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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: 26 min 40 sec ago

Integrating Strong Luminescence and High Mobility in Organic Single Crystals of Covalent Pyrene Dimers

Mon, 17/03/2025 - 10:30

Both high photoluminescence quantum yield (PLQY = 72.17%) and high hole mobility (µ = 32.6 cm2 V−1 s−1) are simultaneously harvested in the single crystal of covalent pyrene dimer, which is substantially ascribed to the strong emission from intramolecular hybridized local and charge−transfer state and the 2D charge transport enabled by the intermolecular uniform herringbone stacking.


Abstract

Simultaneously achieving strong luminescence and high mobility in organic semiconductors remains a challenge. Herein, two covalently dimerized pyrene derivatives (1Py-2Py and 1Py-1Py) with distinct chemical linkages and crystal packing arrangements are presented. Remarkably, the radiative transition of pyrene is gradually unforbidden from 1Py-2Py to 1Py-1Py. Moreover, 1Py-2Py showcases 1D long-range π─π stacking, while 1Py-1Py exhibits 2D herringbone packing formed by a vast network of intermolecular C─H∙∙∙π interactions. To the surprise, both high photoluminescence quantum yield (PLQY = 72.17%) and high hole mobility (µ = 32.6 cm2 V−1 s−1) are simultaneously harvested in 1Py-1Py crystal, which are far superior to those in 1Py-2Py crystal (PLQY = 48.66% and µ = 0.05 cm2 V−1 s−1). These findings underscore the potential of covalent pyrene dimer with 1-position linkages as a promising organic semiconductor for the exceptional combination of strong luminescence and high mobility, which is substantially ascribed to the efficiently unforbidden emission and the favorable 2D charge transport pathways.

High Cell to Module Efficiency Remaining Ratio of ≈90% for the 100 cm2 Fully Roll‐to‐Roll Gravure Printed Flexible Organic Solar Cells From Non‐Halogenated Solvent

Mon, 17/03/2025 - 10:30

This work gives an insight into solvent-dependent rheology properties and phase separation dynamics for the R2R printing of flexible organic solar cells. With o-XY solvent, the fully R2R gravure-printed 1 and 28–104 cm2 large-area modules give efficiencies of 14.67% and over 13%, respectively, with a high cell-to-module remaining ratio of 0.9 during upscaling.


Abstract

The cell-to-module (CTM) efficiency remaining ratio from monolithic device to large-area module indicates the scalability potential for large-area organic solar cells (OSCs). Nowadays, the CTM value is still low as the area increases to larger than 100 cm2. In this work, the crucial role of solvent in CTM for printing, which on one side influenced the large area homogeneity due to the ink rheology property, and on the other side impacted phase separation dynamics because of vaporization and crystalline rate is highlighted. The films from TMB show excessive pure phase and printing line defects in vertical the printing direction due to slow volatilization speed and low adhesion, while Tol-based films present printing line defects along the printing direction due to large surface adhesion are demonstrated. In contrast, the films from non-halogenated solvent, o-XY exhibited a suitable phase separation size and excellent large-area homogeneity. Consequently, the fully printed 1 cm2 FOSCs exhibit an efficiency of 14.81%. Moreover, the FOSCs module with an area of 28–104 cm2 gives an efficiency of over 13%, with a CTM of 0.9. Selecting suitable non-halogenated solvents to achieve large-area uniformity and appropriate phase separation morphology in >100 cm2 modules is of great importance for the industrialization of FOSCs.

Translational Selenium Nanoparticles Promotes Clinical Non‐small‐cell Lung Cancer Chemotherapy via Activating Selenoprotein‐driven Immune Manipulation

Mon, 17/03/2025 - 10:29

This study, for the first time, highlights the translational SeNPs-enhanced therapeutic efficacy against advanced NSCLC and elucidates the underlying mechanisms involving selenoprotein-driven immune manipulation. The clinical Investigator-initiated Trial shows that translational SeNPs supplementation in combination with bevacizumab/cisplatin/pemetrexed exhibits enhanced therapeutic efficacy with an objective response rate of 83.3% and a disease control rate of 100%, through potentiating selenoprotein-driven antitumor immunity.


