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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 27 min ago

Strategic Development of Memristors for Neuromorphic Systems: Low‐Power and Reconfigurable Operation

Tue, 25/03/2025 - 12:25

This review investigates technological trends in brain-inspired artificial reconfigurable memristors, as well as individual non-volatile and volatile devices, according to their operating principles and fabrication methods. It examines case studies of artificial neural network system implementations based on these devices, providing the latest comprehensive design guidelines from fundamentals to advanced systems.


Abstract

The ongoing global energy crisis has heightened the demand for low-power electronic devices, driving interest in neuromorphic computing inspired by the parallel processing of human brains and energy efficiency. Reconfigurable memristors, which integrate both volatile and non-volatile behaviors within a single unit, offer a powerful solution for in-memory computing, addressing the von Neumann bottleneck that limits conventional computing architectures. These versatile devices combine the high density, low power consumption, and adaptability of memristors, positioning them as superior alternatives to traditional complementary metal-oxide-semiconductor (CMOS) technology for emulating brain-like functions. Despite their potential, studies on reconfigurable memristors remain sparse and are often limited to specific materials such as Mott insulators without fully addressing their unique reconfigurability. This review specifically focuses on reconfigurable memristors, examining their dual-mode operation, diverse physical mechanisms, structural designs, material properties, switching behaviors, and neuromorphic applications. It highlights the recent advancements in low-power-consumption solutions within memristor-based neural networks and critically evaluates the challenges in deploying reconfigurable memristors as standalone devices or within artificial neural systems. The review provides in-depth technical insights and quantitative benchmarks to guide the future development and implementation of reconfigurable memristors in low-power neuromorphic computing.

Co‐Enriched High Entropy Oxides for Efficient Continuous Electrochemical Methane Conversion: Catalytic Performance and Sustainability Insights

Tue, 25/03/2025 - 12:19

A Co-rich high-entropy oxide (HEO) catalyst enables efficient electrochemical methane-to-ethanol conversion at room temperature. By leveraging elemental enrichment, the catalyst achieves high selectivity and stability, outperforming conventional systems. Process modeling further highlights its economic viability and significant potential for reducing carbon emissions.


Abstract

The electrochemical conversion of methane offers a sustainable alternative to traditional thermochemical syngas pathways; however, the rational design of catalysts that ensure high productivity remains a significant challenge. In this study, a high-entropy oxide (HEO) catalyst composed of Co, Cr, Fe, Mn, and Ni is explored, with a targeted element enriched, and identify that a Co-rich HEO demonstrates high efficiency in room-temperature electrochemical methane conversion. This analysis of the projected density of states (PDOS) reveals that Co sites in the HEO catalyst possess an optimally positioned p-band center for methane activation. The Co-rich HEO catalyst achieves an ethanol production rate of 12315 µmol/gcat/hr at 1.6 VRHE, with a Faradaic efficiency of 63.5%; a flow cell electrolyzer equipped with this catalyst achieves continuous methane-to-ethanol conversion at a rate of 26533 µmol/gcat/hr over 100 h. Process modeling evaluates the economic and environmental implications, demonstrating that a commercially viable process can be realized through economies of scale while significantly reducing CO₂ emissions.

Establishing Nanoscale Circuitry by Designing a Structure with Atomic Short‐range Order for High‐Rate Energy Storage

Tue, 25/03/2025 - 12:13

A microsized perovskite oxide Ce0.266W0.1Nb0.9O3 is engineered as an anode material for high-rate, long-life Li+ storage, demonstrating impressive performance by maintaining both high areal capacity and high rate capability, even at high mass loadings. This outstanding electrochemical behavior is primarily attributed to the nanoscale circuitry formed by an atomic-scale short-range order structure.


Abstract

High-rate materials necessitate the rapid transportation of both electrons and ions, a requirement that becomes especially challenging at practical mass loadings (>10 mg cm2). To address this challenge, a material is designed with an architecture having atomic-scale short-range order. This design establishes internal nanoscale circuitry at the particle level, which facilitates rapid electronic and ionic transport within micrometer-sized niobium tungsten oxides. The architecture features alternating cerium-depleted and cerium-enriched regions. The continuous cerium-enriched regions with enhanced conductivity provide multilane highways for electron mobility by functioning as electron-conducting wires that significantly boost the overall conductivity. The cerium-depleted regions effectively mitigate electrostatic repulsion and promote rapid ion transport through ion-conducting channels. These structural characteristics provide a continuous network that supports both electrical migration and chemical diffusion to amplify the areal capacity and rate capability even at high mass loadings. These findings not only expand the fundamental understanding of the design of optimal host lattices for advanced energy storage systems but also of the practical application of microsized high-rate electrode materials.

