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Universal Integration of 2D Organic Single Crystals With Fluorinated Polymer Dielectrics for High-Performance Transistors and Single-Pixel Imaging Applications 二维有机单晶与氟化聚合物电介质的通用集成,用于高性能晶体管和单像素成像应用
IF 19 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-04 DOI: 10.1002/adfm.74393
Huchao Li, Shuchao Qin, Wen Xu, Guofeng Tian, Yunfeng Deng, Zhixin Hu, Xin Ye, Hui Yang, Lang Jiang, Deyang Ji, Wenping Hu
Organic single-crystal field-effect transistors (OSCFETs) are regarded as an ideal platform for investigating intrinsic charge transport behaviors and developing high-performance organic electronic devices, thanks to their ordered molecular stacking and minimal grain boundary defects. However, conventional integration methods frequently introduce impurities that induce interface defects or crystal damage, significantly impairing charge transport efficiency-a long-standing limitation plaguing diverse organic semiconductors. To address this critical challenge, we propose a universal strategy for the integration of two-dimensional (2D) organic single crystals with fluorinated polymer dielectrics. This approach synergistically combines an in-house microspacing in-air sublimation (MAS) growth technique with a gentle, damage-free transfer process, effectively eliminating interfacial imperfections. The resulting high-quality crystal-dielectric interfaces enable OSCFETs to achieve exceptional comprehensive performance: a record-high mobility of 18.9 cm2 V−1 s−1, ultralow operating voltage of −5 V, ultrafast photoresponse of 30 µs, outstanding high-speed image acquisition capability, and robust dual-mode driving performance for organic light-emitting diodes (OLED). This work establishes a universal method for constructing high-quality single crystals on polymer dielectrics, which holds broad implications for advancing high-speed sensing, imaging technologies, flexible displays, and integrated logic circuits.
有机单晶场效应晶体管(oscfet)由于其有序的分子堆叠和极小的晶界缺陷,被认为是研究本征电荷输运行为和开发高性能有机电子器件的理想平台。然而,传统的集成方法经常引入杂质,导致界面缺陷或晶体损伤,显著降低电荷传输效率,这是困扰多种有机半导体的长期限制。为了解决这一关键挑战,我们提出了一种将二维(2D)有机单晶与氟化聚合物电介质集成的通用策略。该方法将内部微间距空气升华(MAS)生长技术与温和、无损伤的转移过程相结合,有效地消除了界面缺陷。由此产生的高质量晶体介电界面使oscfet实现了卓越的综合性能:18.9 cm2 V - 1 s - 1的创纪录高迁移率,- 5 V的超低工作电压,30µs的超快光响应,出色的高速图像采集能力,以及有机发光二极管(OLED)的强大双模驱动性能。这项工作建立了在聚合物电介质上构建高质量单晶的通用方法,这对推进高速传感、成像技术、柔性显示和集成逻辑电路具有广泛的意义。
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引用次数: 0
Epoxy Network Hosts Confine Small Molecule Guests for Enhancing Phosphorescence Through F-π and π-π Synergistic Interactions 通过F-π和π-π协同作用增强磷光的环氧网络宿主限制小分子客体
IF 19 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-04 DOI: 10.1002/adfm.202530467
Xinyue Xu, Yanji Zhu, Xuewei Jiao, Haonan Liu, Haodong Hu, Yue Zhang, Junqi Ning, Huaiyuan Wang
Organic room-temperature phosphorescent (RTP) materials have attracted significant interest in information security and anti-counterfeiting due to their unique afterglow properties. However, the role of non-covalent interactions in enhancing phosphorescence remains insufficiently explored. Herein, we report a composite coating based on the synergistic effects of F-π and π-π stacking interactions within a dual-phase 3D covalently cross-linked network, by confining small molecular guests within an epoxy network host. The coating exhibits an ultra-long room-temperature phosphorescence (URTP) lifetime of up to 5.40 s, representing the longest lifetime reported in an epoxy resin system. The coating also displays switchable URTP and excellent surface characteristics, enabling the creation of rewritable anti-counterfeiting labels through light-activated printing and thermal erasure. Its low surface energy (15.85 mN·m−1) and self-cleaning ability ensure the long-term stability and concealment of encoded information. This work highlights the efficacy of engineering non-covalent interactions for the development of high-performance, erasable organic phosphorescent materials in anti-counterfeiting applications.
