Materials Horizons最新文献

{"title":"C-C bonded azole architectures: molecular design and structure-property relationships in energetic materials.","authors":"Abhishek Kumar Yadav, ManojKumar Jujam, Sagar Nehe, Sonali Kukreja, Srinivas Dharavath, Jean'ne M Shreeve","doi":"10.1039/d6mh01967f","DOIUrl":"https://doi.org/10.1039/d6mh01967f","url":null,"abstract":"<p><p>Carbon-carbon (C-C) bonded azoles represent an important and rapidly expanding class of nitrogen-rich heterocyclic compounds with significant relevance to energetic and functional materials. Azole rings, comprising five-membered heterocycles containing nitrogen, oxygen, or sulfur atoms, offer versatile molecular scaffolds for the development of high-energy-density materials (HEDMs). Direct C-C linkage between azole units provides a robust structural framework while enabling modulation of molecular geometry, electronic characteristics, and physicochemical properties. These structural features can strongly influence key material parameters, including density, heat of formation, thermal stability, and sensitivity. In recent years, a diverse range of symmetrical and unsymmetrical C-C-bonded azole architectures has been reported, incorporating heterocycles such as pyrazoles, triazoles, tetrazoles, oxadiazoles, furoxans, and thiadiazoles. Symmetrical systems can facilitate structural regularity and efficient crystal packing, whereas unsymmetrical azole hybrids provide greater molecular diversity and opportunities for tuning properties through the combination of different heterocyclic units. Despite the rapid expansion of this research area, a comprehensive analysis of the structural features and property relationships governing C-C bonded azole systems remains lacking. This review presents a systematic and critical assessment of the synthesis, structural diversity, and physicochemical and energetic properties of C-C bonded azole architectures, organized according to symmetrical and unsymmetrical systems. Particular emphasis is placed on correlating molecular connectivity, substitution patterns, heterocycle combinations, and crystal structures with density, energetic performance, thermal stability, and sensitivity. By identifying emerging structure-property relationships and the factors governing the balance between energy and stability, this review provides molecular design principles for the development of high-performance and safer energetic materials.</p>","PeriodicalId":87,"journal":{"name":"Materials Horizons","volume":" ","pages":""},"PeriodicalIF":11.4,"publicationDate":"2026-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149356965","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Advances in direct ink writing of silicone rubbers: toward high-fidelity architectures and multifunctional integration.","authors":"Xiang Li, Qiong Wu, Shanhui Diao, Guochen Xu, Li Shi, Xianwei Meng","doi":"10.1039/d6mh01548d","DOIUrl":"https://doi.org/10.1039/d6mh01548d","url":null,"abstract":"<p><p>Silicone rubber is widely used in wearable electronics and soft robotics because of its flexibility, biocompatibility, and thermal and chemical stability. However, traditional fabrication methods offer limited flexibility in producing customized geometries and complex internal structures. Direct ink writing (DIW) provides a versatile alternative by accommodating diverse silicone formulations and enabling programmable three-dimensional fabrication. Recent studies on silicone-rubber DIW have addressed shape-fidelity enhancement, multimaterial fabrication, and functional device development, but these areas have not been systematically classified and compared from the perspective of silicone printing. This review groups heating, UV curing, and support-bath printing as high shape-fidelity techniques based on their common role in stabilizing deposited silicone before complete curing. Multimaterial DIW approaches are compared by printhead configuration and the resulting modes of material organization, including material switching, compositional adjustment, and core-shell deposition. Flexible sensors are organized around conductive ink design, sensing architecture design, and core-shell fiber design, while pneumatic actuators are reviewed as an important application in soft robotics. This recategorization reveals that high-fidelity silicone DIW is governed by the coordinated control of ink rheology and post-deposition stabilization, whereas multimaterial integration is strongly influenced by how different materials are spatially organized during printing. By linking formulation, stabilization strategy, material organization, and device architecture, this review provides a unified framework for understanding and designing silicone-rubber DIW systems. Finally, machine-learning-assisted material and process optimization and faster printing are discussed as future directions.