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NanoManufacturing

Michael De Volder, Engineering Department - IfM
 
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Table of Contents for Advanced Materials. List of articles from both the latest and EarlyView issues.
Updated: 1 hour 54 min ago

Doping Mo Triggers Charge Distribution Optimization and P Vacancy of Ni2P@Ni12P5 Heterojunction for Industrial Electrocatalytic Production of Adipic Acid and H2

Tue, 01/04/2025 - 15:01

A robust Mo-dopedNi2P@Ni12P5 heterojunction with rich P vacancies on Ni foam is proposed for accomplishing simultaneous electrooxidation of CHA to AA and HER at large current density with 85.7% yield of AA and 100% Faradaic efficiency of H2 production at 232 mA cm−2. Synergistic charge optimization and P vacancy by Mo Doping endows the enhanced bifunctional performances.


Abstract

Synchronous electrosynthesis of value-added adipic acid (AA) and H2 is extremely crucial for carbon neutrality. However, accomplishing the preparation of AA and H2 at large current density with high selectivity is still challenging. Herein, a robust Mo-doped Ni2P@Ni12P5 heterojunction with more P vacancies on Ni foam is proposed for accomplishing simultaneous electrooxidation of cyclohexanol (CHAOR) to AA and hydrogen evolution reaction (HER) at large current density. Combined X-ray photoelectron spectroscopy, X-ray absorption fine structure, and electron spin resonance confirm that Mo incorporation induces the charge redistribution of Ni2P@Ni12P5, where Mo adjusts electrons from Ni to P, and triggers more P vacancies. Further experimental and theoretical investigations reveal that the d-band center is upshifted, optimizing adsorption energies of water and hydrogen on electron-rich P site for boosting HER activity. Besides, more Ni3+ generated from electron-deficient Ni induced by Mo, alongside more OH* triggered from more P vacancies concurrently promote CHA dehydrogenation and C─C bond cleavage, decreasing energy barrier of CHAOR. Consequently, a two-electrode flow electrolyzer achieves industrial current density (>230 mA cm−2) with 85.7% AA yield, 100% Faradaic efficiency of H2 production. This study showcases an industrial bifunctional electrocatalyst for AA and H2 production with high productivity.

Nanosized Multistate Configurations of Relaxor‐Like Antiferroelectric Revealed by Atomic‐Scale In Situ Electron Microscopy

Tue, 01/04/2025 - 14:59

Atomic-scale in situ heating scanning transmission electron microscopy of the (Pb,La)(Zr,Sn,Ti)O3 materials reveals the origin of characteristic hysteresis behavior of relaxor-like antiferroelectric. The nanosized multistate configurations which encompass antiferroelectric, quasi-paraelectric, and ferroelectric nanoregions are responsible for the slim double hysteresis loops of relaxor-like antiferroelectric. Such nanosized multistate configurations break the common belief of single-phase antiferroelectric nanodomains.


Abstract

Antiferroelectric materials have garnered significant attention for their potential applications in high-power capacitors. Among the four technically important types of ferroelectric states-classical ferroelectric, relaxor ferroelectric, antiferroelectric, and relaxor antiferroelectric-the first three have well-defined physical pictures, while the fourth remains contentious. Here, atomic-scale in situ scanning transmission electron microscopy is demonstrated to provide a clear resolution to this long-standing issue. The temperature-dependent configurational evolution during the transition from room-temperature classical antiferroelectric to high-temperature relaxor-like antiferroelectric in (Pb,La)(Zr,Sn,Ti)O3 materials is directly observed. The nanosized multistate configurations formed during transformation, which encompass antiferroelectric, quasi-paraelectric, and ferroelectric nanoregions, are responsible for the slim double hysteresis loops characteristic of relaxor-like antiferroelectric. These findings offer new guidelines for validating the physical models essential for the development of high-performance relaxor-like antiferroelectrics.

A Bioinspired Micro‐Grooved Structure for Low Snow Adhesion and Effective Snow‐Shedding

Tue, 01/04/2025 - 14:58

A bioinspired micro-groove structure is developed to address the challenges of snow and ice accumulation. By minimizing capillary effects, and reducing mechanical interlocking, this multifunctional design highlights two key metrics for snow prevention surfaces: adhesion reduction and shedding efficiency, paving the way for applications in energy systems and architecture.


