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NanoManufacturing

Michael De Volder, Engineering Department - IfM
 

Thu 13 Nov 15:00: Nanoscale thermodynamics

Nanoscale thermodynamics

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http://talks.cam.ac.uk/show/rss/5408 - Fri, 13/06/2025 - 14:22
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Design of a Tunable, High‐performance Mixed Matrix Membrane Platform for Gas Separations

A high-performance, flexible, tunable, and non-aging mixed matrix membrane platform is developed by incorporating CHA zeolites, featuring a 3D pore system with precise molecular-sieving and tunable chemical interactions, into a polyimide matrix at exceptionally high loadings. This tunable membrane platform significantly outperforms state-of-the-art membranes across a wide range of critical applications and can be beneficial for next-generation molecular separation membrane developments with vast industrial potential.


Abstract

Membrane technology offers substantial economic and environmental benefits for energy-intensive chemical separations. Chabazite-type zeolite, possessing a 3-D channel system with molecular-sieving windows, can be an ideal membrane material, but conditions to synthesize zeolite-only membranes limit optimization strategies. Guided by advanced quantum chemistry calculations on inner-pore molecular interactions, zeolite properties are tailored for different separations and optimized particles incorporated in polyimide at very high loadings. A membrane platform is thus created that largely outperforms state-of-the-art membranes for a broad variety of industry-relevant applications, that is, carbon capture, natural gas/biogas purification, hydrocarbon, helium and hydrogen recovery. Accurate size-sieving of gas molecules is realized together with rational determination of optimal gas-zeolite interactions. Crucial for industrial applications, these well-tuned membranes displayed excellent non-aging properties, high flexibility and higher mixed-gas selectivities than ideal-gas selectivities. Moreover, they performed even better at low CO2-partial pressure in CO2-removal and can be made humidity-insensitive.

A Hydrophobic and High Surface Charge Phosphate Interphase for High Areal Capacity Zinc Metal Batteries

A robust hydrophobic and high-surface-charge phosphate interphase dramatically fosters uniform Zn deposition at the (100) plane, realizing an unprecedented Sand's capacity of over 64 mAh cm−2. The synergy of a narrower Zn2⁺-rich electric double layer and suppressed side reactions delivers stable Zn metal batteries with high areal capacity, long lifespan, and practical viability.


Abstract

Commercial zinc metal batteries require an areal capacity above 4 mAh cm−2 at high rates. However, such performance is rarely reported due to slow mass transport between the diffuse layer and the outer Helmholtz layer at the interface. Herein, it is reported an unprecedented Sand's capacity exceeding 64 mAh cm−2 at 20 mA cm−2, enabled by a hydrophobic and high surface charge iron/zinc phosphate (FZP) nanofilm serving as an artificial solid electrolyte interphase for zinc anode. It is identified the key role of high surface charge with strong Zn2⁺ affinity, which mitigates depletion zones by forming a narrower and Zn2+-rich electric double layer, thereby achieving high areal capacities and promoting preferential exposure of the Zn (100) plane. Consequently, FZP/Zn exhibits stable cycling for 400 h under 60% depth-of-discharge (2.14 mAh cm−2). Full cells with a low N/P ratio deliver an energy density of 176.5 Wh kg−1 electrodes at 6 mAh cm−2. The practical Zn-I2 pouch cells are further demonstrated with ≈97 Ah of cumulative capacity and a high areal capacity of 5.12 mAh cm−2. These findings establish FZP nanofilms as a viable strategy for realizing commercial high-areal-capacity aqueous zinc-ion batteries.

Ternary Inert Element Co‐Doping: a New Approach to Stable 4.7 V LiCoO2

Al–Mg–Ni inert co-doping synergistically enhances structural stability of LiCoO2 at highly delithiated state, with Mg/Ni stabilizing Li layers and suppressing oxygen loss, while Al reinforcing Co–O octahedra, giving a capacity retention of 58.6% after 600 cycles at 4.7 V.