Efficient Photoelectrocatalytic Synthesis of Ammonia by Superionic Conductor with Mixed Ion/Electron Conduction

Tue, 25/03/2025 - 12:11

A van der Waals FePS2.66Li0.87 superionic conductor (SIC) with enhanced mixed electronic/ionic conductivity is applied for solar-driven nitrate conversion to ammonia. The migration of mobile lithium ions between layers significantly promotes the electronic conductivity of FePS2.66Li0.87 SIC, which achieves a remarkable ammonia synthesis yield (134.18 µmol cm−2 h−1) under low bias voltage.


Abstract

Photoelectrochemical (PEC) nitrate reduction shows substantial potential for solar-to-ammonia (NH3) conversion. However, low electron density and disordered electron conduction of conventional catalysts result in limited performance and low Faraday efficiency. Herein, a FePS2.66Li0.87 superionic conductor (SIC) is developed by introducing lithium ions into van der Waals immobile layered of FePS3 catalyst. This layered crystal framework facilitates high-concentration lithium ions confinement and long-range diffusion at room temperature, transitioning the conduction mechanism from electronic to mixed ionic/electronic. The typical nanofluidic ion transport leads to a high ionic conductivity of 16.4 mS cm−1 at room temperature and enhanced electronic conductivity of 5 × 10−6 S cm−1. Furthermore, mobile lithium ions within interlayers enhance the interaction between the low-lying 3dyz orbitals of Fe interacting with 2a2 empty antibonding orbitals of NO3 −. An excellent PEC ammonia production of 134.18 µmol cm−2 h−1 with 96.95% Faradaic efficiency is achieved, and the corresponding solar-to-NH3 efficiency of 57.13% offers a promising pathway toward sustainable ammonia production.

Critical Roles of Ultrafast Energy Funnelling and Ultrafast Singlet‐Triplet Annihilation in Quasi‐2D Perovskite Optical Gain Mechanisms

Tue, 25/03/2025 - 12:11

Ultrafast broadband photoluminescence spectroscopy provides insights into the lasing dynamics, energy transfer, and singlet-triplet annihilation in mixed-layer quasi-2D perovskites. Rapid energy funnelling to the sites of amplified spontaneous emission occurs within sub-picosecond timescales. However, the accumulation of triplet excitons effectively quenches incoming singlet excitons, creating a bottleneck in the energy cascade and hindering the development of population inversion.


Abstract

Quasi-2D (Q2D) perovskite possess considerable potential for light emission and amplification technologies. Recently, mixed films containing Q2D perovskite grains with varying layer thicknesses have shown great promise as carrier concentrators, effectively mitigating trap-mediated recombination. In this strategy, photo-excitations are rapidly funnelled down an energy gradient to the thickest grains, leading to amplified spontaneous emission (ASE). However, the quantum-confined Q2D slabs also stabilize the formation of unwanted triplet excitons, resulting in parasitic quenching of emissive singlet states. Here, a novel ultrafast photoluminescence spectroscopy is used to study photoexcitation dynamics in mixed-layer Q2D perovskites. By analysing spectra with high temporal and energy resolution, this is found that sub-picosecond energy transfer to ASE sites is accompanied by excitation losses due to triplet formation on grains with small and intermediate thicknesses. Further accumulation of triplets creates a bottleneck in the energy cascade, effectively quenching incoming singlet excitons. This ultrafast annihilation within 200 femtosecond outpaces energy transfer to ASE sites, preventing the build-up of population inversion. This study highlights the significance of investigating photoexcitation dynamics on ultrafast timescales, encompassing lasing dynamics, energy transfer, and singlet-triplet annihilation, to gain crucial insights into the photophysics of the optical gain process in Q2D perovskites.