Abstract

Many outdoor devices require effective snow prevention solutions, yet existing passive anti-icing technologies are inadequate for snow repellency due to the variability of snow properties. This study addresses this gap by proposing a bioinspired micro-grooved anti-snow structure that minimizes van der Waals forces through reduced contact area and mitigates capillary effects via a V-shaped design, facilitating the separation of liquid water at the interface. Snow-shedding performance is shown to be highly sensitive to surface roughness, with the periodic smoothness of micro-grooves significantly reducing mechanical interlocking with snow. In contrast, hierarchical superhydrophobic structures strongly interlock with ice grains, preventing spontaneous snow-shedding even at extremely low adhesion forces. By embedding superhydrophobic nanoparticles into the micro-groove structure, this study presents a multifunctional design that integrates anti-icing, anti-snow, and water-repellent properties. Experimental results demonstrate that the structure effectively balances adhesion reduction and snow-shedding performance, showing promising potential for photovoltaic solar power systems and large-scale architectural applications.

Transforming Healthcare: Intelligent Wearable Sensors Empowered by Smart Materials and Artificial Intelligence

Tue, 01/04/2025 - 14:51

Wearable sensors, empowered by AI and smart materials, revolutionize healthcare by enabling intelligent disease diagnosis, personalized therapy, and seamless health monitoring without disrupting daily life. This review explores cutting-edge advancements in smart materials and AI-driven technologies that empower wearable sensors for diagnostics and therapeutics. Current challenges, limitations, and future opportunities in transforming intelligent healthcare are also examined.


Abstract

Intelligent wearable sensors, empowered by machine learning and innovative smart materials, enable rapid, accurate disease diagnosis, personalized therapy, and continuous health monitoring without disrupting daily life. This integration facilitates a shift from traditional, hospital-centered healthcare to a more decentralized, patient-centric model, where wearable sensors can collect real-time physiological data, provide deep analysis of these data streams, and generate actionable insights for point-of-care precise diagnostics and personalized therapy. Despite rapid advancements in smart materials, machine learning, and wearable sensing technologies, there is a lack of comprehensive reviews that systematically examine the intersection of these fields. This review addresses this gap, providing a critical analysis of wearable sensing technologies empowered by smart advanced materials and artificial Intelligence. The state-of-the-art smart materials—including self-healing, metamaterials, and responsive materials—that enhance sensor functionality are first examined. Advanced machine learning methodologies integrated into wearable devices are discussed, and their role in biomedical applications is highlighted. The combined impact of wearable sensors, empowered by smart materials and machine learning, and their applications in intelligent diagnostics and therapeutics are also examined. Finally, existing challenges, including technical and compliance issues, information security concerns, and regulatory considerations are addressed, and future directions for advancing intelligent healthcare are proposed.

Highly Branched Poly(β‐amino ester)s for Efficient mRNA Delivery and Nebulization Treatment of Silicosis

Tue, 01/04/2025 - 14:30

To address off-target organ enrichment and low endosomal escape during mRNA delivery, the study learns from the technology of lipid nanoparticles (LNPs) and integrate cholesterol moieties and zwitterionic species into branched poly(β-amino ester)s (hPAEs) to obtain “four-in-one” LNP-like hPAEs (O-LhPAEs), which have spleen-targeted delivery and have potential for the treatment of silicosis by nebulization.


Abstract

mRNA therapeutics hold tremendous promise for disease prevention and treatment. Development of high-performance mRNA delivery systems with enhanced transfection efficiency and a safety profile will further fulfill their therapeutic potential and expedite their translation. The synthesis of “four-in-one” highly branched poly(β-amino ester)s (O-LhPAEs) is reported by integrating the essential components of lipid nanoparticles (LNPs) for spleen-selective mRNA enrichment and nebulization treatment of silicosis. 60 O-LhPAEs with distinct branched structure and chemical composition, including tertiary/quaternary amines, cholesterol moieties, zwitterionic species, and hydrophobic alkyl tails, are synthesized using sequential Michael addition, ring-opening, and nucleophilic substitution reactions. The unique topological structure and chemical composition collectively enhanced O-LhPAEs/mRNA polyplex serum resistance, cellular uptake, and endosomal escape. The optimal O-LhPAE, 20%b-3C-2P12, exhibits up to 93.1% mRNA transfection across 11 different cell types, including epithelial cells, fibroblasts, cancer cells, stem cells, neurological cells, and astrocytes. Biodistribution study reveals that 20%b-3C-2P12/mRNA polyplexes are mainly enriched in the spleen following systemic administration. Through nebulization, 20%b-3C-2P12 mediated high Tbx2 mRNA expression in the lungs of silicosis mice, effectively restoring lung functions. This study not only establishes a strategy for development of LNP-like O-LhPAEs but also provides promising candidates for highly safe, efficient, and spleen-selective mRNA delivery and nebulization treatment of silicosis.