Abstract

LiCoO2 (LCO) has long dominated the cathode materials in portable electronic batteries due to its high volumetric energy density. However, the pursuit of higher voltages to achieve larger capacities remains a challenge due to severer structural degradation. Herein, a ternary inert element co-doping strategy that can greatly improve the structure stability of LCOs at elevated voltages is reported. Mg and Ni doping at Li site support the layered structure in the highly delithiated state, while Ni also facilitates the separation of O 2p and Co 3d orbits, thereby suppressing oxygen loss. Meanwhile, Al doping at Co site suppresses the distortion of Co–O octahedra and stabilizes the Co layers. The synergistic effects of Al, Mg and Ni co-doping inhibit the irreversible H3–H1-3 phase transitions and mitigate internal stress accumulation. The Al–Mg–Ni co-doped LCO exhibits a capacity of 221 mAh g−1 with a capacity retention of 65.5% after 1500 cycles at 4.6 V. At a higher voltage of 4.7 V, it delivers a capacity of 225.8 mAh g−1 with a capacity retention of 58.6% after 600 cycles. This multiple inert elements co-doping strategy gives an effective method for stabilizing the high-voltage LCO and other related layered oxide materials.

Unlocking NIR‐II Photoluminescence in 2D Copper Tetrasilicate Nanosheets through Flame Spray Synthesis

A flame-spray-pyrolysis method is presented to synthesize ultra-bright CTS nanosheets with tunable NIR-II emission. Achieving quantum yields up to 34%, these materials support high-speed imaging and enable super-resolution in vivo applications such as transcranial microcirculation mapping and macrophage tracking.


Abstract

Expanding fluorescence bioimaging into the second near-infrared spectrum (NIR-II, 1000–1700 nm) unlocks advanced possibilities for diagnostics and therapeutics, offering superior tissue penetration and resolution. 2D copper tetrasilicate (CTS) pigments (MCuSi4O10, M = Ca, Sr, Ba) are known for their brightness and stability, yet synthetic challenges have curbed their integration into bioimaging. Here, flame-spray-pyrolysis (FSP) is introduced as a versatile and scalable synthesis approach to produce ultra-bright, metastable CTS nanosheets (NS) by annealing multi-element metal oxide nanoparticles into 2D crystals through calcination or laser irradiation. Group-II ion incorporation shifts emission into the NIR-II range, with Ba0.33Sr0.33Ca0.33CuSi4O10 peaking at 1007 nm, while minor Mg-doping induces a hypsochromic shift and extends fluorescence lifetimes. The engineered CTS achieves quantum yields of up to 34%, supporting NS high-frame-rate imaging (> 200 fps). These unique properties enable CTS-NS to serve as powerful contrast agents for super-resolution NIR bioimaging, demonstrated in vivo through transcranial microcirculation mapping and macrophage tracking in mice using diffuse optical localization imaging (DOLI). This pioneering synthesis strategy unlocks wavelength-tunable NS for advanced NIR-II bioimaging applications.

Porogen‐Integrated Rapid Oxidation Enables Structured Mesoporous Metal Oxide Films

Porogen-integrated rapid oxidation (PiRO) is a method for high throughput manufacturing of mesoporous metal oxide thin films. PiRO generates up to 500 nm thick layers with through-plane 5–10 nm spheroidal close-packed pores at 230 °C in 30 min or less. The reduced temperatures enable deposition on both rigid and flexible polymeric substrates using roll-to-roll compatible techniques.


Abstract

Structured metal oxide films have promise in optoelectronics, sensing, energy storage, and catalysis but their uptake is predominately limited due to their long and high-temperature syntheses. Here, a self-assembling polymer is used which can act as a chelating fuel source in a solution combustion reaction to generate highly structured mesoporous aluminum oxide films at <250 °C in a matter of minutes through a process termed porogen-integrated rapid oxidation (PiRO). The resulting films with thicknesses up to 500 nm show an open-cell, face-centered cubic structure of spheroidal pores. Further, an additional ligand can be included to control the self-assembly step to yield both through-film ordering or tunable disordering for increased pore volume as confirmed by both grazing incidence small angle X-ray scattering and ellipsometry. Finally, roll-to-roll manufacturing with PiRO is demonstrated on flexible polymeric substrates. The method offers a tunable, scalable, low-temperature, and lower-cost method to generate large-area structured mesoporous metal oxide films.