Hierarchically Structured Porous Polyamide‐Imide Membrane for Switchable Emulsion Separation

Tue, 25/03/2025 - 12:10

A novel amphiphilic polymer Torlon-based membrane with switchable superwettability is developed using a simple one-step phase separation method. Its hierarchical porous structure and surface reorganization enable exceptional oil-water separation with ultrahigh permeance and efficiency. The membrane exhibits excellent antifouling, self-cleaning, and durability, offering a scalable solution for advanced oily wastewater treatment and beyond.


Abstract

The development of advanced membranes with switchable superwettability has attracted considerable attention for the efficient treatment of oily wastewater. However, challenges persist in designing and fabricating such membranes through straightforward methods. In this study, a novel strategy is presented to design switchable superwettable membranes based on micro/nano-structured porous surfaces and surface chemical composition reorganization. A commercial amphiphilic polymer, polyamide-imide (Torlon), is fabricated into a porous symmetric membrane with a hierarchical surface structure using a one-step non-solvent-induced phase separation method. By leveraging the surface reorganization capability of amphiphilic polymers and the hierarchically porous structure, the resulting membranes demonstrate exceptional superamphiphilicity in air, underwater superoleophobicity, and underoil superhydrophobicity. These properties enable ultrahigh permeance and separation efficiency for oil-in-water, water-in-oil, and crude oil/water emulsions through a gravity-driven process, eliminating the need for external energy. Furthermore, the membranes exhibit excellent antifouling and self-cleaning performance, maintaining stable operation over multiple cycles. This work provides an innovative and scalable approach to next-generation switchable superwettable membranes with broad potential applications in oily wastewater treatment and beyond.

Smart Dust for Chemical Mapping

Tue, 25/03/2025 - 12:10

This review article explores the advancement of smart dust networks for high-resolution spatial and temporal chemical mapping. Comprising miniature, wireless sensors, and communication devices, smart dust autonomously collects, processes, and transmits data via swarm-based communication. With applications in environmental monitoring, healthcare, agriculture, and industry, it emphasizes energy efficiency, sustainability, and large-scale deployment to revolutionize chemical analysis in complex environments.


Abstract

This review article explores the transformative potential of smart dust systems by examining how existing chemical sensing technologies can be adapted and advanced to realize their full capabilities. Smart dust, characterized by submillimeter-scale autonomous sensing platforms, offers unparalleled opportunities for real-time, spatiotemporal chemical mapping across diverse environments. This article introduces the technological advancements underpinning these systems, critically evaluates current limitations, and outlines new avenues for development. Key challenges, including multi-compound detection, system control, environmental impact, and cost, are discussed alongside potential solutions. By leveraging innovations in miniaturization, wireless communication, AI-driven data analysis, and sustainable materials, this review highlights the promise of smart dust to address critical challenges in environmental monitoring, healthcare, agriculture, and defense sectors. Through this lens, the article provides a strategic roadmap for advancing smart dust from concept to practical application, emphasizing its role in transforming the understanding and management of complex chemical systems.

A Multifunctional Binder for Current‐Collector‐Free Zn Powder Anodes

Tue, 25/03/2025 - 12:09

By introducing abundant polar groups as Zn2+ absorption sites and hydrogen bond arrays, a protein structure-derived binder for ZP anode and iodine cathode is proposed. This design can regulate the Zn2+ flux, benefit the formation of free-standing electrode, inhibit the side reactions, suppress the shuttle effect of polyiodides, and enable the large-scale potentials.


Abstract

Compared with commonly used Zn foil anodes, Zn powder (ZP) anodes offer superior versatility and processability. However, in aqueous electrolytes, dendrite growth and side reactions, such as corrosion and hydrogen evolution, become more severe in ZP anodes than those in Zn foil anodes because of the rough surfaces and high surface areas of ZP, leading to poor reversibility and limitations in high-loading mass cathodes. In this study, a diisocyanate-polytetrahydrofuran-dihydrazide polymer (DDP) binder is developed, inspired by protein structures. The strong Zn2+ adsorption capability of the binder effectively regulates Zn2+ flux, while its unique hydrogen-bond arrays facilitate the formation of a free-standing ZP anode and inhibit side reactions. The binder exhibits superior mechanical performance, providing ZP electrodes with excellent resistance to various mechanical stresses, including tensile, nanoindentation, scratch, and dynamic bending tests. ZP symmetric cells achieve stable cycling at capacities of 2 and 5 mAh cm−2. In addition, DDP functions as an iodine cathode, effectively mitigating the polyiodide shuttle effect. The fabricated ZP/DDP||I2/DDP full cells demonstrate an excellent rate capability and cycling stability, even under a high-loading conditions. This study presents a novel approach for preparing stable ZP anodes and iodine cathodes, offering a promising strategy for large-scale applications.