Enabling Multicolor Circularly Polarized Organic Long Persistent Luminescence through Chiral Exciplex

Tue, 01/04/2025 - 10:09

Long-lived circularly polarized organic long persistent luminescence (CP-OLPL) is achieved by constructing a chiral exciplex system, with green CP-OLPL emission lasting over 1.5 hours and exhibiting an asymmetry factor of 4.5 × 10− 3. Additionally, by incorporating a fluorophore emitter and utilizing synergistic singlet-singlet and chirality energy transfer, an orange-red CP-OLPL with a duration exceeding 1 hour is realized, showcasing its potential for applications in afterglow display and lighting, and multi-level information encryption.


Abstract

Circularly polarized organic long persistent luminescence (CP-OLPL) has garnered significant attention due to its distinctive properties. However, achieving CP-OLPL materials with ultralong durations remains a formidable challenge. Herein, an effective strategy is proposed to obtain long-lived CP-OLPL by constructing a self-designed chiral donor for developing a host–guest chiral exciplex system. The gradual recombination of long-lived charge-separated states enables a green CP-OLPL emission to persist for over 1.5 hours with an asymmetry factor (|g lum|) of 4.5 × 10−3. More intriguingly, doping with rubrene fluorophore yields an orange-red CP-OLPL system, exhibiting a duration over 1 hour and |g lum| of 2.3 × 10−3 through synergistic singlet-singlet and chirality energy transfer. These properties render the development of chiral afterglow display, multi-level information encryption, and afterglow lighting. This work not only represents a significant advancement in the design of chiral donors for ultralong CP-OLPL exciplex system with durations but also provides valuable insights into exciton dynamics.

Recent Advances in Wide‐Bandgap Perovskite Solar Cells

Tue, 01/04/2025 - 10:03

Ubiquitous defects predominately account for photo-instability and open-circuit voltage losses in wide-bandgap perovskite solar cells (WBG PSCs). This review comprehensively presents the underlying impact mechanisms, summarizes the advanced optimization strategies across various functional layers and their interfaces to develop efficient and stable WBG PSCs, and evaluates their performance in semitransparent solar cells, tandem solar cells, and indoor photovoltaic applications.


Abstract

Wide-bandgap (WBG) perovskite solar cells (PSCs) have garnered considerable attention of late for their potential as semitransparent photovoltaics for building integration, top-cells in tandem configurations, and indoor photovoltaics (IPVs) for Internet of Things (IoT) applications. However, recent investigations have unveiled that underlying defect-mediated phase segregation, ion migration, lattice strain, and other factors can give rise to self-accelerated degradation reactions and the contraction of quasi-Fermi level splitting (QFLS) within devices. Extensive efforts have been undertaken to reduce defect densities in bulks, at surfaces, and across interfaces with charge transport layers (CTLs). This review provides a timely and comprehensive understanding of the intrinsic defect ecosystem in WBG perovskites, and mechanistically elucidates their impacts on device stability and open circuit voltage losses. Subsequently, recent advances in defect passivation strategies are cross-sectionally overviewed, covering various components of devices. The applications of WBG PSCs in semitransparent devices, tandem applications, and IPVs are discussed. Finally, prospects and challenges are proposed, providing insights for future research and technological advancements.