Scalable Jet Swimmer Driven by Pulsatile Artificial Muscles and Soft Chamber Buckling

Inspired by nautiluses, a scalable robotic jet swimmer is developed, featuring a soft chamber that buckles instantly to amplify jetting speed. It demonstrates the successful integration of smart materials and smart structures in a robotic system, offering a promising pathway for developing efficient, adaptable, and intelligent underwater soft robots.


Abstract

Cephalopods, such as squid and nautilus, achieve fast swimming by jetting water swiftly from their chambers, offering benefits in swimming speed, energy efficiency, and silent operation. Inspired by these animals, a scalable soft robotic jet swimmer that utilizes soft chamber buckling to enable rapid water jetting is proposed. The design incorporates three main components: the knotted artificial muscle (KAM), an origami-inspired soft chamber, and a custom control module. The KAM generates significant force and stroke with minimal self-weight, but its actuation speed is insufficient for propelling water. To address this limit, an origami-inspired soft chamber that buckles instantly when the KAM's pulling force reaches a critical threshold is designed, thereby amplifying actuation speed and enabling rapid water jetting. The control module periodically activates the KAM to tighten and release, facilitating effective pulsatile propulsion. Similar to Cephalopods, this design is scalable and robust. Effective swimming of two robots is demonstrated with drastically different sizes, achieving a top speed of 0.62 body length per second. We also show that the propulsion is minimally compromised even when the KAM is significantly damaged. To further enable guided locomotion, a shape memory alloy rudder is incorporated for steering via infrared stimulation. This work demonstrates successful pulsatile jet swimming through the integration of smart materials and smart structures, laying the groundwork for future innovations in underwater soft robotics.

On‐the‐Fly Synthesis of Freestanding Spin‐Crossover Architectures With Tunable Magnetic Properties

3D flow-focusing devices are an ideal platform for the processing and integration of functional materials within polymeric matrices. In this article, A. Tuan Ngo, D. Aguilà, T. Sotto Mayor, M. Palacios-Corella, J. Puigmartí-Luis show the on-the-fly processing of a prototypical SCO material—known for its challenging processability—thereby opening new avenues for its implementation in real-world applications.


Abstract

Spin-crossover (SCO) molecular-based switches have shown promise across a range of applications since their discovery, including sensing, information storage, actuators, and displays. Yet limited processability remains a barrier to their real-world implementation, as traditional methods for integrating SCO materials into polymer matrices are often complex, expensive, and prone to producing uneven material distributions. Herein, we demonstrate how 3D flow-focusing chemistry enables unprecedented control for the direct fabrication of SCO composite materials, addressing key challenges in processability, scalability, and cost. By using a 3D coaxial flow-focusing microfluidic device, we simultaneously synthesize [Fe(Htrz)2(trz)](BF4) and achieve its homogeneous incorporation into alginate fibers in a continuous manner. The device’s versatility allows for precise manipulation of the reaction-diffusion (RD) zone, resulting in SCO composite fibers with tunable physicochemical and magnetic properties. Additionally, we demonstrate the ability to isolate these fibers as freestanding architectures and highlight the potential for printing them with defined shapes. Finally, we show that the 3D control of the RD zone granted by continuous flow microfluidic devices offers precise spatiotemporal control over the distribution of SCO complexes within the fibers, effectively encoding SCO materials into them. SCO-encoded fibers can seamlessly combine adaptability and functionality, offering innovative solutions for application-specific customization.

Homogeneous “Hard‐Soft” Biphasic Bone Adhesives Promote Comminuted Fracture Healing through Interfacial Adaptation and Mechanical Property Maintenance

For the instant and sustainable fixation of bone fragments in treating highly comminuted fractures, phase engineering is employed to construct a homogeneous hard-soft biphasic bone adhesive (PTN). The conversion of tetracalcium phosphate in the hard phase and the deposition of hydroxyapatite in the soft phase endow its anti-swelling and mechanical resistance while adapting to the interfacial changes for sustainable adhesion.