Abstract

Reconstructing the tumor immune microenvironment is an effective strategy to enhance therapeutic efficacy limited by immunosuppression in non-small-cell lung cancer (NSCLC). In this study, it is found that selenium (Se) depletion and immune dysfunction are present in patients with advanced NSCLC compared with healthy volunteers. Surprisingly, Se deficiency resulted in decreased immunity and accelerated rapid tumor growth in the mice model, which further reveals that the correlation between micronutrient Se and lung cancer progression. This pioneering work achieves 500-L scale production of Se nanoparticles (SeNPs) at GMP level and utilizes it to reveal how and why the trace element Se can enhance clinical immune-mediated treatment efficacy against NSCLC. The results found that translational SeNPs can promote the proliferation of NK cells and enhance its cytotoxicity against cancer cells by activating mTOR signaling pathway driven by GPXs to regulate the secretion of cytokines to achieve an antitumor response. Moreover, a clinical study of an Investigator-initiated Trial shows that translational SeNPs supplementation in combination with bevacizumab/cisplatin/pemetrexed exhibits enhanced therapeutic efficacy with an objective response rate of 83.3% and a disease control rate of 100%, through potentiating selenoprotein-driven antitumor immunity. Taken together, this study, for the first time, highlights the translational SeNPs-enhanced therapeutic efficacy against clinical advanced NSCLC.

Metalloenzyme‐Inspired Cluster Fabrication within Mesoporous Channels Featuring Optimized Catalytic Microenvironments for Efficient Neutral pH H2O2 Electrosynthesis

Mon, 17/03/2025 - 10:28

Inspired by some metalloenzymes, bismuth metal clusters are used as active sites and coupled with mesoporous channels to create a favorable catalytic microenvironment, enabling efficient electrocatalysis of the two-electron oxygen reduction reaction in neutral media, with an industrially relevant current density and an exceptional H2O2 production rate of 21.4 mol gcatalyst −1 h−1 over 120 h.


Abstract

In nature, some metalloenzymes facilitate highly efficient catalytic transformations of small molecules, primarily attributed to the effective coupling between their metal cluster active sites and the surrounding microenvironment. Inspired by this, a thermotropic redispersion strategy to incorporate bismuth nanoclusters (Bi NCs) into mesoporous channels, mimicking metalloenzyme-like catalysis to enhance the two-electron oxygen reduction reaction (2e− ORR) for efficient neutral pH H2O2 electrosynthesis, is developed. This model electrocatalyst exhibits exceptional 2e− ORR performance with >95% H2O2 selectivity across 0.2–0.6 V vs RHE in neutral electrolyte. Notably, the system produces up to 7.2 wt% neutral H2O2 solution at an industrially relevant current density of ≈320 mA cm−2, with 90% Faradaic efficiency for H2O2 over 120 h in a flow cell, demonstrating significant practical potential. Mechanistic insights reveal that the introduction of Bi NCs enhances the adsorption of the *OOH intermediate, facilitating a highly active 2e− ORR process. Moreover, the mesoporous channels of the carbon support create a favorable catalytic microenvironment for O2 aeration and local alkalinity, further boosting H2O2 productivity. This catalyst design mimics metalloenzymes by optimal integration of the active site with the surrounding microenvironment, offering valuable insights for the rational design of nature-inspired small-molecule catalysts.

Constructing Biomimetic Nanochannels for High‐Capacity Capture of Uranyl Tricarbonate Complex Ions

Mon, 17/03/2025 - 10:25

Various quaternary ammonium monomers with lengths of 6.2–8.4 Å are decorated on 1D porous channels of the TpBDOH framework to obtain biomimetic nanochannels for [UO2(CO3)3]4− ions. The unique structure enabled a selective capture of [UO2(CO3)3]4− ions from natural seawater, achieving a high uptake of 25.3 mg g−1 in 35 days.


Abstract

Biomimetic nanochannels enable fast and selective transport of mononuclear metal ions; however, their construction for complex ion transport remains in its infancy due to the nonuniform charge distribution and large geometric dimensions of coordination compounds. Herein, an ionic electrostatic interaction template strategy is proposed to prepare biomimetic channels for the capture of complex ions. Using the [UO2(CO3)3]4− ion as a template, various quaternary ammonium monomers with lengths of 6.2−8.4 Å are decorated on 1D porous channels of the TpBDOH framework via the Williamson ether reaction. Accordingly, the pore size is modulated in the sub-nanometer range of 9−13 Å, facilitating multiple electrostatic attractions between quaternary ammonium fragments and the three equatorial carbonate ions on the [UO2(CO3)3]4− ion. The unique structure enabled highly efficient uranium adsorption with a capacity of 501.5 mg g−1 and a high selectivity coefficient for uranium over vanadium of >163.1. The resulting electropositive nanochannels selectively captured [UO2(CO3)3]4− ions from natural seawater, achieving a high uptake of 25.3 mg g−1 in 35 days.