Efficient White Electroluminescence from Cu‐based Perovskite Achieved by High Hole Injection Core/Shell Structures

Tue, 01/04/2025 - 10:01

This study demonstrates a p-type cuprous sulfide lattice connectedly capping over Cs3Cu2I5 to form lattice-matched core/shell nanocrystals by controlling the reactivity of sulfur precursor in the synthesis. The resulting pure white PeLEDs achieved by combining with yellow emission CsCu2I3 exhibit a recorded EQE of 3.45% and a high CRI of 91.


Abstract

The copper-based (Cu-based) halide perovskite possesses eco-friendly features, bright self-trapped-exciton (broadband) emission, and a high color-rendering index (CRI) for achieving white emission. However, the limited hole injection (HI) of Cu-based perovskites has been bottle-necking the efficiency of white electroluminescence and thus their application in white perovskite light-emitting diodes (W-PeLEDs). In this study, we demonstrate a p-type cuprous sulfide (Cu2S) lattice-connectedly capping over Cs3Cu2I5 to form lattice-matched core/shell nanocrystals (NCs) by controlling the reactivity of sulfur (S) precursor in the synthesis. Interestingly, the resultant Cs3Cu2I5/Cu2S NCs significantly enhance the hole mobility compared to Cs3Cu2I5 NCs. Besides, the photoluminescence quantum yield of Cs3Cu2I5 NCs increases from 26.8% to 70.6% after the Cu2S lattice-connected capping. Consequently, by establishing the structure of CsCu2I3/Cs3Cu2I5/Cu2S in W-PeLEDs, an external quantum efficiency of 3.45% and a CRI of 91 is realized, representing the highest reported electroluminescent performance in lead-free Cu-based W-PeLEDs. These findings contribute to establishing guidelines and effective strategies for designing broadband electroluminescent materials and device structures of PeLEDs.

Direct Observation of Unidirectional Exciton Polaritons in Layered van der Waals Semiconductors

Tue, 01/04/2025 - 09:59

Real-space nanoimaging of unidirectional hybridized exciton-polariton (EPs). The resolution to observe near-field SOC can be very high (down to 10 nm) and the contrast can be clearly distinguished at the real-space. The work provides an alternative but more direct approach to uncover the underlying physics of optical SOC and EP properties.


Abstract

Unidirectional excitation of highly confined guided modes is essential for nanoscale energy transport, photonic integrated devices, and quantum information processing. Among various feasible approaches, the mechanism based on optical spin–orbit coupling is investigated for unidirectional routing of surface plasmons and valley exciton-polaritons, without needing the use of complicated magneto-optical effects and parity symmetry breaking. So far, the direct near-field nanoimaging of such exotic polaritonic modes based on optical spin–orbit coupling has remained elusive. Here, the real-space nanoimaging of unidirectional polaritons in van der Waals semiconductors are reported. Specifically, photonic spins are coupled into the tip of a scattering-type scanning near-field optical microscopy for circular dipolar excitations of spin–orbit interactions, thus enabling the unidirectional waveguide exciton-polariton propagation with remarkable unidirectionality (ratio of spectrum amplitudes under opposite circularly polarized illumination) R = 0.291 for TM mode. Via switching to the opposite helicities, the reversed opposite directions are observed. The work offers a promising avenue for detecting and processing spin information for future communication technology at the nanoscale.

Synchronous Sterilization and Immunoreaction Termination for Corneal Transparency Protection in Treating Pseudomonas aeruginosa Induced Bacterial Keratitis

Tue, 01/04/2025 - 09:55

The large-pore MSNs with a high specific surface area serve as a platform for covalent PMB grafting and bactericidal CQD loading. CQD@lMSN-PMB exhibits efficient antibacterial activity alongside synchronous endotoxin neutralization. In Gram-negative bacterial keratitis, CQD@lMSN-PMB effectively and comprehensively suppresses the immune-inflammatory response, preserving corneal integrity and transparency.