</p>","PeriodicalId":87,"journal":{"name":"Materials Horizons","volume":" ","pages":""},"PeriodicalIF":11.4,"publicationDate":"2026-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149331743","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Tuning of exciton delocalization dynamics in organic/inorganic hybrid heterostructures through solvent-mediated ordering for neuromorphic applications.","authors":"Sourav Dey, Md Saifuddin, P K Giri","doi":"10.1039/d6mh01951j","DOIUrl":"https://doi.org/10.1039/d6mh01951j","url":null,"abstract":"<p><p>Optoelectronic synapses (OESs) with linear photocurrent generation and prolonged decay are critical for energy-efficient neuromorphic vision and in-memory computing. In solution-processed organic/inorganic hybrid heterostructures (HHs), however, the role of exciton dynamics in the organic layer in governing photocarrier relaxation behavior remains poorly understood. Here, we demonstrate that exciton delocalization in poly(3-hexylthiophene) [P3HT] can be systematically tuned <i>via</i> solvent-controlled molecular ordering in P3HT/Bi₂O₂Se HHs to tailor synaptic performance. By varying the casting solvent, we modulate P3HT crystallinity, conjugation length, and energetic disorder, which directly regulates exciton delocalization and interfacial charge separation, while Bi₂O₂Se provides a high-mobility transport channel. Chloroform-processed P3HT films with the highest aggregate fraction, longest conjugation length, and lowest disorder exhibit sublinear photocurrent generation and extended photomemory, ideal for temporal integration. In contrast, chlorobenzene-processed films show faster, more nonlinear responses with rapid decay due to suppressed exciton delocalization. The chloroform-processed OES operates at an ultralow voltage of 100 mV and emulates essential synaptic functions under optical stimuli. Leveraging experimentally extracted long-term potentiation characteristics, artificial neural networks achieve 92.0% accuracy on MNIST and 89.6% on ORL face recognition. A hardware-inspired U-Net further attains 85.5% validation accuracy on Cityscapes semantic segmentation. This work establishes solvent engineering as a general strategy to tailor exciton dynamics in organic/inorganic HHs, enabling high-performance OESs for energy-efficient neuromorphic vision and computing.</p>","PeriodicalId":87,"journal":{"name":"Materials Horizons","volume":" ","pages":""},"PeriodicalIF":11.4,"publicationDate":"2026-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149331744","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"A unified analytical model for antiambipolar transport in organic mixed ionic-electronic transistors.","authors":"Marcos Luginieski, Bruno Bassi Millan Torres, Bianca de Andrade Feitosa, Henrique Frulani de Paula Barbosa, Björn Lüssem, Gregório Couto Faria","doi":"10.1039/d6mh01595f","DOIUrl":"https://doi.org/10.1039/d6mh01595f","url":null,"abstract":"<p><p>Antiambipolar transport, characterized by a bell-shaped transfer response with gate bias, has emerged as a key functionality for unconventional electronic devices, including neuromorphic circuits, single-transistor artificial neurons, and signal processing elements. Despite increasing experimental reports in organic electrochemical transistors (OECTs), a predictive understanding of the physical mechanisms governing antiambipolar behavior remains lacking, limiting rational device design. Here, we establish a general comprehensive analytical framework that captures antiambipolar transport in OECTs by explicitly coupling redox processes with electronic conduction. The model reveals that antiambipolarity arises from the competition between singly and doubly charged species, leading to a non-monotonic modulation of channel current. We derive closed-form expressions