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Fundamentals, Status, and Prospects of Liquid Organic Electrolytes for High-Energy Sodium-Ion Batteries. 高能钠离子电池用有机液体电解质的基本原理、现状与展望
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-19 DOI: 10.1002/adma.202519965
Xinke Cui,Shuicen Ding,Yuankun Wang,Hao Teng,Yuhe Feng,Xue Han,Xiaohui Rong,Kai Xi,Qiong Zheng,Yaxiang Lu,Weijiang Xue
Sodium-ion batteries (SIBs) have emerged as one of the most promising candidates among post-Li-ion batteries (LIBs) due to abundance and low cost of sodium resources. However, the commercialization of SIBs is hindered by their limited cell performance. Although great efforts have been made, it is still challenging to balance the trade-off between energy density and cycle life while simultaneously meeting the requirements for practical applications, which are largely governed by the stability of the electrode/electrolyte interfaces. Therefore, it is crucial to design new electrolyte components or formulations to stabilize the interphases and thus the cycling stability for high-energy and high-capacity cathodes/anodes. In this review, based on a comprehensive comparison of the fundamental mechanisms between SIBs and LIBs, the challenges and governing principles for electrolyte design in SIBs are first introduced. The progress in electrolyte designs for various high-energy cathodes is summarized according to their ion-transport characteristics and the interphase formation. Electrolyte design strategies, particularly for the high-capacity anodes, are also surveyed, together with effective electrolyte design strategies to fulfill the requirements under practical operating conditions. Finally, future perspectives on electrolyte development from the viewpoints of full cell-level performance, cost, and feasibility are highlighted. This review aims to provide a roadmap for advancing electrolyte design toward practical SIBs competitive with LIBs.
钠离子电池(SIBs)由于其丰富的钠资源和低廉的成本而成为后锂离子电池(LIBs)中最有前途的候选者之一。然而,sib的商业化受到其有限的单元性能的阻碍。尽管已经做出了巨大的努力,但在满足实际应用要求的同时,平衡能量密度和循环寿命之间的权衡仍然具有挑战性,这在很大程度上取决于电极/电解质界面的稳定性。因此,设计新的电解质成分或配方来稳定界面,从而稳定高能量和高容量阴极/阳极的循环稳定性至关重要。本文在对sib和lib的基本机理进行全面比较的基础上,首先介绍了sib中电解质设计的挑战和指导原则。从离子输运特性和间相形成方面综述了各种高能阴极电解质设计的进展。电解质设计策略,特别是大容量阳极,也进行了调查,以及有效的电解质设计策略,以满足实际操作条件下的要求。最后,从全电池级性能、成本和可行性的角度对电解质的未来发展进行了展望。这篇综述旨在为推进电解质的设计提供一个路线图,以实现与lib竞争的实用sib。
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引用次数: 0
Operationally Stable Perovskite Solar Modules Enabled by MA-Free Perovskite Crystallization and Passivation via Scalable Coating. 无ma钙钛矿结晶和可扩展涂层钝化实现运行稳定的钙钛矿太阳能组件。
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-19 DOI: 10.1002/adma.202519198
Jiazhe Xu,Shaochen Zhang,Donger Jin,Zhendong Cheng,Xiaonan Wang,Xiaohe Miao,Qinggui Li,Qile Jin,Dawei Di,Jingjing Xue,Rui Wang
Perovskite solar modules (PSMs) must deliver not only high-power conversion efficiency (PCE) but also long-term operational stability to approach commercialization. Yet efficiency and stability are both compromised when translating laboratory spin-coated perovskite solar cells (PSCs) into scalable PSMs, owing to mismatched crystallization dynamics, ineffective defect passivation, and compositional degradation. Here we resolve these challenges through a three-pronged strategy. First, we deconstruct the compositional origins of operational stability, identifying MA (methylammonium)-free Cs-FA (formamidinium) composition as intrinsically robust against continuous operation. Second, we tailor the phase-transition and crystallization pathways of air-processed scalable-coating by controlled Br incorporation in CsPbX3, which reconciles precursor solubility, nucleation kinetics, and α-phase stability, yielding dense and defect-suppressed films. Finally, we analyze the root cause of scalable passivation inefficacy and developed cyclohexanecarboxamidinium (CHCA) as a blade-coating-compatible passivator enabling uniform and durable defect suppression. The optimized devices exhibited improved PCEs up to 26.1% (0.646 cm2) and 22.8% (20.8 cm2). Meanwhile, we documented exceptional operational stability with ∼3200 h T96 for PSC and ∼2000 h T84 for PSM. Our findings establish a mechanistic framework for achieving operationally stable perovskite solar modules under industrially relevant conditions.