Electromagnetically Heating and Oscillating Liquid Metal for Catalyzing Polyester Depolymerization

Mon, 17/03/2025 - 10:24

Gallium-based liquid metal alloys provide dynamic interactions between the catalyst and reactants, spontaneous metal enriching, and oxidation within their surface layers. Under alternating electromagnetic fields, these alloys can serve as the efficient self-heater, mechanic disturber, and catalyst for thermolysis depolymerization of polycaprolactone with a rate ≈700 mg h−1 mL−1 and monomer selectivity ≈95.5%, offering an unprecedented “all-in-one” platform for continuous polyester depolymerization.


Abstract

Depolymerization and recycling of polyesters have shown great significance to economy, ecology, carbon neutrality and human health. Efficient catalysts for thermolysis depolymerization have long been pursued to achieve rapid depolymerization, high selectivity, and low energy consumption. In this study, it is found that liquid metal (LM) can serve as the efficient self-heater, mechanic disturber and catalyst for thermolysis depolymerization of polyesters under alternating electromagnetic fields. When dissolving different metals (e.g., Sn, Zn, Al, and Mg) into gallium, LMs may provide dynamic interactions between the catalyst and reactants, spontaneous metal enriching, and oxidation within the LM surface layer. Without any conventional heaters and mechanic shakers, polycaprolactone is catalytically depolymerized into ɛ-caprolactone at the rate of ≈700 mg h−1 mL−1 with the selectivity of 95.5%. The high surface tension and high mobility of LM also enable continuous depolymerization at an appropriate feeding speed of polyesters (including polyethylene terephthalate, polyhydroxybutyrate and polylactic acid). Thus, this study may offer an unprecedented “all-in-one” platform of liquid metal for continuous thermolysis depolymerization of polyesters, while without any requirement of external heater, mixer, and catalysts.

Anion Vacancies Coupling with Heterostructures Enable Advanced Aerogel Cathode for Ultrafast Aqueous Zinc‐Ion Storage

Mon, 17/03/2025 - 10:24

Inspired by DFT calculations, a novel 3D sulfur vacancy-rich and heterostructured MnS/MXene aerogel is designed based on the synergistic modification strategy of sulfur vacancies and heterostructures, and utilized as a cathode for ZIBs/ZICs for the first time, achieving significantly enhanced electrochemical performance. Meanwhile, systematic kinetic analyses, ex situ characterizations, and DFT calculations are utilized to reveal the phase transition mechanism.


Abstract

As a potential cathode material, manganese-based sulfide has recently attracted increasing interest due to its many advantages in aqueous zinc-ion storage. Unfortunately, some challenges such as sluggish kinetics, unstable structure, and controversial phase transition mechanism during the energy storage process hinder its practical application. Herein, inspired by density functional theory (DFT) calculations, a novel 3D sulfur vacancy-rich and heterostructured MnS/MXene aerogel is designed, and used as a cathode for aqueous Zn-ion batteries/hybrid capacitors (ZIBs/ZICs) for the first time. Thanks to the synergistic modification strategy of sulfur vacancies and heterostructures, the as-constructed MnS/MXene//Zn ZIBs exhibit significantly enhanced electrochemical properties, especially outstanding rate capability and cyclic stability. More encouragingly, the as-assembled MnS/MXene//porous carbon (PC) ZICs exhibit an ultrahigh energy density, a high power density, and a splendid cycling lifespan. Most notably, systematic kinetic analyses, ex situ characterizations, and DFT calculations illustrate that MnS/MXene first irreversibly converts into MnOx@ZnMnO3/MXene, and then undergoes a reversible conversion from MnOx@ZnMnO3/MXene to MnOOH@ZnMn2O4/MXene, accompanied by the co-insertion/extraction of H+ and Zn2+. The synergistic modification strategy of sulfur vacancies and heterostructures and the thorough mechanistic study proposed in this work offer valuable guidance for designing and exploiting high-performance cathodes in aqueous zinc-based energy storage devices.