that quantitatively reproduce the transfer characteristics and identify key parameters controlling peak position, width, and magnitude. The framework provides direct design rules to engineer antiambipolar response through material properties, device geometry, and operating conditions. In fact, the model is shown to closely reproduce the response of ten commonly used p- and n-type OMIECs operated in varying electrolytes, including poly(benzimidazobenzophenanthroline) (BBL) and poly(3-hexylthiophene) (P3HT), highlighting the generality of the model and establishing a pathway to achieve this transport regime in a broad range of organic semiconductors. These results unify previous observations and enable rational design of antiambipolar functionalities in mixed ionic-electronic systems, paving the way for their broader implementation in advanced electronic systems.</p>","PeriodicalId":87,"journal":{"name":"Materials Horizons","volume":" ","pages":""},"PeriodicalIF":11.4,"publicationDate":"2026-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149316140","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Accelerated intraporous blood flow in directional sponges amplifies coagulation factor activation for rapid hemostasis.","authors":"Jiahui Liu, Zifan Zheng, Zehuan Li, Wenjie Fu, Xuanke Huang, Weiling He, Liqiong Liao, Qianming Lin","doi":"10.1039/d6mh01715k","DOIUrl":"https://doi.org/10.1039/d6mh01715k","url":null,"abstract":"<p><p>Rapid blood uptake is essential for porous hemostats, yet fast intraporous transport can hinder clot stabilization by dispersing coagulation components before a stable clot forms. Here, we show that directional confinement transforms rapid blood flow from a potential liability into an active driver of coagulation. Directionally freeze-cast sponges with tunable, aligned channels were engineered to regulate intraporous blood flow while maintaining comparable bulk chemistry. Within the investigated flow regime, faster directional flow promoted the early delivery and enrichment of erythrocytes, platelets, blood proteins, and coagulation factor XII (FXII) throughout the aligned pore network. Mechanistically, flow-mediated FXII enrichment accelerated its conversion to activated FXII (FXIIa) and strengthened the FXIIa/plasma kallikrein-dependent contact activation loop. This response propagated through increased factor Xa (FXa) and thrombin (FIIa) generation, ultimately accelerating fibrin formation and producing dense clot networks that incorporated abundant erythrocytes and platelets. <i>In vitro</i> coagulation assays and <i>in vivo</i> bleeding models further demonstrated that blood-flow-accelerating sponges coupled rapid blood uptake with accelerated clot formation, thereby reducing blood loss and shortening the time to hemostasis. These findings establish confined intraporous blood flow as an active and programmable material parameter that regulates coagulation-factor delivery and sequential cascade activation. Harnessing flow-amplified contact activation provides a counterintuitive design principle for reconciling rapid blood transport with robust clot consolidation in porous hemostatic dressings.</p>","PeriodicalId":87,"journal":{"name":"Materials Horizons","volume":" ","pages":""},"PeriodicalIF":11.4,"publicationDate":"2026-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149316141","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Location-dependent effect of spectator cations on the hydrogen evolution reaction.","authors":"Mohamed Okasha, Saikiran S Khamgaonkar, Vivek Maheshwari","doi":"10.1039/d6mh01436d","DOIUrl":"https://doi.org/10.1039/d6mh01436d","url":null,"abstract":"<p><p>Incorporating alkaline earth metal cations (Mg²⁺, Ca²⁺, Sr²⁺, and Ba²⁺) into the Stern layer of Au and Au-Pt chain-like nanoparticle catalysts <i>via</i> a self-assembly process has been found to modulate alkaline and acidic HERs by tuning both water adsorption/desorption and OH^- desorption <i>via</i> hard-soft acid-base (HSAB)-governed interfacial interactions. By independently varying the cations in the Stern layer and the diffuse layer, a distinct effect is observed on the HER. The results demonstrate that cations in the Stern layer and the diffuse layer may modulate distinct elementary steps in the reaction and must be considered jointly when designing electrocatalysts for efficient hydrogen evolution.