2D Rhodium‐Isocyanide Frameworks

Tue, 25/03/2025 - 12:09

Rhodium-carbon coordination-based 2D metal-organic frameworks are rationally synthesized and exhibit ultra-narrow bandgaps (0.10–0.28 eV) and intrinsic charge mobilities up to 560 ± 46 cm2 V−1 s−1 via time-resolved terahertz spectroscopy.


Abstract

2D metal-organic frameworks (2D MOFs) are emerging organic van der Waals materials with great potential in various applications owing to their structural diversity, and tunable optoelectronic properties. So far, most reported 2D MOFs rely on metal-heteroatom coordination (e.g., metal–nitrogen, metal–oxygen, and metal–sulfur); synthesis of metal-carbon coordination based 2D MOFs remains a formidable challenge. This study reports the rhodium–carbon (Rh–C) coordination-based 2D MOFs, using isocyanide as the ligand and Rh(I) as metal node. The synthesized MOFs show excellent crystallinity with quasi-square lattice networks. These MOFs show ultra-narrow bandgaps (0.1–0.28 eV) resulting from the interaction between Rh(I) and isocyano groups. Terahertz spectroscopy demonstrates exceptional short-range charge mobilities up to 560 ± 46 cm2 V−1 s−1 in the as-synthesized MOFs. Moreover, these MOFs are used as electrocatalysts for nitrogen reduction reaction and show an excellent NH3 yield rate of 56.0 ± 1.5 µg h−1 mgcat −1 and a record Faradaic efficiency of 87.1 ± 1.8%. In situ experiments reveal dual pathways involving Rh(I) during the catalytic process. This work represents a pioneering step toward 2D MOFs based on metal–carbon coordination and paves the way for novel reticular materials with ultra-high carrier mobility and for versatile optoelectronic devices.

Universally Applicable and Ultra‐Long Life Cyclic Power Generation Induced by Interfacial Ion‐Oscillation

Tue, 25/03/2025 - 05:49

An electric power generating cell is developed based on potential difference driven reversible ion migration, which generates ultra-long life electric output over 8-month with a high short-circuit of over 40 mA and output power density of up to 6 W m−2, surpassing the values reported for many other sorts of typical electricity generators.


Abstract

Sustainable energy supply without relying on external power sources is one of the bottlenecks in achieving self-supportive wearable electronics and Internet-of-things (IoT) systems. Here a new type of universally applicable and ultra-long life cyclic power generation is developed induced by interfacial redox reaction-mediated ion-oscillation, which can provide cycling electric energy in a self-charging manner without extra pre-charge. Based on asymmetric manganese dioxide and molybdenum disulfide electrode pairs, the proof-concept electric potential difference power generating cell (EPDC) offers ultra-long life electric output over 8-month testing period for tens of thousands of cycles. A layer-stacking EPDC unit supplies a high direct current of more than 40 mA and a power density of ≈6 W m−2. Such recyclable power-generating process mainly relies on reversible ion migration at an asymmetric interface in response to relative variation of electric potentials. The universal applicability of EPDC is validated by a combination of diverse electrode pairs. Large-scale manufacture of EPDCs is achievable by industry-compatible auto-blade coating technology with on-demand power output, providing a long-acting power supply platform for self-charging electronic systems.

Bottom‐Up Selective Growth of Ultralong Organic Phosphorescence Nanocrystals with Optimized Crystal Forms for In Vivo Optical Imaging

Tue, 25/03/2025 - 05:39

Ultralong organic phosphorescence (UOP) nanocrystals have attracted great attention in the field of in vivo optical imaging due to their ability to effectively minimize the interference of fluorescence background from biological tissues. In this work, a bottom-up strategy is proposed for preparing UOP nanocrystals with different crystal forms for in vivo biological imaging.