Ultra‐Flexible Pixelated Perovskite Photodetectors Enabled by Honeycomb Polymer Grids for High‐Resolution Imaging

Mon, 17/03/2025 - 07:15

Nature-inspired, photolithography-free, flexible, pixelated perovskite photosensitive films serve not only as a high-resolution pixelation platform but also as a stress-relief mechanism for otherwise brittle perovskite films, enabling enhanced mechanical flexibility. This synergetic approach yields pixelated perovskite layers with ≈1.5 µm pixel sizes, ≈100 nm gaps, and 2000 PPI resolution. Assembled photodetector arrays offer detectivity greater than 1013 Jones with cross-talk-free imaging. The flexible polymer grid also enhances mechanical durability, expanding potential applications in robotics, biomedical imaging, and virtual/augmented reality.


Abstract

A nature-inspired fabrication method based on a photolithography-free flexible polymer grid is reported for high-resolution pixelation of perovskite photodiode arrays with exceptional mechanical ductility and a morphology resembling that of natural compound eyes. The resulting pixelated perovskite photosensitive layer has a ≈1 µm pixel size with 2000 Pixels per inch (PPI) resolution when fully assembled as a photodetector array, delivering a detectivity of >1013 Jones while providing cross-talk free imaging. Using a polymer grid effectively releases stress on the perovskite platform, greatly increasing the mechanical agility of the otherwise brittle perovskite film. This novel fabrication methodology and device design offer new possibilities for applications in robotics, biomedical imaging, and virtual and augmented reality.

Dual Oxidation Suppression in Lead‐Free Perovskites for Low‐Threshold and Long‐Lifespan Lasing

Mon, 17/03/2025 - 07:15

A dual oxidation suppression strategy is developed to suppress the Sn2+ oxidation in 2D tin perovskites, i.e. adopting an oxygen-free two-step growth to enhance the crystal quality and incorporating electron-donating biuret molecules to coordinate with Sn2+. As a result, nanolasers based on these tin perovskite flakes exhibited an ultralow lasing threshold of <1 µJ cm−2 and superior lasing stability.


Abstract

Low lasing threshold and long-term operational stability are essential in advancing cost-effective, efficient lead-free (tin) halide perovskite lasers. However, the rapid crystallization of tin perovskites and oxidation of Sn2+ lead to substantial amounts of lattice defects, detrimental to laser performance enhancement. Herein, a dual oxidation suppression strategy is developed to suppress the oxidation of Sn2+ 2D tin halide perovskites, i.e., adopting an oxygen-free two-step growth to enhance the crystal quality and incorporating electron-donating biuret molecules to coordinate with Sn2+ during the crystal growth, which led to the substantial reduction of lasing threshold to <1 µJ cm− 2 in (PEA)2MASn2I7. This represents the lowest value in lead-free perovskite nanolasers and approximately one order of magnitude lower than those previously reported for tin-based nanolasers. Investigations into the spontaneous photoluminescence (PL) and stimulated lasing emission revealed that 2D tin perovskites exhibited superior photostability and lasing stability compared to their lead counterparts. Specifically, the lasing intensity of (PEA)2MA2Sn3I10 constantly increased by >300% under optical pumping and the lasing threshold decreased by ≈17%, which is not observed in their lead counterparts. The findings highlight the prospect of 2D tin halide perovskites as lead-free gain materials and cavities for solution-processed nanolasers with low lasing thresholds and exceptional stability.

High‐Entropy High‐Temperature High‐Piezoelectricity Ceramics

Mon, 17/03/2025 - 06:55

The introduction of a high-entropy strategy into CaBi2Nb2O9 achieves significant breakthroughs in piezoelectric and ferroelectric performance by designing local polarization configuration and defect structure, which causes the formation of high-density 2D amorphous defect, contributing to extra out-of-plane polarization components. This work provides a widely applicable paradigm for designing more novel high-performance bismuth layer-structured ferroelectrics.