</p>","PeriodicalId":87,"journal":{"name":"Materials Horizons","volume":" ","pages":""},"PeriodicalIF":11.4,"publicationDate":"2026-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149316143","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Dual-modal synaptic operation in a van der Waals heterostructure for emotion-inspired neuromorphic processing.","authors":"Prabana Jetty, Windy Ayu Lestari, Riya Chatterjee, Yerkezhan Amangeldinova, Wonbeom Kim, Kamila Karybayeva, Somnath S Kundale, Jun Hong Park","doi":"10.1039/d6mh01495j","DOIUrl":"https://doi.org/10.1039/d6mh01495j","url":null,"abstract":"<p><p>Substantial progress has been made in artificial emotion-recognition systems; however, reproducing neurotransmitter-mediated emotional processing remains a major challenge for neuromorphic computing. In this study, we report bimodally modulated artificial synapses based on a van der Waals-stacked graphene quantum dot (GQD)/MoS₂ heterostructure that integrates dopamine and optical stimuli for emotion-inspired neuromorphic processing. Incorporation of GQDs increases the ON-state current and dynamic range and improves relearning behavior and synaptic weight modulation. The GQD/MoS₂ heterostructure exhibits dopamine-dependent electrical responses at concentrations of 1-5 nM and stable synaptic plasticity with retention maintained over the 1000 s measurement period. Optical stimulation in the presence of dopamine produces postsynaptic current (PSC) increases that exceed the additive expectation calculated from the individual optical-only and dopamine-only responses, supporting synergistic enhancement under the tested conditions. Device-informed facial emotion recognition simulations achieved an accuracy of 73.4% on the FER-2013 dataset using a convolutional neural network (CNN). Separately, classification of PSC-derived temporal signals using electroencephalography (EEG)-inspired processing achieved an accuracy of 76.6% with a support vector machine (SVM). These findings highlight the potential of this approach for affective computing and human-machine interaction.</p>","PeriodicalId":87,"journal":{"name":"Materials Horizons","volume":" ","pages":""},"PeriodicalIF":11.4,"publicationDate":"2026-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149316142","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Valley-selective transport in 2D ferrovalley semiconductors <i>via</i> interfacial coupling and external fields.","authors":"Yu Shu, Naihua Miao, Shangbin Wu, Jing Yu, Siyu Han, Jichuan Dai, Linggang Zhu, Jian Zhou, Zhimei Sun","doi":"10.1039/d6mh01475e","DOIUrl":"https://doi.org/10.1039/d6mh01475e","url":null,"abstract":"<p><p>Harnessing the intrinsic valley degree of freedom for carrier injection is pivotal for low-power valleytronic logic and nonvolatile memory. However, designing efficient, selective injection at high-quality metal/ferrovalley-semiconductor (MFVS) interfaces remains a critical challenge. Herein, we propose a valley-selective contact strategy to achieve highly efficient carrier injection in MFVS junctions. Our investigation into interface physics across diverse electrodes reveals a trade-off: while strong-coupling contacts lower tunneling barriers, metal-induced gap states significantly degrade intrinsic valley properties. We further demonstrate that strain engineering induced by lattice mismatch not only modifies the magnitude of valley splitting but also induces a complete reversal of valley polarization. Notably, a vertical electric field enables precise modulation of the interfacial band alignment, shifting the K and K' valleys relative to the Fermi level and thereby allowing electrical switching among overall-valley Schottky, single-valley Ohmic, and overall-valley Ohmic contact regimes, leading to highly selective valley transport. Based on these mechanisms, we develop a high-performance dual-gate device model verifying electrically controlled carrier injection under ideal transport conditions. This work establishes a robust design framework for integrating valleytronic functionalities, paving the way for advanced valley-based electronics.