Abstract

In the treatment of infectious keratitis, therapeutic strategies often prioritize enhancing bactericidal efficacy. However, endotoxins released from Gram-negative bacteria cause inflammatory reaction, leading to corneal structural damage and scar formation. Given that polymyxin B (PMB) can bind and neutralize lipopolysaccharide (LPS), this study employs large-pore mesoporous silica nanoparticles (lMSNs) grafted with PMB as carriers for cationic antibacterial carbon quantum dots (CQDs) to prepare CQD@lMSN-PMB, which enables synchronous sterilization and endotoxin neutralization. In the acidic infectious microenvironment, the accelerated release of CQDs eliminates 99.88% bacteria within 2 h, effectively substituting immune mediated sterilization. Notably, CQD@lMSN-PMB exhibits exceptional LPS neutralization performance (2.22 µg LPS/mg CQD@lMSN-PMB) due to its high specific surface area. In an infectious keratitis model, inflammation subsides significantly within the first day of CQD@lMSN-PMB intervention and is completely resolved by day 3. By day 2, interleukin-1β, interleukin-6 and tumor necrosis factor-α in CQD@lMSN-PMB group decrease by 86.99%, 91.15%, and 77.56%, respectively, compared to the CQDs-only sterilization group. Ultimately, corneal integrity and transparency are preserved, with suppressed expressions of fibrosis-related factors including matrix metalloproteinase 9, transforming growth factor-β and α-smooth muscle actin. Therefore, this synchronous sterilization and endotoxin neutralization strategy outperforms monotherapy strategies focused solely on sterilization or endotoxin neutralization.

High‐Performance Hybrid Organic‐Inorganic Lanthanide Halide Glass Scintillators Enabled by Dehydration for Efficient X‐Ray Imaging

Tue, 01/04/2025 - 09:54

This study presents an effective strategy for developing high-performance hybrid organic-inorganic lanthanide halide glass scintillators for X-ray imaging through the dehydration of crystalline precursors. This process not only effectively suppresses melt crystallization but also enhances radioluminescence by improving X-ray-to-visible photon conversion efficiency. Thus, it enables the fabrication of large, transparent scintillators suitable for high-resolution X-ray imaging.


Abstract

Although glass scintillators hold great promise for high-resolution X-ray imaging, the practical application is often limited by thermodynamic instability, leading to uncontrolled glass-to-crystal transformations that degrade imaging resolution. Herein, a novel strategy is presented to synthesize (methyl(triphenyl)phosphonium)3EuCl6 ((MTP)3EuCl6) glass scintillators through the dehydration of their crystalline precursors. The findings reveal that the dehydration process significantly enhances the stability of the glass scintillators by confining the constituent ions within a rigid, highly viscous matrix. This confinement effectively restricts ion mobility and prevents the reorganization required for crystal nucleation. Moreover, the dehydration reduces the trapping of in situ generated charge carriers and increases the photoluminescence quantum yield, leading to enhanced radioluminescence performance. The resulting (MTP)3EuCl6 glass scintillators demonstrate an X-ray detection limit as low as 95.8 nGyair s⁻¹ and achieve a spatial imaging resolution of 14.3 lp mm−1 at a dose rate of 5 mGyair s⁻¹. This work provides valuable insights into designing glass scintillators that integrate long-term thermodynamic stability with optimized scintillation performance, offering significant potential for advanced X-ray imaging applications.

Cell‐Sheet Shape Transformation by Internally‐Driven, Oriented Forces

Tue, 01/04/2025 - 09:50

A strategy is implemented to embed dermal fibroblasts in collagen in contact with anisotropic hydrogel fibers. Fibroblasts generate traction forces and remodel the collagen matrix, following the alignment cues of the hydrogel template. The orientational order is transferred to the fibroblasts, inducing collective alignment. Cell alignment generates internally driven, oriented forces that ultimately lead to programmed 2D and 3D shape changes of the cell-laden collagen matrices, such as transforming from square to diamond, or from flat to dome. This approach provides insights into the role of topological defects in morphogenesis and advances new techniques for developing shape-morphing materials with programmable forces.


Abstract

During morphogenesis, cells collectively execute directional forces that drive the programmed folding and growth of the layers, forming tissues and organs. The ability to recapitulate aspects of these processes in  vitro will constitute a significant leap forward in the field of tissue engineering. Free-standing, self-organizing, cell-laden matrices are fabricated using a sequential deposition approach that uses liquid crystal-templated hydrogel fibers to direct cell arrangements. The orientation of hydrogel fibers is controlled using flow or boundary cues, while their microstructures are controlled by depletion interaction and probed by scattering and microscopy. These fibers effectively direct cells embedded in a collagen matrix, creating multilayer structures through contact guidance and by leveraging steric interactions amongst the cells. In uniformly aligned cell matrices, oriented cells exert traction forces that can induce preferential contraction of the matrix. Simultaneously, the matrix densifies and develops anisotropy through cell remodeling. Such an approach can be extended to create cell arrangements with arbitrary in-plane patterns, allowing for coordinated cell forces and pre-programmed, macroscopic shape changes. This work reveals a fundamentally new path for controlled force generation, emphasizing the role of a carefully designed initial orientational field for manipulating shape transformations of reconstituted matrices.