Abstract

High-temperature piezoelectric materials are essential components of transducers and accelerometers applied in the fields of aircraft engines, automobiles, nuclear power units, etc., yet how to achieve large piezoelectricity accompanied by high Curie temperature and superior resistivity is still a big challenge. Here, the high-entropy strategy is utilized to design bismuth-layer high-temperature piezoelectric ceramics, resulting in an excellent comprehensive piezoelectric performance with a record-high figure of merit (d 33 * T C) and a high electrical DC resistivity of 1.0 × 106 Ω cm at 750 °C. High-energy synchrotron X-ray diffraction and transmission electron microscopy results suggest that there is no significant change in long-range average orthorhombic structure through high-entropy engineering, providing a structural basis for retaining a high T C. Encouragingly, highly dense bismuth-layer vacancies occupied by alien atoms trigger extra unique out-of-plane polarization in perovskite layers around these 2D amorphous defects, as confirmed by quantitative analysis of local polarization configurations and density functional theory calculations. Together with the decreased polarization reversal energy barrier, the high entropy strategy benefits polarization flexibility under external stimulation and offers breakthroughs in electrical properties. This work provides new insight into the improvement of comprehensive functional properties through the cocktail effect and structure mechanism for designing novel high-entropy materials.

Formulation and Characterization of Novel Ionizable and Cationic Lipid Nanoparticles for the Delivery of Splice‐Switching Oligonucleotides

Mon, 17/03/2025 - 06:53

Lipid nanoparticles (LNPs) of unconventional composition and defined structures are investigated as small oligonucleotide carriers. A composition is identified that outperforms Onpattro in cargo delivery to HeLa cells. The structure of these LNPs resembles a micellar cubic phase not commonly associated with high-performing LNPs. The results shed light on the LNP structure-function relationship and highlight the complexity of these platforms.


Abstract

Despite increasing knowledge about the mechanistic aspects of lipid nanoparticles (LNPs) as oligonucleotide carriers, the structure-function relationship in LNPs has been generally overlooked. Understanding this correlation is critical in the rational design of LNPs. Here, a materials characterization approach is utilized, applying structural information from small-angle X-ray scattering experiments to design novel LNPs focusing on distinct lipid organizations with a minimal compositional variation. The lipid phase structures are characterized in these LNPs and their corresponding bulk lipid mixtures with small-angle scattering techniques, and the LNP-cell interactions in vitro with respect to cytotoxicity, hemolysis, cargo delivery, cell uptake, and lysosomal swelling. An LNP is identified that outperforms Onpattro lipid composition using lipid components and molar ratios which differ from the gold standard clinical LNPs. The base structure of these LNPs has an inverse micellar phase organization, whereas the LNPs with inverted hexagonal phases are not functional, suggesting that this phase formation may not be needed for LNP-mediated oligonucleotide delivery. The importance of stabilizer choice for the LNP function is demonstrated and super-resolution microscopy highlights the complexity of the delivery mechanisms, where lysosomal swelling for the majority of LNPs is observed. This study highlights the importance of advanced characterization for the rational design of LNPs to enable the study of structure-function relationships.

Triplet State Suppression for Energy Loss Reduction in 20% Nonhalogenated Solvent Processed Binary Organic Solar Cells

Mon, 17/03/2025 - 06:51

Asymmetric small molecule acceptor with a methoxylated end group is produced here, whose oxygen vibration is found effective in suppressing triplet state formation, thereby minimizing non-radiative energy loss for 20% efficiency in nonhalogenated solvent cast binary organic solar cells.


Abstract

Boosting power conversion efficiency (PCE) of organic solar cells (OSCs) has been restricted by its undesirably high energy loss, especially for those nonhalogenated solvent-processed ones. Here,a dichloro-methoxylated terminal group in an asymmetric small molecular acceptor design, which realizes a significantly reduced non-radiative energy loss (0.179 eV) compared to its symmetric counterpart (0.202 eV), is reported. Consequently, the device efficiency is improved by up to 20% for PM6:BTP-eC9-4ClO, without sacrificing the photon harvest or charge transport ability of the control system PM6:BTP-eC9. Further characterizations reveal the asymmetric acceptor BTP-eC9-4ClO's blend film demonstrates a suppressed triplet state formation, enabled by an enhanced electron delocalization. In addition, the asymmetric BTP-eC9-4ClO is found to be thermally stabler than BTP-eC9, and thus providing an improved device stability, whose T80 value reaches > 7800 h under 80 °C anneal in N2 via linear extrapolation. This work represents state-of-the-art device performance for nonhalogenated solvent-processed binary OSCs with certified results (19.45%).

The Large‐Scale Manufacturing of Polymer Dielectric Capacitors: Advancements and Challenges

Mon, 17/03/2025 - 06:45

Polymer dielectric capacitors are widely used in microelectronics to industrial systems, such as oil extraction and electronic circuits, due to their good reliability, excellent voltage endurance, and minimal dissipation factor. This review examines persistent challenges in scaling laboratory innovations to industrial production, with particular emphasis on polymer dielectrics in the laboratory as well as developments in capacitor manufacturing processes.