钙钛矿太阳能组件(psm)不仅要提供高功率转换效率(PCE),还要提供长期的运行稳定性,才能实现商业化。然而,当将实验室自旋涂覆钙钛矿太阳能电池(PSCs)转化为可扩展的psm时,由于结晶动力学不匹配,无效的缺陷钝化和成分降解,效率和稳定性都受到损害。在这里,我们通过三管齐下的战略来解决这些挑战。首先,我们解构了操作稳定性的成分来源,确定了MA(甲基铵)free Cs-FA(甲脒)组合物在连续操作中具有内在的鲁棒性。其次,我们通过在CsPbX3中控制Br的掺入来调整空气加工可缩放涂层的相变和结晶途径,从而协调前驱体溶解度、成核动力学和α-相稳定性,从而产生致密和缺陷抑制的薄膜。最后,我们分析了可扩展钝化无效的根本原因,并开发了环己烷羧基酰胺(CHCA)作为叶片-涂层兼容的钝化剂,可以均匀持久地抑制缺陷。优化后器件的pce分别提高了26.1% (0.646 cm2)和22.8% (20.8 cm2)。同时,我们记录了卓越的操作稳定性,PSC为~ 3200 h T96, PSM为~ 2000 h T84。我们的研究结果为在工业相关条件下实现操作稳定的钙钛矿太阳能组件建立了一个机制框架。
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引用次数: 0
Reconfigurable Multi-Stimuli Responsive Smart Phosphorescent Polymer Composites with Time-Dependent and Wavelength-Dependent Phosphorescence Color Evolution. 具有时间和波长依赖性磷光颜色演化的可重构多刺激响应智能磷光聚合物复合材料。
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-19 DOI: 10.1002/adma.202512099
Xiao Chen,Bin Tian,Xin Guo,Ziyi Gong,Wei Wu
Developing smart systems based on phosphorescent materials that can control the time-dependent phosphorescent color (TDPC) in response to external stimuli holds promise for advancing information encryption, but significant challenges remain. Herein, a facile strategy is proposed to construct smart phosphorescent polymer composites through immobilizing dual-emission centers with distinct stimuli sensitivities within a soft-rigid coupled hybrid matrix. The smart phosphorescent polymer composites show switchable phosphorescence between static phosphorescence and wavelength-dependent dynamic TDPC, induced by multi-stimuli (light, humidity, heat). The photoactivated phosphorescent composites transform from initial static monochromatic emission to dynamic multicolor TDPC through the synergistic effect of triplet oxygen depletion-induced selective activation of the emission centers and the distinct decay rates of the dual-emission centers. The evolution paths of TDPC also exhibit excitation-dependence. Moreover, the photoactivated composites enable reversible switching between dynamic TDPC and monochromatic phosphorescence through water and thermal stimuli, due to the combined effects of water-induced dissociation of the rigid hydrogen-bonding network and differential quenching of the dual-emission centers. The composites also exhibit recyclability and self-healing capability. The processable smart phosphorescent polymer composites with good stability demonstrate outstanding potential in multi-dimensional information encryption, opening up a new perspective for upgrading security technologies.