From Molecule to Aggregate: Designing AIE Nanocrystals for Low‐Power Backward Third‐Harmonic Generation Angiography

Tue, 01/04/2025 - 09:48

An organic BTHG agent called OTBP with prominent crystallinity is developed. The resonant absorption at 433 nm and prominent crystallinity of OTBP enhance its BTHG efficiency when excited by a 1300 nm femtosecond laser. Tuning the size of OTBP nanocrystals based on Mie scattering theory successfully enables them to achieve high-contrast muti-organ angiography with ultra-low pulse energy (100 pJ) and thereby negligible photodamage risk.


Abstract

Organic materials featuring third harmonic generation (THG) hold great promise for deep-tissue bioimaging due to their good biocompatibility and second near-infrared excitation. However, minimizing photodamage from the incident light necessitates significant improvements in the third-order nonlinear susceptibility. Herein, an organic luminogen called OTBP is developed as a backward THG (BTHG) contrast agent for second near-infrared (NIR-II) angiography. OTBP's intense absorption at 433 nm resonantly enhances its BTHG efficiency when excited by a 1300 nm femtosecond laser. In the aggregate state, the robust intermolecular interactions among OTBP molecules realize excellent crystallinity and the facile preparation of nanocrystals (NCs) with a high refractive index of 1.78. By leveraging Mie scattering theory, the best size of OTBP NCs for BTHG collection is attained. These integrated properties result in a high BTHG efficiency of OTBP NCs. Encapsulating the NCs with F-127 enables ultralow-power but high-contrast 3D vasculature imaging with negligible photodamage and background interference. Further elevating the laser power to 60 mW enables the visualization of microvessels at 500 µm with a high SNR of 143. This study offers insights into material design strategies toward efficient organic BTHG contrast agents and paves the way for the materials-oriented non-linear optics.

Charge Polarization Tunable Interfaces for Perovskite Solar Cells and Modules

Tue, 01/04/2025 - 09:44

A novel interfacial chemical tuning strategy is proposed involving proton transfer between the amine of pyridoxamine (PM) and the phosphonic acid of Me-4PACz. This process enhances charge delocalization via electrostatic attraction between oppositely charged molecules, yielding a Me-4PACz-PM charge polarization interface that improves NiOx p-type conductivity, facilitates band alignment, and supports high-quality perovskite films, showcasing its commercial potential.


Abstract

Interfacial localized charges and interfacial losses from incompatible underlayers are critical factors limiting the efficiency improvement and market-integration of perovskite solar cells (PSCs). Herein, a novel interfacial chemical tuning strategy is proposed involving proton transfer between the amine head of pyridoxamine (PM) and the phosphonic acid anchoring group of [4-(3,6-dimethyl-9H-carbazol-9-yl)butyl]phosphonic acid (Me-4PACz), with simultaneous enhancement of charge delocalization through electrostatic attraction between opposite charged molecules. The Me-4PACz-PM charge polarization interface modulates the nickel oxide (NiOx) charge states and the coordination environment at buried interfaces, consequently enhancing p-type conductivity and obtaining a more compatible band arrangement. The high-coverage and wettability of the NiOx/Me-4PACz-PM underlayer also facilitate the deposition of high-quality perovskite films, releasing lattice strain and mitigating trap-assisted non-radiative recombination. Attributing to the implementation of charge polarization tunable interfaces, small-area devices and modules with an aperture area of 69 cm2 achieved impressive power conversion efficiencies (PCEs) of 26.34% (certified 25.48%) and 21.94% (certified 20.50%), respectively, and unencapsulated devices maintained their initial PCEs ≈90% after aging for 2000 h (ISOS-L-1) and 1500 h (ISOS-D-1). The broad applicability of charge polarization tunable interfaces and the successful scaling of large-area modules provide a reference for expanding PSCs applications.