Abstract

Bone adhesives provide remarkable clinical solutions in treating highly comminuted fractures that are difficult to perform surgery with metal fixation. However, no commercial bone adhesives exhibit high adhesion, strength, and osteogenic activity for instant and sustainable fixation in dynamic, wet humoral environments at weight-bearing sites. Here, phase engineering is employed to construct a homogeneous hard-soft biphasic bone adhesive (HB-PTN) with a sea urchin-inspired structure of phosphorylated polyglutamic acid (P-PGA) encapsulating tetracalcium phosphate (TTCP) (hard phase) and a viscoelastic hydrogel composed of amino-functionalized PEGylated poly (glycerol sebacate) (PEGS-NH2) and P-PGA (soft phases) for immediate, stable fixation. The adhesion and strength of the HB-PTN hydrogel can be tuned by modulating the soft phase/hard phase ratio. The PTN-2 hydrogel exhibited an adhesive strength of ≈280 kPa, a compressive modulus of ≈1.02 MPa, and high fatigue resistance (92%). Moreover, the PTN-2 hydrogel showed limited swelling (130%) and maintained mechanical properties (102%) after immersion in simulated human body fluid. Furthermore, this strategy avoids the agglomeration of inorganic particles and the formation of cracks due to stress concentration observed with traditional mixing methods. In vivo, the PTN adhesives reveal durable and stable adhesion and accelerate fracture healing, demonstrating great clinical potential in comminuted fracture repair.

Electric Field Driven Soft Morphing Matter

This study presents soft morphing matter robots that exhibit extremely high morphological adaptability and complex multimodal electric field response. They can undergo large, controlled body deformation and show complex locomotion on different terrains under the manipulation of external electric fields, making a significant step beyond current electroactive and soft robots.


Abstract

The manipulation of soft morphing robots using external electric fields and wireless control is challenging. Electric field-driven soft morphing matter, termed electro-morphing gel (e-MG), that exhibits complex multimodal large-scale deformation (showing up to 286% strain, and strain rates up to 500% s−1) and locomotion under external electric fields applied using compact and lightweight electrodes is presented. The distinctive capabilities of e-MG derive from the combination of an elastomeric matrix and nanoparticulate paracrystalline carbon. The material properties, electroactive principle, and control strategies are explored and demonstrate fundamental morphing matter behaviors including rotating, translating, stretching, spreading, bending, and twisting. A range of potential bio-inspired applications, including slim mold-like spreading, snail-like jumping over a gap, object transport, wall climbing, and a frog tongue-inspired gripper is shown. The e-MG provides morphing capabilities beyond the current limitations in wireless control for a wide range of applications in soft and bio-inspired robotics, dexterous manipulation, and space exploration.

Materials Evolution by Programmed Twisting: a DNA‐Inspired Ultrastrong Supercoiled Conformational Fiber for Energy‐Storage and Buffering

Inspired by the supercoiled conformational structures and behaviors of the DNA chain, a material evolution strategy via supercoiled conformational fibers (SCFs) is proposed to achieve a number of extra-ordinary properties/functions, including pseudo-entropic elasticity, high-performance torsional energy-storage, stimulus-triggered energy release, impact buffering, and self-reinforcement.


Abstract

The conformational folding/unfolding behaviors of DNA supercoils serve as a fundamental mechanism governing ultradense bio-information storage and precise genetic transcription. Mimicking those nanoscale dynamic conformational behaviors for macroscopic materials to achieve unusual functionalities will be of great interest but remains unexplored. Herein, a DNA-inspired materials evolution paradigm is presented to create multifunctional supercoiled conformational fibers (SCFs) by programmed twisting controlled self-buckling. Through the programmed twist-stress modulation, a low-density polyethylene strip is transformed into high-performance DNA-like SCF through a unique multiscale microstructure evolution process. This DNA-like SCF exhibits five hallmark characteristics unattainable before, including ultra-large elastic deformability (900 ± 50%), metal-level mechanical strength (330 ± 30 MPa), unprecedented torsional energy-storage density (16.1 ± 0.6 kJ kg−1), torsional energy release upon appropriate stimulations, and impact buffering through conformation-mediated energy-dissipation. Characterization reveals that these unexpected energy-related properties mainly are contributed by the multiscale twisting-reinforced microstructures and conformation mechanics. Potential applications of the SCFs are demonstrated finally by harvest-and-storage of wind energy and soft-landing. The DNA-like SCFs indicate a general platform for materials evolution with extraordinary mechanics and functions.