Abstract

Since the 18th century, capacitors have significantly advanced in theoretical research and industrial applications. With the increasing demand for high-performance capacitors, the focus on advanced materials and manufacturing techniques has become critical. This review aims to provide a comprehensive survey of polymer capacitors, emphasizing their manufacturing processes and the connection between theoretical research and practical applications. Beginning with the fundamental principles of dielectric materials and capacitor design, this review delves into key aspects such as material preparation, film fabrication, and capacitor assembly while addressing the challenges in scale-up manufacturing for practical usage. Special attention is given to the metallization and winding processes, as these are pivotal for ensuring high reliability and performance in polymer capacitors. Additionally, this review analyzes the growing market demand for capacitors with enhanced thermal stability and operational efficiency, identifying research directions to address current limitations. By integrating the latest advancements in high-temperature polymer dielectrics, this review aims to provide valuable insights for both academia and industry. Finally, a forward-looking perspective is provided on future development trends and the obstacles that lie ahead, emphasizing the necessity for stronger collaboration between research and industry to foster innovation in this vital field.

An Adaptive Solid‐State Synapse with Bi‐Directional Relaxation for Multimodal Recognition and Spatio‐Temporal Learning

Mon, 17/03/2025 - 06:44

A purely electric-modulated ferroelectric tunnel junction synapse capable of multimodal recognition and spatiotemporal learning has been successfully designed. Its unique functionality is achieved by integrating volatile oxygen vacancy migration and the nonvolatile polarization switching mechanisms within a single device, providing bidirectional relaxation and adaptive long-term plasticity characteristics, which are essential for multimodal recognition and spatiotemporal learning, respectively.


Abstract

The brain's unique processing power, such as perception, understanding, and interaction with the multimodal world, is achieved through diverse synaptic functionalities, which include varied temporal responses and adaptation. Although specific functions in brain-like computing have been successfully realized, emulating multimodal recognition and spatio-temporal learning remain significant challenges due to the difficulties in achieving multimodal signal processing and adaptive long-term plasticity in a single electronic synapse. Here, a purely electrically-modulated ferroelectric tunnel junction (FTJ) memristive synapse which realizes multimodal recognition and spatio-temporal pattern identification, through the integration of oxygen vacancies migration and ferroelectric polarization switching mechanisms, providing bi-directional relaxation and adaptive long-term plasticity simultaneously in the isolated device. The bi-directional relaxation enables multimodal recognition in the purely electrically-modulated FTJ device by encoding distinct sensory signals with different electrical polarities. The multimodal perception task is implemented with a multimodal computing system combining visual and speech pattern recognition. Moreover, the adaptive long-term plasticity allows spatio-temporal pattern recognition, which is demonstrated by identifying object orientation and direction of motion with a neural network incorporating the arrayed synapses. This work provides a feasible approach for designing bio-realistic electronic synapses and achieving highly intelligent neuromorphic computing.

High‐Entropy Metal Sulfide Nanocrystal Libraries for Highly Reversible Sodium Storage

Mon, 17/03/2025 - 06:44

Employing a two-step synthesis approach, a library of high-entropy metal sulfide (HEMS) materials spanning quinary to duodenary compositions are built by arbitrarily combining 5–12 elements from 28 candidates in the periodic table. The septenary HEMS particles exhibit remarkable cycling stability—retaining≈230 mAh g−1 over 3000 cycles—attributed to uniform metal mixing during discharge.


Abstract

Controlled synthesis of high-entropy materials offers a unique platform to explore unprecedented electrochemical properties. High-entropy metal sulfides (HEMSs) have recently emerged as promising electrodes in electrochemical energy storage applications. However, synthesizing HEMSs with a tunable number of components and composition is still challenging. Here, a HEMS library is built by using a general synthetic approach, enabling the synthesis of HEMS with arbitrary combinations of 5 to 12 out of 28 elements in the periodic table. The formation of a solid solution of HEMS is attributed to the two-step method that lowers the energy barrier and facilitates the sulfur diffusion during the synthesis. The hard soft acid base (HSAB) theory is used to precisely describe the conversion rates of the metal precursors during the synthesis. The HEMSs as cathodes in Na-ion batteries (SIBs) is investigated, where 7-component HEMS (7-HEMS) delivers a promising rate capability and an exceptional sodium storage performance with reversible a capacity of 230 mAh g−1 over 3000 cycles. This work paves the way for the multidisciplinary exploration of HEMSs and their potential in electrochemical energy storage.