{"title":"Epoxy Network Hosts Confine Small Molecule Guests for Enhancing Phosphorescence Through F-π and π-π Synergistic Interactions","authors":"Xinyue Xu, Yanji Zhu, Xuewei Jiao, Haonan Liu, Haodong Hu, Yue Zhang, Junqi Ning, Huaiyuan Wang","doi":"10.1002/adfm.202530467","DOIUrl":"https://doi.org/10.1002/adfm.202530467","url":null,"abstract":"Organic room-temperature phosphorescent (RTP) materials have attracted significant interest in information security and anti-counterfeiting due to their unique afterglow properties. However, the role of non-covalent interactions in enhancing phosphorescence remains insufficiently explored. Herein, we report a composite coating based on the synergistic effects of F-π and π-π stacking interactions within a dual-phase 3D covalently cross-linked network, by confining small molecular guests within an epoxy network host. The coating exhibits an ultra-long room-temperature phosphorescence (URTP) lifetime of up to 5.40 s, representing the longest lifetime reported in an epoxy resin system. The coating also displays switchable URTP and excellent surface characteristics, enabling the creation of rewritable anti-counterfeiting labels through light-activated printing and thermal erasure. Its low surface energy (15.85 mN·m<sup>−1</sup>) and self-cleaning ability ensure the long-term stability and concealment of encoded information. This work highlights the efficacy of engineering non-covalent interactions for the development of high-performance, erasable organic phosphorescent materials in anti-counterfeiting applications.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"302 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122406","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Carbon Nanotubes Assembled Ordered Macro-Microporous Superstructure as Bifunctional Oxygen Electrocatalyst for Long-Life Rechargeable Zn–Air Batteries 碳纳米管组装有序宏观微孔上层结构作为长寿命可充电锌空气电池的双功能氧电催化剂
IF 19 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-04 DOI: 10.1002/adfm.202531733
Shilong Wen, Ke Ma, Yongfang Zhang, Ying Wang, Wenjie Yu, Liyang Shao, Xue Yang, Yanchao Zhao, Cong Han, Rutao Wang, Jianxing Shen, Enyan Guo, Liting Yan, Lili Han, Xuebo Zhao, Lianzhou Wang
Achieving precise fabrication of ordered superstructures with multifunctional catalytic activity is fascinating but elusive due to uncontrollable interfacial energy and growth kinetics at the material surface. Herein, we develop a facile strategy for oriented formation of carbon nanotubes (CNT) anchored on three-dimensionally ordered macro-microporous (3DOM) superstructure derived from a Co-based 3DOM metal-organic framework (3DOM-MOF). Mechanism studies based on density functional theory (DFT) calculations and in situ spectroscopy reveal that the synergistic coupling of curved CNTs supports and Co nanoparticles in the as-prepared Co-based porous superstructures CNTs catalysts (Co-HOPS-CNTs20D) can regulate the electronic structure of the isolated Co-N4 sites, thus optimizing the binding strength of the oxygenated intermediates and facilitating intrinsic catalyst activity. The unique feature of the superstructure is validated using 3D transmission electron microscopy tomography, and the corresponding finite element analysis (FEA) simulations prove enhanced conductivity of Co-HOPS-CNTs20D superstructure, which facilitates transfer efficiency of electrons and improves catalytic activity. As a result, the Co-HOPS-CNTs20D exhibits a low overpotential of 287 mV at 10 mA cm−2 for OER and a high ORR half-wave potential of 0.863 V. The zinc-air battery incorporating Co-HOPS-CNTs20D demonstrates efficient and stable operation over a period of 160 h.