</p>","PeriodicalId":87,"journal":{"name":"Materials Horizons","volume":" ","pages":""},"PeriodicalIF":11.4,"publicationDate":"2026-11-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149316144","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Emulsion-based strategy for size-exclusion redox flow batteries using compartmentalized redox-active electrolytes.","authors":"Seokjun Han, Benjamin Bermudez, Won Tae Choi","doi":"10.1039/d6mh01712f","DOIUrl":"10.1039/d6mh01712f","url":null,"abstract":"<p><p>While promising for grid-scale energy storage, redox flow batteries (RFBs) are hindered by ion-exchange membranes that are costly, impose conductivity-selectivity trade-offs, and undergo long-term degradation. Accordingly, replacing ion-exchange membranes with low-cost alternatives has become a critical challenge. Here, we introduce an emulsion-based size-exclusion RFB (ESRFB), representing the first demonstration of an RFB architecture that uses compartmentalized liquid droplets to suppress redox species crossover through inexpensive porous separators. Hydrophobic redox mediators, ferrocene and menadione, are confined within oil-in-water droplets whose average size (<i>ca.</i> 200 nm) exceeds the separator pore size (<i>ca.</i> 45 nm), enabling size-exclusive retention while the continuous aqueous phase maintains ionic conduction. Chronoamperometry at a carbon ultramicroelectrode verified electrochemical reactions of droplet-confined mediators upon droplet-electrode collision. Flow cell testing demonstrated stable capacity and voltage efficiency over 90 cycles, with 63% energy efficiency. These results establish the feasibility of cost-effective size-exclusion RFBs based on compartmentalized electrolytes.</p>","PeriodicalId":87,"journal":{"name":"Materials Horizons","volume":" ","pages":""},"PeriodicalIF":11.4,"publicationDate":"2026-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149293344","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Closing the perovskite loop: aqueous recovery and reuse of MAPbI₃ for film, device, and nanocrystal reuse.","authors":"Zhaoyi Du, Ding Ding, Longren Li, Weitao Qian, Enny Tran, Milo S P Shaffer, Artem A Bakulin, Nicola Gasparini, Martyn A McLachlan","doi":"10.1039/d6mh01719c","DOIUrl":"https://doi.org/10.1039/d6mh01719c","url":null,"abstract":"<p><p>The rapid commercialisation of organic-inorganic metal halide perovskites (MHPs) presents significant end-of-life challenges, particularly owing to the environmental and health risks their lead content poses. Despite efforts to improve perovskite device performance, comparatively little attention has been given to safe and sustainable recycling, with reported approaches being reliant on hazardous solvents, including DMF. Here, we report the development and use of a water-based solvent for the selective recovery of methylammonium lead iodide (MAPbI₃) from MHP devices. The solvent comprises of water with low concentrations of dissolved malic acid, β-alanine, and sodium iodide (NaI), in which the organic additives enable MAPbI₃ dissolution and NaI supports direct MHP recovery. Owing to the temperature dependent solubility of MAPbI₃ in our solvent, high-purity powders can be recovered through precipitation by solvent cooling. Films fabricated from recycled MAPbI₃ exhibit microstructures and bandgaps comparable to those prepared from pristine MAPbI₃, whilst recycled films show improved morphological uniformity and reduced non-radiative recombination. In photoconductor devices, recycled MAPbI₃ films deliver a higher photocurrent density, 1.48 × 10^-5 A cm^-2, and lower dark current density, 1.25 × 10^-7 A cm^-2 compared to their pristine analogues. When incorporated into p-i-n photovoltaic devices, recycled MAPbI₃ films retain >90% of the efficiency of pristine devices. Furthermore, demonstrating the versatility of the solvent system beyond thin-film reuse, MAPbI₃ recovered from thin films is successfully repurposed for the preparation of perovskite nanocrystals. Overall, this work establishes a green and efficient route for the recovery, recycling, and reuse of metal halide perovskites (MHPs), supporting a more circular lifecycle for emerging perovskite optoelectronics.</p>","PeriodicalId":87,"journal":{"name":"Materials Horizons","volume":" ","pages":""},"PeriodicalIF":11.4,"publicationDate":"2026-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC13717556/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149293297","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}