In Situ Cross‐Linking and Interfacial Engineering via Multifunctional Diamine Additive for High‐Temperature Magnesium Metal Batteries

Mon, 17/03/2025 - 06:30

A robust in situ cross-linked polymer electrolyte and its derived Mg3N2-rich bilayer interphase are obtained by a multifunctional diamine additive. The assembled Mo6S8//Mg cells demonstrate stable cycling over 200 cycles at 150 °C with 80% capacity retention.


Abstract

The electrolyte and its interfacial chemistry are crucial for the development of high-temperature magnesium metal batteries. Here, a robust in situ cross-linked gel polymer electrolyte (MgB@CGPE) and its derived Mg3N2-rich (Mg3N2 and related Mg─N─H complexes) interphase are obtained by a multifunctional diamine additive. The Mg3N2-rich interphase exhibits low magnesium ion migration activation energy and can effectively inhibit the continuous decomposition of electrolyte at the interface under elevated temperatures. Moreover, the MgB@CGPE can enable reversible magnesium deposition and dissolution over a wide temperature range of 30–180 °C. The assembled Mo6S8//MgB@CGPE//Mg cells demonstrate stable cycling over 200 cycles at 150 °C with 80% capacity retention. Additionally, these cells also address crucial mechanical and thermal safety concerns, indicating their potential for use under extreme conditions. This work presents a universal and practical strategy for designing polymer electrolytes that operate at elevated temperatures.

Manipulating Molecular Stacking for Semitransparent Organic Photovoltaics Achieving Light Utilization Efficiency >6%

Mon, 17/03/2025 - 06:23

Through delicate design of host-guest active layer, the hydrogen bonding interactions between host donor D18 and guest BTO-BO facilitate the formation of predominant J-type stacking of D18 during crystallization, significantly reducing visible absorption and enhancing hole transport. The resultant ST-OSCs with optical modulation achieved record light utilization efficiencies of 6.02%, while also demonstrating excellent flexibility and scalability.


Abstract

The trade-off between average visible transmittance (AVT) and power conversion efficiency (PCE), governed by the molecular stacking of the donor and acceptor materials in semitransparent organic solar cells (ST-OSCs), significantly constrains improvements in light utilization efficiency (LUE). Here, simultaneous enhancement of AVT and PCE is achieved by meticulously designing host-guest active layers to fine-tune the molecular stacking. A systematic investigation of various host donor and guest material combinations reveals that the donor material (D18) with more electron-deficient hydrogen atoms tends to form C─H···O interactions with the guest material (BTO-BO) that features electron-rich oxygen atoms. Hydrogen bonding interactions between host donor D18 and guest BTO-BO facilitate the transition from mixed J-type and H-type molecular stacking modes of the donor to predominant J-type stacking during crystallization, significantly reducing visible absorption and enhancing hole transport. Additionally, BTO-BO can act as a nucleation agent for the host acceptor BTP-eC9 to increase the crystallinity and absorption coefficient of the active layer, thereby, enhancing near-infrared light absorption. The resultant toluene-processed ST-OSCs with optical modulation exhibit simultaneous improvement in PCE and AVT, delivering record LUEs of 6.02%. Notably, this host-guest active layer demonstrates exceptional compatibility with flexible devices and promising scalability for greenhouse photovoltaic applications.

Smart Polydimethylsiloxane Materials: Versatility for Electrical and Electronic Devices Applications

Mon, 17/03/2025 - 06:21

PDMS materials have found widespread applications in flexible wearable devices, medical technologies, coating protection, and thermal management. The development of smart PDMS materials featuring self-healing, self-cleaning, and self-reporting functionalities offers effective strategies to mitigate and prevent damage and degradation caused by exposure to harsh environments and mechanical/thermal stresses during practical applications.