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引用次数: 0
Heterogeneous Coherent Interface Enabling Nonstochastic Crystallization for Phase-Change Memory 实现相变存储器非随机结晶的异质相干接口
IF 19 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-04 DOI: 10.1002/adfm.202523223
Tian-Yu Zhao, Jiahao Li, Nian-Ke Chen, Bai-Qian Wang, Xiaomin Cheng, Shun-Yao Qin, Huan-Ran Ding, Shengbai Zhang, Hong-Bo Sun, Xiangshui Miao, Xian-Bin Li
Phase-change memory (PCM) displays great promise for the storage-class memory (SCM) technology due to its combination of fast speed of dynamic random-access memory and nonvolatility of Flash. Yet, to meet the high industrial requirement of write/erase speed for the SCM application, robust strategies for further accelerating phase transition, particularly from amorphous to crystalline PCM materials, are urgently needed. In this work, we propose a unique strategy of coherent-interface induced ultrafast crystallization in PCM materials. Employing rock-salt YAs/Ge2Sb2Te5 as a prototype, systematic first-principles molecular dynamics demonstrate that rapid nonstochastic crystallization behaviors can be achieved by the rock-salt-lattice-matching and high-temperature-resistant heterogeneous interface attached to the popular PCM material Ge2Sb2Te5 (GST). Further experiment shows that the YAs-incorporated GST device has a faster SET process compared with the pure GST device. Finally, to extend the strategy in the family of inorganic materials, high-throughput screening from over 150 000 structures discovers as many as 71 candidates for coherent interfaces with PCM GST. The present study establishes a promising strategy to overcome the speed bottleneck of PCM through atomic-scale interface design for future storage-class memory implementation.
相变存储器(PCM)由于其结合了动态随机存取存储器的快速速度和闪存的非易失性,在存储级存储器(SCM)技术中显示出很大的发展前景。然而,为了满足SCM应用对写入/擦除速度的高工业要求,迫切需要进一步加速相变的稳健策略,特别是从非晶到结晶的PCM材料。在这项工作中,我们提出了一种独特的相干界面诱导PCM材料的超快结晶策略。以岩盐YAs/Ge2Sb2Te5为原型,系统第一性原理分子动力学表明,岩盐晶格匹配和耐高温非均相界面附着在流行的PCM材料Ge2Sb2Te5 (GST)上可以实现快速非随机结晶行为。进一步的实验表明,与纯GST器件相比,yas - GST器件具有更快的SET过程。最后,为了将该策略扩展到无机材料家族,从超过150,000种结构中进行高通量筛选,发现了多达71种与PCM GST相一致的候选界面。本研究建立了一个有希望的策略,通过原子尺度的接口设计来克服PCM的速度瓶颈,以实现未来的存储级存储器。
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引用次数: 0
Diethyl Sulfide as a Multifunctional Electrolyte Additive for Enhancing Electrochemical Performance of Lithium Metal Batteries 二乙基硫化物作为提高锂金属电池电化学性能的多功能电解质添加剂
IF 19 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-04 DOI: 10.1002/adfm.202529688
Wenjie Zhang, Xiaosong Xiong, Run Xu, Guangyao Xiang, Tao Wang, Xu Liu, Yong Wang, Lili Liu, Yuping Wu
With the increasing demand for energy storage devices with higher energy density, lithium metal anode (LMA) has emerged as promising candidate due to ultra-high theoretical specific capacity (3860 mAh g−1) and the lowest reduction potential (-3.04 V vs. S.H.E.). However, the practical application of LMA is still restricted by notorious active lithium loss and lithium dendrite growth, which cause low Coulombic efficiency, poor cycling life, and even potential safety hazards. In this study, a multifunctional diethyl sulfide electrolyte additive is proposed to synergistically construct a stable Li2S-rich solid electrolyte interphase (SEI) and Li2S/Li2SO4/Li2SO3-rich cathode electrolyte interphases (CEI), which could accelerate Li ions (Li+) transport kinetics and enhance the interfacial stability during long-term cycling. Moreover, the sulfur-rich composite in electrolyte interface could reduce the energy barrier for Li+ desolvation and thereby enhance interface dynamics. Based on these merits, the introduction of 2.0 vol.% diethyl sulfide into a carbonate electrolyte (without FEC) enables the lithium anode to achieve a 7-fold enhancement in long-term cycling performance. More impressively, the Li||LiFePO4 (LFP) pouch cell with the modified electrolyte achieves an outstanding capacity retention of 98.75% after 200 cycles at 0.1 C. The multifunctional diethyl sulfide additive paves the way for high-performance LMBs for practical applications.