Integrated Polarization, Distance, and Rotation for Multi‐DoF Diffractive Processor and Information Encryption

A multi-DoF processor is designed to perform versatile inference tasks, including single-/dual-digit and single-/dual-fashion product classification, logic operations, and image transformation. Moreover, a high-security information transmission framework is experimentally demonstrated that transforms a large volume of input data—encoded across multiple channels—into Morse code, with the true information subsequently synthesized through further decoding.


Abstract

All-optical diffractive deep neural networks (D2NNs) offer significant advantages in processing speed and power consumption, thereby accelerating the development of optical computing and artificial intelligence (AI). Integrating multiple degrees of freedom (multi-DoF) into D2NNs is a pivotal role in improving information processing and task-loading capacity, an enormous challenge in current all-optical diffractive computing/processors. Here, a multi-DoF diffractive processor is proposed and experimentally demonstrated that leverages a metasurfaces-based approach to integrate polarization, distance, and rotation channels for versatile inference tasks and information encryption. The approach is validated using three-layer metasurfaces that enable high task-capacity tasks, including single-/dual-digit and single-/dual-fashion-product classification, logic operators, and image transformation. Moreover, by mapping large volumes of input data into multi-DoF channels and encoding the information in Morse code with our D2NNs framework, a high-security information transmission system is experimentally implemented. The integration of polarization, distance, and rotation channels into an all-optical diffractive processor with multifunctional capabilities paves the way for multifunctional integrated devices and communication.

Fluorine–Mediated Interfacial Microenvironment for Boosting pH–Universal CO2 Reduction

Ni species (single atoms and atomic clusters) are successfully anchored onto fluorocarbon substrates (FC), forming a highly efficient and stable CO2RR electrocatalyst. The optimized Ni/FC exhibits excellent FECO in acidic, neutral, and alkaline electrolytes, respectively. More importantly, Ni/FC can maintain excellent FECO while operating at industrial currents density for 3000 h. Mechanistic studies reveal that the high–electronegativity of F will cause the formation of a positive Cδ+ center, which inhibits the adsorption of hydrogen and elevates the dissociation energy barrier of interfacial water, thereby suppressing the competitive HER process.


Abstract

Achieving highly efficient and stable conversion of carbon dioxide reduction reaction (CO2RR) into value-added chemicals at industrial current density is crucial but challenging due to its complex gas–solid–liquid interface. Here the local microenvironment of three–phase interface is successfully regulated to boost the CO2RR performance of Ni species in the universal pH range by introducing the highly electronegative F. The optimized Ni/FC achieves high–performance in converting CO2 to CO with Faraday efficiencies (FEs) over 90% in pH–universal conditions, while the main product of Ni/C is H2, especially under acidic conditions. Significantly, it can steadily operate at a high current density of 200 mA cm−2 for over 3000 h in a broad pH range, outperforming most recently reported CO2RR electrocatalysts. Detail in situ experiments and density functional theory calculations reveal that the presence of highly electronegative F will cause the formation of a positive Cδ+ center, which inhibits the adsorption of hydrogen and increases the dissociation energy barrier of interfacial water, thereby suppressing the competitive hydrogen evolution reaction (HER). This work highlights the importance of regulating the local microenvironment of interfacial water, providing a new perspective in the field of electrocatalysis for suppressing competitive HER.

Unveiling the Multifunctional Potential of MXenes in Rechargeable Batteries beyond Electrode Active Materials

This review provides comprehensive perspectives on MXene's application as passive components in rechargeable battery systems, as current collectors, electrolytes additives, separators, binders, and hosts for active materials. It aims to forecast the multifunctional potential of MXenes in batteries, gain valuable insights into their broader applicability, and contribute to the innovation of energy storage systems.