Abstract

Bio-inspired autonomous smart polydimethylsiloxane (PDMS) and its composite materials hold immense promise for a wide range of applications in electrical and electronic devices. These materials mimic natural protective mechanisms with self-healing, self-reporting, and self-cleaning properties, enabling innovative and efficient device design. Smart PDMS materials autonomously activate repair mechanisms in response to mechanical or electrical damage, achieving rapid structural and functional recovery and preventing failure due to the accumulation of minor damage. These materials can intuitively report their status through striking color changes, fluorescence, or luminescence when exposed to external stimuli, providing efficient and practical visual feedback for device health monitoring and fault warning. They also have the capacity to effectively eliminate contaminants and ice deposits from their surfaces, thereby ensuring stable device operation. This review aims to introduce the current research progress in self-healing, self-cleaning, and self-reporting PDMS materials. The review systematically discusses the principles, methodological innovations, mechanistic analysis, and applications of these materials, highlighting their significant potential for applications in the field of electrical and electronic devices. Moreover, the review provides an in-depth analysis of the key challenges facing current research and offers insights into future research directions and strategies.

Core/Shell‐Structured Carbon Support Boosting Fuel Cell Durability

Mon, 17/03/2025 - 06:15

The study designs a bifunctional core/shell-structured carbon support with the core of highly graphitized carbon and the shell of heteroatom-doped amorphous carbon, precise control of Pt nanoparticles semi-embedded by the amorphous shell contributes to the realization of simultaneously exceeded durability targets of electrocatalysts and carbon support for PEMFCs.


Abstract

To enhance the lifetime of proton exchange membrane fuel cells, developing highly durable platinum-based cathode catalysts is essential. While two degradation pathways for the cathode catalyst—carbon corrosion and electrocatalyst (platinum nanoparticles) coarsening—have been identified, current approaches to enhance its durability are limited to addressing individual degradation pathways. Herein, the study develops a core/shell-structured carbon support that is designed to afford cathode catalysts capable of simultaneously inhibiting carbon corrosion and electrocatalyst coarsening. The core/shell structure is distinguished by its bifunctional nature: the core is made of highly graphitized carbon tailored to build a robust carbon skeleton, and the shell comprises heteroatom-doped amorphous carbon engineered to prevent electrocatalyst coarsening by chemical/physical anchoring of platinum nanoparticles. Thanks to this elaborate design, the catalyst surpasses the durability targets for carbon supports and electrocatalysts set by the U.S. Department of Energy, as supported by the achieved durability metrics after the square-wave/triangle-wave accelerated stress tests: electrochemical surface area loss at 13%/3%, mass activity loss at 27%/17%, and voltage loss of 29 mV (at 0.8 A cm− 2)/4 mV (at 1.5 A cm− 2).

Gradient‐Metasurface‐Contact Photodetector for Visible‐to‐Near‐Infrared Spin Light

Mon, 17/03/2025 - 06:14

This work presents the design and functionality of a gradient-metasurface-contact CPL photodetector that operates at zero bias, offering a high discrimination ratio (≈1.6 ✗ 104), broadband response (500–1100 nm), and immunity to non-CPL fields. By integrating InSe flakes with CPL-selective metasurface contacts, it achieves CPL-dependent vectorial photocurrents. Additionally, its application in multivalued logic and CPL-encrypted communication showcases its potential in advanced on-chip polarization detection systems.


Abstract

Spin light detection is a rapidly advancing field with significant impact on diverse applications in biology, medicine, and photonics. Developing integrated circularly polarized light (CPL) detectors is pivotal for next-generation compact polarimeters. However, previous compact CPL detectors, based on natural materials or artificial resonant nanostructures, exhibit intrinsically weak CPL polarization sensitivity, are susceptible to other polarization states, and suffer from limited bandwidths. A gradient-metasurface-contact CPL photodetector is demonstrated operating at zero-bias with a high discrimination ratio (≈1.6 ✗ 104), broadband response (500–1100 nm), and immunity to non-CPL field components. The photodetector integrates InSe flakes with CPL-selective metasurface contacts, forming an asymmetric junction interface driven by CPL-dependent unidirectional propagating surface plasmon waves, generating zero-bias vectorial photocurrents. Furthermore, it is implemented the developed CPL photodetector in a multivalued logic system and demonstrated the optical decoding of CPL-encrypted communication signals. This metasurface contact engineering represents a new paradigm in light property detection, paving the way for future integrated optoelectronic systems for on-chip polarization detection.

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4 January 2021

We are seeking to hire a research assistant to work on carbon nanotube based microdevices. More information is available here: www.jobs.cam.ac.uk/job/28202/

We are Hiring!

4 January 2021

We are seeking to hire a postdoc researcher to work on the structuring of Li-ion battery electrodes. More information is available here: www.jobs.cam.ac.uk/job/28197/