随着对高能量密度储能器件的需求不断增加,锂金属阳极(LMA)因其超高的理论比容量(3860 mAh g - 1)和最低的还原电位(-3.04 V vs. S.H.E.)而成为有希望的候选材料。然而,LMA的实际应用仍然受到活性锂损失和锂枝晶生长严重的制约,导致库仑效率低,循环寿命差,甚至存在安全隐患。本研究提出了一种多功能二乙基硫化物电解质添加剂,协同构建稳定的富Li2S固体电解质界面(SEI)和富Li2S/Li2SO4/ li2so3阴极电解质界面(CEI),加速Li离子(Li+)传输动力学,增强界面在长期循环过程中的稳定性。此外,电解质界面中的富硫复合材料可以降低Li+脱溶的能垒,从而增强界面动力学。基于这些优点,在碳酸电解质(不含FEC)中引入2.0 vol.%的二乙基硫化物,使锂阳极的长期循环性能提高了7倍。更令人印象深刻的是,在0.1℃下,经过200次循环后,Li||LiFePO4 (LFP)袋状电池的容量保持率达到98.75%。多功能二乙基硫化物添加剂为高性能LFP的实际应用铺平了道路。
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引用次数: 0
An All-in-One DNA Nanodevice as a Programmed Theranostic Platform for Intelligent Cancer Cell Identification and On-Site Drug Release 一个一体化的DNA纳米装置作为智能癌细胞识别和现场药物释放的程序治疗平台
IF 19 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-04 DOI: 10.1002/adfm.202531762
Yi Yuan, Qiufeng Song, Linwen Lan, Xuefen Chen, Jiangchuan Du, Linjun Zhang, Nan Chen, Zhifa Shen, Chang Xue
Chemotherapy remains the cornerstone of malignant tumor treatment; however, off-target effects and severe systemic toxicity limit its efficacy. Here, we developed a programmable theranostic platform based on an all-in-one smart DNA nanodevice (SND) that integrates a programmable cancer-cell classifier (PCC) with a responsive delivery system (RDS). By employing a modular design that permits the customization of aptamer combinations for specific cancer cell types, the platform achieves accurate tumor recognition and spatially controlled drug release. Functioning as a dual-aptamer molecular guide, the PCC utilizes an interlocked configuration to identify cell-surface biomarkers in a stepwise manner, thereby ensuring highly specific target cell recognition. The RDS is constructed from a 1D central trunk flanked by double-stranded drug-loading units, a structure that confers high payload capacity and nuclease-enhanced resistance. These peripheral units also function as recognition elements for endogenous stimuli; upon activation, they trigger conformational changes that facilitate efficient intracellular drug release. In vivo studies in tumor-bearing mice demonstrate that this programmable theranostic platform selectively accumulates in tumor tissues, leading to marked inhibition of tumor growth and a substantial reduction in systemic toxicity. By integrating programmable molecular recognition with stimulus-responsive drug delivery, our theranostic platform offers a promising strategy for advancing targeted cancer therapy.