Abstract

MXene materials have emerged as prominent candidates for revolutionizing energy storage technologies due to their unique properties and versatile applications. This review highlights the multifaceted roles of MXenes (beyond electrode active materials) in improving various components of rechargeable batteries. MXenes exhibit exceptional electrical conductivity, tunable surface functionalities, and a 2D structure, rendering them suitable for enhancing electrode or electrolyte materials, current collectors, binders, and separators. As electrode hosts, MXenes accommodate active materials such as sulfur, silicon, selenium, and novel compounds, addressing challenges related to volume expansion, electronic conductivity, and chemical interactions. Furthermore, MXene-based conductive agents and additives ameliorate the stability and performance of solid-state devices, overcoming issues associated with flammable liquid electrolytes. MXene materials excel as current collectors by improving contact between active materials, mitigating dendrite formation, extending battery lifespan, and improving safety. Additionally, MXene-modified separators and interlayers effectively hinder the shuttle effect and dendrite growth in Li-S and other battery systems with stability and longevity. With their distinct attributes to offer transformative opportunities for addressing limitations in next-generation rechargeable batteries, MXenes hold the promise of shaping a more efficient, secure, and sustainable energy storage landscape.

Emerging Surface Engineering Methods for Lithium Metal Anodes: Critical Review Beyond Conventional SEI and Surface Coatings

This review explores innovative strategies to overcome the limitations of traditional lithium metal anodes by focusing on tunable SEI designs, chemical synergies, and advanced fabrication techniques. It highlights recent breakthroughs that improve battery performance and safety while proposing integrative approaches to address remaining challenges for practical applications.


Abstract

For rechargeable lithium batteries with high energy density, lithium metal anode is an ideal candidate due to its high theoretical capacity (3860 mAh g−1) and low electrode potential (−3.04 V versus standard hydrogen electrode). Despite its promising characteristics, it faces formidable obstacles such as dendritic growth and poor formation of solid electrolyte interphase (SEI) layers. To overcome such obstacles, multifaceted unconventional surface engineering approaches are hypothesized, tested, and examined. In this review, in addition to the conventional SEI and surface coatings, the principles and recent progress of the unconventional surface engineering methods are summarized and assessed, based on the interfacial thermodynamics and factors governing the interface between the electrode and the electrolyte. It connects and provides the newest insight on material science, design methodologies, and fabrication techniques, which require significant attention. This review reveals the significance of unconventional methods in enhancing both electrochemical performance and safety of the next-generation lithium metal batteries, providing a comprehensive understanding of the current research landscape and roadmaps for future technological breakthroughs.

Dynamic Gradient Oxygen Layer Enables Stable Sn Anode for Lithium Storage

During lithiation/delithiation, SnOx helped to form a stable solid electrolyte interface film. In addition, the disordered SnOx lamellar structures can release stress to prevent particle pulverization during its transformation into a denser amorphous layer. Its mechanism of lithium storage in the intercalation layer and dynamic oxygen concentration gradient can enable the rapid exchange of lithium ions.


Abstract

Sn-based anodes are of significant interest due to their high capacity and resource abundance for lithium-ion batteries. However, incomplete lithiation and severe volume expansion result in their low capacity and electrode pulverization. Here, a rationally designed coating layer, composed of disordered SnOx (x = 1, 2) lamellar structures, on the Sn particles surface (Sn@SnOx) is proposed. This coating effectively mitigates volume expansion and minimizes lithium consumption owing to the intercalation behaviors of SnOx. During lithiation and delithiation, a dense, amorphous, mechanical coating with a dynamic gradient of oxygen forms in situ, providing excellent protection against continuous pulverization of the Sn particles. The intercalation-type dynamic gradient oxygen with high ionic conductivity enables rapid exchange of lithium ions, thus promoting the deep lithiation of Sn to form Li4.4Sn. Such gradient oxygen protection mechanism of the oxide layer in Sn@SnOx brings a high reversible capacity after 900 cycles with a capacity retention of 84%. This work offers a new strategy to design a protective coating layer on alloy-based anodes for high-performance lithium storage.