Abstract

Ultralong organic phosphorescence (UOP) materials are valuable for biological imaging to avoid interference from fluorescence background signals because of their delayed emission property. Obtaining nanocrystals with high phosphorescence quantum yield is a critical factor to achieve high-quality UOP imaging. Herein, a pair of host–guest UOP doped system with variable crystal forms for the host is constructed. By exploring the relationship between the crystal form of the host and the UOP of the doped system, the importance of host crystal form is revealed to achieve high quantum yield UOP in doped systems. Furthermore, to overcome the low crystallinity and numerous defects faced by traditional bottom-up strategies for nanocrystal preparation, a strategy is proposed for the selective preparation of nanocrystals with the target crystal form. Through controlling the evaporation rate of the solvent, the ordered growth of crystals can be effectively regulated to obtain nanocrystals with different crystal forms for bioimaging applications.

Spontaneous Twist of Ferroelectric Smectic Blocks in Polar Fluids

Mon, 24/03/2025 - 12:14

A chiral ground state of ferroelectric smectric is discovered which emerges in an achiral rod mesogen. This is not due to the torque-driven effect on the surface. The research confirms that the polar smectric blocks are twisted despite its high elasticity. Such a structure is predominantly generated in molecules with larger dipole moments, smaller dipole angles, and smaller aspect ratios.


Abstract

In soft matter, the polar orientational order of molecules can facilitate the coexistence of structural chirality and ferroelectricity. The ferroelectric nematic (NF) state, exhibited by achiral calamitic molecules with large dipole moments, serves as an ideal model for the emergence of spontaneous structural chirality. This chiral ground state arises from a left- or right-handed twist of polarization due to depolarization effects. In contrast, the ferroelectric smectic state, characterized by a polar lamellar structure with lower symmetry, experiences significantly higher energy associated with layer-twisting deformations and the formation of domain walls, thus avoiding a continuously twisted layered structure. In this study, two types of achiral molecules (BOE-NO2 and DIOLT) are reported that possess different molecular structures but exhibit a NF–ferroelectric smectic phase sequence. It is demonstrated that the chiral ground state of NF is inherited in the ferroelectric smectic phases of BOE-NO2 , which features larger dipole moments and a steric hindrance moiety, thereby triggering the formation of the twisted polar smectic blocks.

Molecular Stitching in Polysaccharide Precursor for Fabricating Hard Carbon with Ultra‐High Plateau Capacity of Sodium Storage

Mon, 24/03/2025 - 11:55

This work opens the avenue to molecular-level modulation in organic precursors for developing high-performance hard carbon in sodium-ion batteries. The highly cross-linked polymeric network in the precursor is constructed by unique molecular stitching strategy. The network evolves into highly twisted graphitic lattices with abundant closed ultramicro-pores (<0.3 nm), thereby enabling the storage of massive sodium clusters in hard carbon.


Abstract

High energy density of sodium-ion batteries (SIBs) requires high low-voltage capacity and initial Coulombic efficiency for hard carbon. However, simultaneously achieving both characteristics is a substantial challenge. Herein, a unique molecular stitching strategy is proposed to edit the polymeric structure of common starch for synthesizing cost-effective hard carbon (STHC-MS). A mild air-heating treatment toward starch is employed to trigger the esterification reaction between carboxyl and hydroxy groups, which can effectively connect the branched polysaccharide chains thereby constructing a highly cross-linked polymeric network. In contrast with the pristine branched-chain starch, the cross-linking structured precursor evolves into highly twisted graphitic lattices creating a large population of closed ultramicro-pores (<0.3 nm) enabling the storage of massive sodium clusters. Resultantly, STHC-MS delivers a reversible capacity of 348 mAh g−1 with a remarkable low-voltage (below 0.1 V) capacity of 294 mAh g−1, which becomes more attractive by combining the high initial Coulombic efficiency of 93.3%. Moreover, STHC-MS exhibits outstanding stability of 0.008% decay per cycle over 4800 cycles at 1 A g−1. STHC-MS||Na3V2(PO3)4 full cells achieve an energy density of 266 Wh kg−1, largely surpassing the commercial hard carbon-based counterpart. This work opens the avenue of molecular-level modulation in organic precursors for developing high-performance hard carbon in SIBs.