{"title":"An All-in-One DNA Nanodevice as a Programmed Theranostic Platform for Intelligent Cancer Cell Identification and On-Site Drug Release","authors":"Yi Yuan, Qiufeng Song, Linwen Lan, Xuefen Chen, Jiangchuan Du, Linjun Zhang, Nan Chen, Zhifa Shen, Chang Xue","doi":"10.1002/adfm.202531762","DOIUrl":"https://doi.org/10.1002/adfm.202531762","url":null,"abstract":"Chemotherapy remains the cornerstone of malignant tumor treatment; however, off-target effects and severe systemic toxicity limit its efficacy. Here, we developed a programmable theranostic platform based on an all-in-one smart DNA nanodevice (SND) that integrates a programmable cancer-cell classifier (PCC) with a responsive delivery system (RDS). By employing a modular design that permits the customization of aptamer combinations for specific cancer cell types, the platform achieves accurate tumor recognition and spatially controlled drug release. Functioning as a dual-aptamer molecular guide, the PCC utilizes an interlocked configuration to identify cell-surface biomarkers in a stepwise manner, thereby ensuring highly specific target cell recognition. The RDS is constructed from a 1D central trunk flanked by double-stranded drug-loading units, a structure that confers high payload capacity and nuclease-enhanced resistance. These peripheral units also function as recognition elements for endogenous stimuli; upon activation, they trigger conformational changes that facilitate efficient intracellular drug release. In vivo studies in tumor-bearing mice demonstrate that this programmable theranostic platform selectively accumulates in tumor tissues, leading to marked inhibition of tumor growth and a substantial reduction in systemic toxicity. By integrating programmable molecular recognition with stimulus-responsive drug delivery, our theranostic platform offers a promising strategy for advancing targeted cancer therapy.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"38 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122276","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Laser Engineering of HfN-Based Nanoparticles for Safe NIR-I Photothermal and X-ray Enhancing Cancer Therapies 用于NIR-I光热和x射线增强癌症治疗的hnfn纳米颗粒激光工程
IF 19 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-04 DOI: 10.1002/adfm.202529532
Julia S. Babkova, Ivan V. Zelepukin, Lyubov V. Gorelik, Anton L. Popov, Andrei I. Pastukhov, Gleb V. Tikhonowski, Maxim S. Savinov, Danil D. Kolmanovich, Nikita A. Pivovarov, Alina Yu. Kapitannikova, Anton A. Popov, Anna S. Sogomonyan, Vsevolod A. Skribitsky, Aziz B. Mirkasymov, Andrei V. Kabashin, Sergey M. Deyev
Transition metal nitrides are robust alternatives to noble metals in plasmonics, offering strong NIR absorption, high melting points, and chemical stability. Hafnium nitride (HfN) nanoparticles are especially promising owing to the high atomic number of hafnium, which could provide X-ray-based theranostic functionalities in addition to the prominent plasmonic properties. However, their biomedical potential has remained unexplored due to difficulties in synthesis of pure water-dispersible nanostructures. Here, we use femtosecond laser ablation in acetone to produce HfN-based nanoparticles exhibiting a red-shifted plasmon resonance spanning both the NIR-I and NIR-II windows. We then present the first in vivo assessment of the biocompatibility, photothermal performance, and radiosensitizing capacity of HfN-based nanomaterials. We show that PEGylated HfN nanoparticles exhibit negligible cytotoxicity across three cancer cell lines in vitro and no significant long-term adverse effects in healthy mice following intravenous administration. NIR-I photothermal therapy of 4T1 tumor-bearing mice after systemic nanoparticle administration leads to a 2.4-fold suppression of tumor growth and a significant extension of survival. The multimodal therapeutic potential of HfN is demonstrated by the enhanced efficacy of X-ray radiotherapy after local administration of nanoparticles. Laser ablated engineering of hafnium nitrides establishes this nanomaterial as a promising candidate for multimodal optical and radiosensitizing theranostics.