Visualizing dynamic competitive reconstruction of trimetallic hybrid catalysts for stable hybrid water electrolysis at large current density

http://feeds.rsc.org/rss/ee - Fri, 13/06/2025 - 06:43
Energy Environ. Sci., 2025, Accepted Manuscript
DOI: 10.1039/D5EE00172B, PaperYong Zhang, Liling Liao, Haiqing Zhou, Ying Qi, Jingying Sun, Yan Zhang, Qian Zhou, yu wang, Dongsheng Tang, Fang Yu
Glycerol electrooxidation is an intriguing surrogate reaction for sluggish oxygen evolution in water electrolysis and can simultaneously produce value-added chemicals at the anode, however, the majority of non-precious catalysts suffer...
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Ultra‐Sensitive Optoelectronics Enabled by Atomically Tailored Interfaces Engineering for Advanced Perceptual Imaging

A broadband, self-powered photodetector is developed by integrating Cl-substituted 2D perovskites with MoS2/WSe2 heterostructures via interface engineering. The device enables weak-light detection down to 0.54 µW cm−2, offering enhanced carrier transport and photogating effects. This strategy highlights a general approach to boosting the performance of 2D material-based optoelectronic devices.


Abstract

Ultra-weak light detection represents a critical enabling technology for next-generation imaging, remote monitoring, and autonomous systems, where efficient charge transfer is essential to achieve ultralow detection thresholds. Herein, an interfacial lattice-distortion engineering strategy is proposed by selectively substituting phenylethyl ammonium (PEA) cations with 4-chlorophenylethylammonium (Cl-PEA) at perovskite heterointerfaces. This substitution induces beneficial octahedral distortions, boosting hole transport efficiency in few-layer 2D perovskites by 26%. When integrated with MoS2/WSe2 heterostructures, the optimized van der Waals contact and enhanced energy-level alignment yield a high-performance photodetection, including a responsivity of 2.7 × 104 A/W, a detectivity up to 5.26 × 1014 Jones, and an exceptionally low noise equivalent power of 0.42 fW Hz−1/2. Notably, the device operates self-powered at incident power densities as low as 0.54 µW cm−2, enabling real-time, on-chip image processing even under dim-light conditions. This functionality is further utilized for noise reduction in traffic-light images prior to object detection with YOLOv11 network, establishing a direct bridge between device-level photodetection and machine-learning-driven recognition. This interfacial lattice distortion engineering paradigm in van der Waals-contacted 2D devices opens new avenues for designing ultrasensitive, low-noise, and functionally integrated optoelectronic devices.

Direct‐Ink‐Writing Printed Aerogels with Dynamically Reversible Thermal Management and Tunable Electromagnetic Interference Shielding

Honeycomb-structured (Ti3C2T x /Fe3O4/CCMC)–(AgNW/CCMC) aerogels with tunable EMI shielding performance up to 80 dB are fabricated via DIW 3D printing, achieving compression-driven shielding adjustability, infrared stealth, and reversible thermal insulation–conduction conversion for dynamic thermal management in harsh environments.


Abstract

Achieving both structural precision and tunable performance in electromagnetic interference (EMI) shielding materials remains a critical challenge, particularly for adaptive applications. Herein, a strategy is proposed that integrates calcium chloride (CaCl₂)-induced elastic activation of carboxymethyl cellulose (CMC) with direct ink writing (DIW) 3D printing to address the limitations in structural design and performance adjustability of EMI shielding materials. By leveraging CaCl₂-crosslinked CMC (CCMC) as a flexible matrix, honeycomb-structured (Ti₃C₂Tx/Fe₃O₄/CCMC)–(Ag nanowire (AgNW)/CCMC) aerogels is fabricated with precise architecture and tunable shielding effectiveness under mechanical compression. With a 35% printing fill density, 40 wt% Ti₃C₂Tx, and 60% compressive strain, the aerogel achieves an optimal shielding effectiveness of 80 dB. Additionally, the aerogel exhibits reversible infrared stealth and dynamically switchable thermal properties (from 0.08 to 0.67 W·m⁻¹·K⁻¹) in response to environmental humidity variations. This work demonstrates a versatile approach for structurally adaptive EMI shielding materials with self-regulating thermal behavior, offering promising applications in harsh environment protection, intelligent thermal camouflage, and adaptive shielding for next-generation aerospace and communication technologies.

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