Resolving Dynamic Behavior of Electrocatalysts via Advances of Operando X‐Ray Absorption Spectroscopies: Potential Artifacts and Practical Guidelines

Mon, 24/03/2025 - 11:50

Resolving dynamically fine structure of electrocatalysts is realized by advanced X-ray spectroscopies. Based on a case study of operando X-ray absorption spectroscopy at various beamlines, potential artifacts generated by X-ray irradiation are validated and it is identified whether the dynamic behaviors are electrochemical reaction related. A practical protocol is proposed for conducting reliable X-ray spectroscopic measurements for accurate spectra interpretation.


Abstract

Although numerous techniques are developed to enable real-time understanding of dynamic interactions at the solid–liquid interface during electrochemical reactions, further progress in the development of these methods over the last several decades has faced challenges. With the rapid development of high-brilliance synchrotron sources, operando X-ray spectroscopies have become increasingly popular for revealing interfacial features and catalytic mechanisms in electrocatalysis. Nevertheless, the resulting spectra are highly sensitive to factors such as X-ray radiation, reaction environment, and acquisition procedures, all of which may potentially introduce artifacts that are often overlooked, leading to misinterpretations of electrocatalytic behaviors. In this perspective, several emerging hard X-ray spectroscopies used in electrocatalysis research are reviewed, highlighting their electronic transition processes, detection modes, and functional complementarity. Significantly, based on a case study of operando X-ray absorption spectroscopy at various beamlines, potential artifacts generated by X-ray irradiation are systematically investigated through photon-flux density-, dose-, and time-dependent studies of typical copper electrocatalysts. Accordingly, a practical protocol for conducting reliable X-ray spectroscopic measurements in operando electrocatalytic studies to minimize potential artifacts that can affect the resulting X-ray spectra, thereby ensuring accurate interpretation and a deeper understanding of interfacial interactions and electrocatalytic mechanisms, is established.

An n‐Doped Organic Cross‐Linked Electron Transport Layer with High Electrical Conductivity for High‐Efficiency Tandem Organic Photovoltaics

Mon, 24/03/2025 - 07:26

An n-doped ETL, that is c-NDI-Br:PEI with high electrical conductivity, strong work function modification ability and good solvent resistance, is developed via a simple in situ cross-linking reaction. The tandem OPVs, with the all-solution-processed organic/organic ICL (m-PEDOT:PSS/c-NDI-Br:PEI) achieve 20.06% efficiency under solar radiation, and 38.50% efficiency under 808 nm laser. This study provides a new method to design high-perfoimance ICLs.


Abstract

With merits of good solution processability, intrinsic flexibility, etc, organic/organic interconnecting layers (ICLs) are highly desirable for tandem organic photovoltaics (OPVs). Herein, an n-doped cross-linked organic electron transport layer (ETL), named c-NDI-Br:PEI is developed, via a simple in situ quaternization reaction between bromopentyl-substituted naphthalene diimide derivative (NDI-Br) and polyethylenimine (PEI). Due to strong self-doping, c-NDI-Br:PEI films exhibit a high electrical conductivity (0.06 S cm−1), which is important for efficient hole and electron reombination in ICL of tandem OPVs. In addition, the cross-linked ETLs show strong work function modulation ability, and good solvent-resistance. The above features enable c-NDI-Br:PEI to function as an efficient ETL not only for single-junction OPVs, but also for tandem devices without any metal layer in ICL. Under solar radiation, the single-junction device with c-NDI-Br:PEI as ETL achieves a power conversion efficiency (PCE) of 18.18%, surpassing the ZnO-based device (17.09%). The homo- and hetero-tandem devices with m-PEDOT:PSS:c-NDI-Br:PEI as ICL exhibit remarkable PCEs of 19.06% and 20.06%, respectively. Under 808 nm laser radiation with a photon flux of 57 mW cm−2, the homo-tandem device presents a superior PCE of 38.5%. This study provides a new ETL for constructing all-solution-processed organic/organic ICL, which can be integrated in flexible and wearable devices.

Regulating Interfacial H2O Activity and H2 Bubbles by Core/Shell Nanoarrays for 800 h Stable Alkaline Seawater Electrolysis

Mon, 24/03/2025 - 07:25

To concurrently improve activity and stability for seawater electrolysis under high current densities, the problems of firm adherence and coverage of H2 bubbles with core/shell nanoarrays, addressed which further regulates the interfacial H2O activity to reduce overpotentials, hence highlighting its potential as a sustainable and economically feasible application for large-scale hydrogen production.