{"title":"Laser Engineering of HfN-Based Nanoparticles for Safe NIR-I Photothermal and X-ray Enhancing Cancer Therapies","authors":"Julia S. Babkova, Ivan V. Zelepukin, Lyubov V. Gorelik, Anton L. Popov, Andrei I. Pastukhov, Gleb V. Tikhonowski, Maxim S. Savinov, Danil D. Kolmanovich, Nikita A. Pivovarov, Alina Yu. Kapitannikova, Anton A. Popov, Anna S. Sogomonyan, Vsevolod A. Skribitsky, Aziz B. Mirkasymov, Andrei V. Kabashin, Sergey M. Deyev","doi":"10.1002/adfm.202529532","DOIUrl":"https://doi.org/10.1002/adfm.202529532","url":null,"abstract":"Transition metal nitrides are robust alternatives to noble metals in plasmonics, offering strong NIR absorption, high melting points, and chemical stability. Hafnium nitride (HfN) nanoparticles are especially promising owing to the high atomic number of hafnium, which could provide X-ray-based theranostic functionalities in addition to the prominent plasmonic properties. However, their biomedical potential has remained unexplored due to difficulties in synthesis of pure water-dispersible nanostructures. Here, we use femtosecond laser ablation in acetone to produce HfN-based nanoparticles exhibiting a red-shifted plasmon resonance spanning both the NIR-I and NIR-II windows. We then present the first in vivo assessment of the biocompatibility, photothermal performance, and radiosensitizing capacity of HfN-based nanomaterials. We show that PEGylated HfN nanoparticles exhibit negligible cytotoxicity across three cancer cell lines in vitro and no significant long-term adverse effects in healthy mice following intravenous administration. NIR-I photothermal therapy of 4T1 tumor-bearing mice after systemic nanoparticle administration leads to a 2.4-fold suppression of tumor growth and a significant extension of survival. The multimodal therapeutic potential of HfN is demonstrated by the enhanced efficacy of X-ray radiotherapy after local administration of nanoparticles. Laser ablated engineering of hafnium nitrides establishes this nanomaterial as a promising candidate for multimodal optical and radiosensitizing theranostics.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"288 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122316","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Accelerated Discovery of High Performance Ni3S4/Ni3Mo HER Catalysts via Bayesian Optimization 利用贝叶斯优化加速发现高性能Ni3S4/Ni3Mo HER催化剂
IF 19 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-04 DOI: 10.1002/adfm.202528363
Namuersaihan Namuersaihan, Zhiqiang Zhao, Oliver J. Conquest, Ying Shu, Haoyue Sun, Chunjing Su, Qi Cheng, Aloysius Soon, Catherine Stampfl, Jun Huang
The hydrogen evolution reaction (HER) in alkaline media is a promising strategy for sustainable hydrogen production, but the exploration of efficient and durable HER electrocatalysts is often hindered by the empirical and time-consuming nature of traditional synthesis. Herein, a machine learning (ML)–driven strategy combining Bayesian optimization is introduced to achieve the rational design of Ni3S4/Ni3Mo heterostructures for alkaline HER. By coupling predictive modeling with experimental feedback, this approach efficiently navigated a complex synthesis space and identified conditions yielding a structurally and electronically optimized catalyst. The optimized Ni3S4/Ni3Mo exhibits a vibrant morphological evolution—from compact buds to blooming petal-like structures—enabling enriched active sites and accelerated mass transport. Guided by Bayesian optimization, the optimized Ni3S4/Ni3Mo achieves a 10.5-fold enhancement in Cdl and delivers an exceptionally low overpotential of 18.2 mV at 100 mA cm−2, outperforming most reported transition-metal catalysts and even surpassing commercial Pt/C. Mechanistic insights from in situ Raman and DFT reveal that interfacial charge redistribution between Ni3S4 and Ni3Mo optimizes H* adsorption (ΔGH* ≈ 0.04 eV) and significantly reduces the water-dissociation barrier (0.08 eV), thereby accelerating reaction kinetics. This work demonstrates how the ML-guided optimization can synergistically couple morphology control, interfacial engineering with electronic tuning, offering a generalizable framework for intelligent catalyst discovery and mechanistic understanding in electrochemical energy conversion.