Conductive Polymer Coatings Control Reaction Selectivity in All‐Iron Redox Flow Batteries

Tue, 01/04/2025 - 09:01

Aqueous redox flow batteries are limited by the competing hydrogen evolution reaction (HER) at their negative electrodes. In this work, conductive polymers are conformally coated on porous carbonaceous electrodes to improve the reaction selectivity of hybrid all-iron redox flow batteries. Poly(pyrrole)/PSS coating inhibits HER in acidic media and increases the battery lifetime, while PEDOT/PSS electrode improves the roundtrip efficiency.


Abstract

Aqueous all-iron redox flow batteries are an attractive and economic technology for grid-scale energy storage owing to their use of abundant and environmentally benign iron as the redox active material and water as solvent. However, the battery operation is challenged by the plating/stripping reactions of iron and the competing hydrogen evolution reaction at the negative electrode, which hinder performance and durability. Here, the reaction selectivity of the negative electrode is tailored by introducing conductive polymer coatings onto porous carbonaceous electrodes. Two conductive polymers, poly(3,4-ethylenedioxythiophene) (PEDOT) and poly(pyrrole) (PPy) are conformally coated with the dopant poly(4-styrenesulfonate) (PSS) and the resulting electrochemistry is studied on model electroanalytical platforms and redox flow batteries. Both polymers decrease the hydrogen evolution current on rotating disc electrodes, with PPy/PSS strongly inhibiting the reaction at high overpotentials. In full all-iron redox flow cells, PPy/PSS coating extends cyclability and significantly reduces hydrogen evolution, while PEDOT/PSS coating improves the round-trip efficiency, possibly acting as a redox shuttle for the iron stripping reaction. These findings motivate broader investigation and implementation of conductive polymers to engineer reaction selectivity for flow batteries and other electrochemical technologies.

Metal‐polyphenol Multistage Competitive Coordination System for Colorimetric Monitoring Meat Freshness

Tue, 01/04/2025 - 09:00

This research proposes a multistage competitive coordination chromogenic mechanism between metal-polyphenols and amines. Based on this, a metal-polyphenol network colorimetric sensor array (MPN-CSA) for real-time monitoring of meat freshness has been developed, achieving a detection rate of 99.83% through convolutional neural network technology. This sensitive, accurate, stable, eco-friendly, and economical solution can enhance food safety and reduce food waste.


Abstract

A low-cost, high-precision, and secure real-time system for monitoring food freshness can significantly improve spoilage issues, yet traditional colorimetric sensor arrays often suffer from chemical dyes’ high toxicity and limited color changes. Here, a metal-polyphenol network colorimetric sensor array (MPN-CSA) is built for detecting total volatile base nitrogen (TVB-N) markers of meat freshness. The multi-level competitive coordination process between the metal-polyphenol system and amine substances endows the system with color changes far beyond those of traditional dyes (reaching a detection limit of 300 ppb). By integrating convolutional neural network (CNN) technology, an online platform is developed for monitoring meat freshness, achieving an overall detection accuracy rate of 99.83%. This environmentally friendly, economically viable MPN-CSA that monitors the freshness of meat in complex storage environments can be incorporated into food packaging boxes, enabling consumers and suppliers to assess the freshness of meat in real-time, thus helping to reduce food waste and prevent foodborne illnesses.

In Situ Construction of a 3D Superionic Skeleton in Sodium Anode for Solid‐State Sodium Batteries with a 15 000‐Cycle Lifespan at 3C

Mon, 31/03/2025 - 08:44

In this work, a 3D superionic transport skeleton Na3P is in situ constructed within the sodium anode, which successfully enhances the ion diffusion coefficient of the anode from 2.54 × 10‒8 to 1.33 × 10‒7 cm2 s‒1. Thanks to the ultrafast ion transport and excellent interfacial stability, the solid-state sodium-metal battery can be stably cycled for more than 15 000-cycle at 3C.