Abstract

The catalytic activity and stability under high current densities for hydrogen evolution reactions (HER) are impeded by firm adherence and coverage of H2 bubbles to the catalytic sites. Herein, we systematically synthesize core/shell nanoarrays to engineer bubble transport channels, which further remarkably regulate interfacial H2O activity, and swift H2 bubble generation and release. The self-supported catalyst holds uniform ultra-low Ru active sites of 0.38 wt% and promotes the rapid formation of plentiful small H2 bubbles, which are rapidly released by the upright channels, mitigating the blockage of active sites and avoiding surface damage from bubble movements. As a result, these core/shell nanoarrays achieve ultralow overpotentials of 18 and 24 mV to reach 10 mA cm−2 for HER in 1 M KOH freshwater and seawater, respectively. Additionally, the assembled electrolyzer demonstrates stable durability over 800 hours with a high current density of 2 A cm−2 in 1 M KOH seawater. The techno-economic analysis (TEA) indicates that the unit cost of the hydrogen production system is nearly half of the DOE's (Department of Energy) 2026 target. Our work addresses the stability challenges of HER and highlights its potential as a sustainable and economically feasible solution for large-scale hydrogen production of seawater.

Non‐Invasive Diagnosis of Early Colorectal Cancerization via Amplified Sensing of MicroRNA‐21 in NIR‐II Window

Mon, 24/03/2025 - 07:13

An amplified sensing strategy is reported in the second near-infrared long-wavelength (NIR-II-L, 1500–1900 nm) window for non-invasivel in situ visualization of early cancerization biomarker miRNA-21, providing a promising alternative for early diagnosis of cancerization and a guidance for therapeutic management.


Abstract

Accurate, sensitive, and in situ visualization of aberrant expression level of low-abundant biomolecules is crucial for early colorectal cancer (CRC) detection ahead of tumor morphology change. However, the clinical used colonoscopy and biopsy methods are invasive and lack of sensitivity at early-stage of cancerization. Here, an amplified sensing strategy is developed in the second near-infrared long-wavelength subregion (NIR-II-L, 1500–1900 nm) by integrating DNAzyme-triggered signal amplification technology and lanthanide-dye hybrid system. In the early-stage of CRC, the overexpressed biomarker microRNA-21 initiates the NIR-II-L luminescence ratiometric signal amplification of the CRCsensor. The high sensitivity with a limit of detection (LOD) of 1.26 pm allows non-invasive visualization of orthotopic colorectal cancerization via rectal administration, which achieves early and accurate in situ diagnosis at 2 weeks ahead of the in vitro histological results. This innovative approach offers a promising tool for early diagnosis and long-term monitoring of carcinogenesis progression, with potential applications in other cancer-related biomarkers.

Van der Waals Ferroelectric CuCrP2S6‐Enabled Hysteresis‐Free Negative Capacitance Field‐Effect Transistors

Mon, 24/03/2025 - 06:53

This study explores 2D ferroelectric CuCrP2S6 for developing advanced NC-FET technology. Using MoS2 as the channel material, NC-FETs with optimized capacitance matching conditions achieve ultra-steep subthreshold swings (12 mV dec−1) and negligible hysteresis. A resistor-loaded inverter operating at 0.2 V with hysteresis-free characteristics highlights the potential of engineered 2D ferroelectrics for next-generation low-power electronics.


Abstract

The relentless pursuit of miniaturization and reduced power consumption in information technology demands innovative device architectures. Negative capacitance field-effect transistors (NC-FETs) offer a promising solution by harnessing the negative capacitance effect of ferroelectric materials to amplify gate voltage and achieve steep subthreshold swings (SS). In this work, 2D van der Waals (vdW) ferroelectric CuCrP2S6 (CCPS) is employed as the gate dielectric to realize hysteresis-free NC-FETs technology. Scanning microwave impedance microscopy (sMIM) is employed to investigate the dielectric property of CCPS, revealing a thickness-independent dielectric constant of ≈35. Subsequently, NC-FETs are fabricated with MoS2 channel, and the capacitance matching conditions are meticulously investigated. The optimized devices exhibit simultaneously ultra-steep SS (≈12 mV dec−1) and negligible hysteresis, with immunity to both voltage scan range and scan rate. Finally, a resistor-loaded inverter is demonstrated manifesting a low operation voltage down to 0.2 V and hysteresis-free transfer characteristics. This work paves the way for the development of high-performance, low-power electronics by exploiting 2D vdW ferroelectric materials.