{"title":"Accelerated Discovery of High Performance Ni3S4/Ni3Mo HER Catalysts via Bayesian Optimization","authors":"Namuersaihan Namuersaihan, Zhiqiang Zhao, Oliver J. Conquest, Ying Shu, Haoyue Sun, Chunjing Su, Qi Cheng, Aloysius Soon, Catherine Stampfl, Jun Huang","doi":"10.1002/adfm.202528363","DOIUrl":"https://doi.org/10.1002/adfm.202528363","url":null,"abstract":"The hydrogen evolution reaction (HER) in alkaline media is a promising strategy for sustainable hydrogen production, but the exploration of efficient and durable HER electrocatalysts is often hindered by the empirical and time-consuming nature of traditional synthesis. Herein, a machine learning (ML)–driven strategy combining Bayesian optimization is introduced to achieve the rational design of Ni<sub>3</sub>S<sub>4</sub>/Ni<sub>3</sub>Mo heterostructures for alkaline HER. By coupling predictive modeling with experimental feedback, this approach efficiently navigated a complex synthesis space and identified conditions yielding a structurally and electronically optimized catalyst. The optimized Ni<sub>3</sub>S<sub>4</sub>/Ni<sub>3</sub>Mo exhibits a vibrant morphological evolution—from compact buds to blooming petal-like structures—enabling enriched active sites and accelerated mass transport. Guided by Bayesian optimization, the optimized Ni<sub>3</sub>S<sub>4</sub>/Ni<sub>3</sub>Mo achieves a 10.5-fold enhancement in <i>C</i><sub>dl</sub> and delivers an exceptionally low overpotential of 18.2 mV at 100 mA cm<sup>−2</sup>, outperforming most reported transition-metal catalysts and even surpassing commercial Pt/C. Mechanistic insights from in situ Raman and DFT reveal that interfacial charge redistribution between Ni<sub>3</sub>S<sub>4</sub> and Ni<sub>3</sub>Mo optimizes H* adsorption (Δ<i>G</i><sub>H*</sub> ≈ 0.04 eV) and significantly reduces the water-dissociation barrier (0.08 eV), thereby accelerating reaction kinetics. This work demonstrates how the ML-guided optimization can synergistically couple morphology control, interfacial engineering with electronic tuning, offering a generalizable framework for intelligent catalyst discovery and mechanistic understanding in electrochemical energy conversion.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"47 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122403","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Beyond the Edge: Charge-Transfer Excitons in Organic Donor-Acceptor Cocrystals 超越边缘:有机供体-受体共晶中的电荷转移激子
IF 19 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-04 DOI: 10.1002/adfm.202530499
Sebastian Anhäuser, Ana M. Valencia, Sergei I. Ivlev, Marc Zeplichal, Andreas Terfort, Caterina Cocchi, Gregor Witte
Charge-transfer excitons (CTXs) at organic donor/acceptor interfaces are crucial intermediates for charge separation in photovoltaic devices. While blends used in real-world devices hamper detailed characterization of CTXs, atomistic models of cocrystals offer powerful alternatives for gaining microscopic insights. In this work, we investigate electronic and optical properties of acene-perfluoroacene cocrystals (anthracene, tetracene, and pentacene), combining experimental synthesis and characterization with first-principles calculations based on many-body theory. We prepare ultrathin cocrystals for polarization-resolved transmission-absorption spectroscopy, linking exciton polarization with molecular packing. Complementing this analysis, density-functional and many-body perturbation theory reveal complex excitonic landscapes that challenge several common assumptions about CTXs in weakly interacting donor-acceptor systems. For the studied cocrystals, we demonstrate that such CTXs are not limited to the absorption onset, but also occur at higher energy and produce sharp, intense absorption features. Adopting the intrinsic molecular coordinate system, we categorize the various excitons according to their polarization and show that the transition dipole moment of the lowest energy CTX is not necessarily aligned with the donor-acceptor stacking axis. We further characterize triplet excitons from first principles, which are only indirectly accessible experimentally. This work provides a deep understanding of CTXs in organic cocrystals, developing a refined conceptual framework that is crucial for future design of environmentally sustainable photoactive materials.
