.21 m2 min−1 are achieved, surpassing conventional protocols by 2–4 orders of magnitude. This approach can extend to 1D and 3D materials if they are uniformly dispersible in rapidly evaporable liquids. More details can be found in article number 2411447 by, Chuan Wang, Dongwook Lee, and co-workers.

Organic redox mediators (ORMs) reactive nature with 1O2 causes the functional degradation but the reactivity of ORMs is often neglected. The ORM is systematically designed, which has superior 1O2 stability than ORMs with similar molecular structures and promises enhanced cyclability sustaining its catalytic function. This work emphasizes the necessity of suitable design of ORMs and the importance of controlling 1O2.

The utilization of redox mediators (RMs) in lithium–oxygen batteries (LOBs) has underscored their utility in high overpotential during the charging process. Among the currently known RMs, it is exceptionally challenging to identify those with a redox potential capable of attenuating singlet oxygen (1O2) generation while resisting degradation by reactive oxygen species (ROS), such as 1O2 and superoxide (O2 •−). In this context, computational and experimental approaches for rational molecular design have led to the development of 7,7′-bi-7-azabicyclo[2.2.1]heptane (BAC), a newly suggested RM incorporating N–N interconnected aza-bicycles. BAC harnesses the advantages of falling within the potential range that suppresses 1O2 generation, as previously reported N–N embedded non-bicyclic RMs, and effectively defends against ROS-induced degradation due to the incorporation of a novel bicyclic moiety. Unlike the non-bicyclic RMs, which exhibit reduced O2 evolution after exposure to 1O2, BAC maintains consistent O2 profiles during charging, indicating its superior 1O2 resistance and steady redox-catalyst performance in LOBs. This study introduces a precise and rational design strategy for low-molecular-weight RMs, marking a significant step forward in advancing LOB development by improving efficiency, stability, and practical applicability.

This note responds to Schwartz and Hutchison's Comment. Differences appear to have arisen not in the experimental results themselves but in their interpretation: more extensive experiments allow one to distinguish between “true positive” and “false positive” results. Potential evidence of non-polaritonic effects in Schwartz and Hutchison's own work is identified. It is hoped that this work will encourage others to produce more systematic investigations of strong coupling.

Out-of-plane ferroelectricity is observed in 1T′/1H MoS2 bilayers synthesized via chemical vapor deposition (CVD). The phenomenon is confirmed through structural analysis using scanning transmission electron microscopy (STEM) and second-harmonic generation (SHG), as well as switching behavior characterized by piezoresponse force microscopy (PFM) and ferroelectric tunnel junction (FTJ) measurements. Density functional theory (DFT) calculations reveal that the ferroelectricity originates from interlayer sliding. This discovery extends the scope of 2D ferroelectrics to vertically stacked heterophase systems, offering new opportunities for exploring coupled phenomena in transition metal dichalcogenides (TMDCs).

The emergence of heterophase 2D materials, distinguished by their unique structures, has led to the discovery of a multitude of intriguing physical properties and a broad range of potential applications. Here, out-of-plane ferroelectricity is uncovered in a heterophase structure of 1T′/1H MoS2, which is synthesized via chemical vapor deposition (CVD) by tuning the formation energies for MoS2 with varied phases. The atomically resolved structures of the obtained 1T′/1H MoS2 bilayers are captured using scanning transmission electron microscopy (STEM) and are confirmed to be non-centrosymmetric using second-harmonic generation (SHG) characterizations. The intrinsic out-of-plane polarization is visualized by piezoresponse force microscopy (PFM), which reveals that ferroelectric domains can be manipulated under an applied electric field. Ferroelectric tunnel junction (FTJ) devices fabricated on these bilayers exhibit reversible switching between a high resistance state (HRS) and a low resistance state (LRS). Density functional theory (DFT) calculations elucidate that the intrinsic ferroelectricity in 1T′/1H bilayers is attributed to interlayer sliding and lattice mismatch. The findings not only expand the scope of 2D ferroelectrics to include vertically stacked heterophase bilayers but also open avenues for exploring the coupling effect between ferroelectricity and other phenomena such as magnetism, superconductivity, and photocatalysis in 2D heterophase TMDCs.