Tracking Dynamics of Supported Indium Oxide Catalysts in CO2 Hydrogenation to Methanol by In Situ TEM

Mon, 24/03/2025 - 06:52

Combining in situ scanning transmission electron microscopy imaging with machine learning-based image analysis, this study directly visualizes and tracks dynamic restructuring in reducible oxide catalysts for green methanol synthesis. The findings reveal how supports modulate dynamic behaviors of reaction-induced InO x species, underpinning the superior methanol productivity of the In2O3/m-ZrO2 catalyst.


Abstract

Supported reducible oxides, such as indium oxide on monoclinic zirconia (In2O3/m-ZrO2), are promising catalysts for green methanol synthesis via CO2 hydrogenation. Growing evidence suggests that dynamic restructuring under reaction conditions plays a crucial but poorly understood role in catalytic performance. To address this, the direct visualization of the state-of-the-art In2O3/m-ZrO2 catalyst under CO2 hydrogenation conditions (T  =  553 K, P  =  1.9 bar, CO2:H2  =  1:4) is pioneered using in situ scanning transmission electron microscopy (STEM), comparing its behavior to In2O3 on supports with similar (tetragonal, t-ZrO2 or anatase TiO2) or lower (LSm-ZrO2) surface areas. Complementary in situ infrared spectroscopy and catalytic tests confirm methanol formation under equivalent conditions. A machine-learning-based difference imaging approach differentiates and ranks restructuring patterns, revealing that partially reduced InO x species on m-ZrO2 undergo cyclic aggregation-redispersion via atomic surface migration, maintaining high active phase dispersion. High-resolution ex situ STEM analysis further shows the epitaxial formation of In2O3 mono- and bilayers on (100) m-ZrO2 facets, highlighting strong oxide-support interactions. In contrast, sintering prevails on t-ZrO2, a-TiO2, and low-surface m-ZrO2, correlating with lower methanol productivity. This work underscores the pivotal role of oxide-support interfacial interactions in the reaction-induced restructuring of InO x species and establishes a framework for tracking nanoscale catalyst dynamics.

Chiral Pseudogap Metal Emerging from a Disordered Van der Waals Mott Insulator 1T‐TaS2 − xSex

Mon, 24/03/2025 - 06:51

An intriguing metal was discovered in a chiral charge density wave material, 1T-TaS2. The random substitution of S by Se induces a transition from an insulator to a metal with a strongly suppressed electron density at the Fermi energy. The pseudogap comes from electronic disorder on with substantial electron correlation and exhibits unprecedented chirality, which may induce exotic superconductivity.


Abstract

The emergence of a pseudogap is a hallmark of anomalous electronic states formed through substantial manybody interaction but the mechanism of the pseudogap formation and its role in related emerging quantum states such as unconventional superconductivity remain largely elusive. Here, the emergence of an unusual pseudogap in a representative van der Waals chiral charge density wave (CDW) materials with strong electron correlation, 1T-TaS2 is reported, through isoelectronic substitute of S. The evolution of electronic band dispersions of 1T-TaS2 − x Se x (0 ⩽ x ⩽ 2) is systematically investigated using angle-resolved photoemission spectroscopy (ARPES). The results show that the Se substitution induces a quantum transition from an insulating to a pseudogap metallic phase with the CDW order preserved. Moreover, the asymmetry of the pseudogap spectral function is found, which reflects the chiral nature of CDW structure. The present observation is contrasted with the previous suggestions of a Mott transition driven by band width control or charge transfer. Instead, the pseudogap phase is attributed to a disordered Mott insulator in line with the recent observation of substantial lateral electronic disorder. These findings provide a unique electronic system with chiral pseudogap, where the complex interplay between CDW, chirality, disorder, and electronic correlation may lead to unconventional emergent physics.

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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/