Abstract

Solid-state sodium-metal batteries (SSSMBs) have emerged as a promising candidate for next-generation energy storage systems due to their natural abundance, cost-effectiveness, and high safety. However, the intrinsically low ionic conductivity of sodium anode (SA) and poor wettability to solid-state electrolyte (SSE) severely hinder the development of SSSMBs. In this study, a 3D superionic transport skeleton Na3P is in situ constructed within the sodium anode by simply melting inexpensive and low-density red phosphorus with sodium, which successfully enhances the ion diffusion rate from 2.54 × 10‒8 to 1.33 × 10‒7 cm2 s‒1. Moreover, Na3P in the composite sodium anode (CSA) effectively induces the uniform deposition of Na on the surface of SSE, significantly reducing the interface impedance of symmetric cells from the initial value of 749.15 to 14.97 Ω cm2. Enabled by the integrated 3D superionic transport skeleton, the symmetric cell achieves exceptional cycle stability of over 7000 h at 0.1 mA cm‒2 and 4000 h at 0.3 mA cm‒2. Furthermore, SSSMBs incorporating CSA demonstrate an ultralong lifespan of over 15 000 cycles at 3C while maintaining a high-loading operation capability, significantly outperforming previously reported studies. This study highlights the crucial role of cost-effective CSA design with enhanced ion transport in advancing high-performance SSSMBs.

Wettability Sequence Optimization and Interface Strain Buffering in Triple Mesoporous Layer‐Based Printable Perovskite Solar Cells for Enhanced Performance

Mon, 31/03/2025 - 08:35

The interface in printable mesoscopic perovskite solar cells is regulated via the flexible molecule of dodecaethylene glycol (DEG) with abundant polar oxygen atoms. The regulation modulated the wetting sequence of the scaffold, promoted perovskite crystallization in the scaffold, and relaxed interface stress. The device with interface regulation successfully achieved an improved power conversion efficiency of 20.27% and demonstrated good stability.


Abstract

Perovskite solar cells have achieved remarkable progress in photovoltaic performance, driven by advancements in interface engineering. The buried interface between the electron transport layer and the perovskite layer is particularly critical, as it governs both perovskite crystallization and the formation of residual strain. In this study, the buried interface in printable mesoscopic perovskite solar cells (p-MPSCs) based on a triple-mesoporous scaffold of TiO2/ZrO2/carbon is reconstructed by employing dodecaethylene glycol (DEG), a long chain molecule rich in polar oxygen atoms, to enhance device performance. Treating the scaffold with DEG optimizes the wettability sequence across the three layers by improving the TiO2 surface's wettability, facilitating the preferential crystallization of perovskite in the underlying TiO2 layer. Moreover, the DEG layer effectively buffers residual strain and suppresses detrimental defects at the interface. As a result, p-MPSCs with the optimized interface achieve a power conversion efficiency (PCE) of 20.27% and retain over 92% of their initial PCE after 500 h of continuous operation under maximum power point tracking.

Optothermal‐Stimulated Persistent Luminescence Imaging and Therapy (OSPLIT)

Mon, 31/03/2025 - 08:29

This study reports an effective strategy, OSPLIT (optothermal-stimulated persistent luminescence imaging and therapy), which enables high-contrast imaging and the thermal ablation of lymph node metastases. The rational design of these nanomaterials is detailed and mechanistic insights are provided, demonstrating the advantages of optothermal-stimulated NIR-II persistent luminescence in lanthanide-doped nanoparticles over conventional NIR-II fluorescence imaging.


Abstract

Persistent luminescent nanomaterials have significantly advanced in vivo bioimaging and biosensing by emitting photons after excitation ceases, effectively minimizing tissue autofluorescence. However, their application in biomedical fields such as tumor theranostics is limited by low brightness and rapid signal decay. To address these issues, OSPLIT (optothermal-stimulated persistent luminescence imaging therapy), a dual-function strategy for imaging and treatment is introduced. The OSPLIT approach enhances the release of charge carriers from deep traps in lanthanide-doped nanoparticles, resulting in a 73 fold increase in persistent luminescence within the second near-infrared (NIR-II) window. In living mice, it enables high-contrast imaging of lymph node metastases, with a signal-to-background ratio 11.8 times greater than conventional NIR-II fluorescence. Optothermal-boosted nanoparticles are effective in ablating lymph node metastasis and preventing tumor spread. These findings highlight the potential of optothermal stimulation to enhance persistent luminescence for both imaging and therapeutic applications.

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