{"title":"Beyond the Edge: Charge-Transfer Excitons in Organic Donor-Acceptor Cocrystals","authors":"Sebastian Anhäuser, Ana M. Valencia, Sergei I. Ivlev, Marc Zeplichal, Andreas Terfort, Caterina Cocchi, Gregor Witte","doi":"10.1002/adfm.202530499","DOIUrl":"https://doi.org/10.1002/adfm.202530499","url":null,"abstract":"Charge-transfer excitons (CTXs) at organic donor/acceptor interfaces are crucial intermediates for charge separation in photovoltaic devices. While blends used in real-world devices hamper detailed characterization of CTXs, atomistic models of cocrystals offer powerful alternatives for gaining microscopic insights. In this work, we investigate electronic and optical properties of acene-perfluoroacene cocrystals (anthracene, tetracene, and pentacene), combining experimental synthesis and characterization with first-principles calculations based on many-body theory. We prepare ultrathin cocrystals for polarization-resolved transmission-absorption spectroscopy, linking exciton polarization with molecular packing. Complementing this analysis, density-functional and many-body perturbation theory reveal complex excitonic landscapes that challenge several common assumptions about CTXs in weakly interacting donor-acceptor systems. For the studied cocrystals, we demonstrate that such CTXs are not limited to the absorption onset, but also occur at higher energy and produce sharp, intense absorption features. Adopting the intrinsic molecular coordinate system, we categorize the various excitons according to their polarization and show that the transition dipole moment of the lowest energy CTX is not necessarily aligned with the donor-acceptor stacking axis. We further characterize triplet excitons from first principles, which are only indirectly accessible experimentally. This work provides a deep understanding of CTXs in organic cocrystals, developing a refined conceptual framework that is crucial for future design of environmentally sustainable photoactive materials.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"12 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122404","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Operando SAXS/WAXS Reveals the Formation of Li+ Conduction Pathways Enabled by Apocynum Venetum-Derived Nanocellulose Operando SAXS/WAXS揭示了罗布麻衍生纳米纤维素激活Li+传导途径的形成
IF 19 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-04 DOI: 10.1002/adfm.202523000
Wenhui Cui, Shuaitong Liang, Junping Miao, Wenli Li, Hanwen An, Rongrong Yu, Juan Zhou, Ruiqi Shao, Zhiwei Xu
Molecular engineering of cellulose is essential for improving ionic conductivity and mechanical stability in solid polymer electrolytes. This work presents the first utilization of apocynum venetum, a drought-resistant biomass, as a sustainable source of cellulose nanofibers (CNFs) to investigate lithium-ion (Li+) transport mechanisms in composite polymer electrolytes for lithium metal batteries (LMBs). The reconstructed type II cellulose disrupts the polymer chain order by reorganizing hydrogen bonds and expanding amorphous regions, leading to a high Li+ transference number of 0.67 and an extended electrochemical window of 5.5 V. Operando synchrotron SAXS/WAXS reveals that CNFs modulate the structural evolution of the electrolyte and facilitate the formation of continuous Li+ conduction pathways within the amorphous phase. Through ion–dipole interactions among CNFs hydroxyl groups, PEO ether oxygens, and Li+, dynamic Li+─O coordination structures are formed, enhancing Li+ mobility. This work demonstrates the critical role of apocynum venetum-derived nanocellulose in enhancing the performance of bio-based polymer electrolytes.
{"title":"Operando SAXS/WAXS Reveals the Formation of Li+ Conduction Pathways Enabled by Apocynum Venetum-Derived Nanocellulose","authors":"Wenhui Cui, Shuaitong Liang, Junping Miao, Wenli Li, Hanwen An, Rongrong Yu, Juan Zhou, Ruiqi Shao, Zhiwei Xu","doi":"10.1002/adfm.202523000","DOIUrl":"https://doi.org/10.1002/adfm.202523000","url":null,"abstract":"Molecular engineering of cellulose is essential for improving ionic conductivity and mechanical stability in solid polymer electrolytes. This work presents the first utilization of apocynum venetum, a drought-resistant biomass, as a sustainable source of cellulose nanofibers (CNFs) to investigate lithium-ion (Li<sup>+</sup>) transport mechanisms in composite polymer electrolytes for lithium metal batteries (LMBs). The reconstructed type II cellulose disrupts the polymer chain order by reorganizing hydrogen bonds and expanding amorphous regions, leading to a high Li<sup>+</sup> transference number of 0.67 and an extended electrochemical window of 5.5 V. Operando synchrotron SAXS/WAXS reveals that CNFs modulate the structural evolution of the electrolyte and facilitate the formation of continuous Li<sup>+</sup> conduction pathways within the amorphous phase. Through ion–dipole interactions among CNFs hydroxyl groups, PEO ether oxygens, and Li<sup>+</sup>, dynamic Li<sup>+</sup>─O coordination structures are formed, enhancing Li<sup>+</sup> mobility. This work demonstrates the critical role of apocynum venetum-derived nanocellulose in enhancing the performance of bio-based polymer electrolytes.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"23 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122405","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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Advanced Functional Materials
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