开发基于磷光材料的智能系统,可以根据外部刺激控制时间依赖性磷光颜色(TDPC),这有望推进信息加密,但仍存在重大挑战。本文提出了一种简单的策略,通过在软-刚性耦合混合矩阵中固定具有不同刺激灵敏度的双发射中心来构建智能磷光聚合物复合材料。智能磷光聚合物复合材料在多种刺激(光、湿、热)诱导下,在静态磷光和波长依赖的动态TDPC之间切换磷光。光激活磷光复合材料通过三态耗氧诱导的发射中心选择性活化和双发射中心不同的衰减速率的协同作用,从初始的静态单色发光转变为动态的多色TDPC。TDPC的进化路径也表现出兴奋依赖性。此外,由于水诱导的刚性氢键网络解离和双发射中心的微分猝灭的共同作用,光激活复合材料可以通过水和热刺激在动态TDPC和单色磷光之间可逆切换。复合材料还具有可回收性和自修复能力。具有良好稳定性的可加工智能磷光聚合物复合材料在多维信息加密方面具有突出的潜力,为安全技术升级开辟了新的前景。
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引用次数: 0
Photoswitchable Dual-Color Fluorescence With Large Stokes Shift From Dye-Encapsulated Metal-Organic Framework for Dynamic Cellular Imaging. 染料包封金属-有机框架中具有大斯托克斯位移的可光开关双色荧光用于动态细胞成像。
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-19 DOI: 10.1002/adma.202518371
Chenyu Li,He-Qi Zheng,Weilu Xu,Zheyan Xu,Zhengluan Liao,Guodong Qian,Yuanjing Cui
Photoswitchable dual-color fluorescent materials are highly valuable for applications in cellular imaging and super-resolution microscopy. However, realizing these materials, especially broadening their Stokes shift remains a critical challenge. Herein, a novel strategy for achieving photoswitchable dual-emission fluorescence with a large Stokes shift is proposed via a cascade energy transfer (ET) process in metal-organic frameworks (MOFs). By incorporating the photoisomerizable molecule spiropyran as an ET intermediate, and two fluorescent dyes coumarin 153 (Cou153) and methylene blue (MB) within a MOF, rho-ZMOF, the dual-color dynamic luminescent material rho-ZMOF⊃Cou153&SP&MB is achieved. When excited at 400 nm, rho-ZMOF⊃Cou153&SP&MB exhibits coumarin-centered green emission at 516 nm and methylene blue-centered red fluorescence at 700 nm, with a maximum Stokes shift of 300 nm. More importantly, these dual-color emissions can be reversibly switched on or off upon altering UV- and visible-light irradiation because of the photoswitchable cascade energy transfer from coumarin 153 to methylene blue based on the photochromic transformation of spiropyran. As an example, the potential use of rho-ZMOF⊃Cou153&SP&MB in high-resolution and depth-resolved bioimaging is demonstrated.
光开关双色荧光材料在细胞成像和超分辨率显微镜中具有重要的应用价值。然而,实现这些材料,特别是扩大它们的斯托克斯转变仍然是一个关键的挑战。本文提出了一种在金属-有机框架(mof)中通过级联能量转移(ET)过程实现具有大Stokes位移的光开关双发射荧光的新策略。通过将光异构分子螺吡喃作为ET中间体,在MOF中加入两种荧光染料香豆素153 (Cou153)和亚甲基蓝(MB), rho-ZMOF,实现了双色动态发光材料rho-ZMOF、Cou153& sp&mb。当在400 nm处激发时,rro - zmof、Cou153&SP&MB在516 nm处表现出香豆素中心的绿色荧光,在700 nm处表现出亚甲基蓝中心的红色荧光,最大斯托克斯位移为300 nm。更重要的是,这些双色发射可以在改变紫外线和可见光照射时可逆地打开或关闭,因为基于螺吡喃的光致变色转化,香豆素153的光可切换级联能量转移到亚甲基蓝。作为一个例子,展示了rho-ZMOF、Cou153&SP&MB在高分辨率和深度分辨率生物成像中的潜在用途。
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引用次数: 0
Semi-Artificial Photosynthetic Machinery for Carbon Dioxide Capture and Conversion. 二氧化碳捕获和转化的半人工光合机制。
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-19 DOI: 10.1002/adma.202521092
Shuting Huang,Qiuyuan Ren,Tianxing Zhang,Qingfeng Xu,Najun Li,Hua Li,Tao Wang,Dongyun Chen,Jianmei Lu
Producing value-added chemicals directly from CO2 powered by sunlight offers a sustainable approach to addressing both environmental and economic challenges. However, the inherent chemical stability of CO2 poses a grand challenge in achieving highly active and selective CO2 conversion. Herein, we develop a biohybrid semi-artificial photosynthetic system that integrates carbonic anhydrase (CA) and a CuZn nanozyme photosensitizer with a dendritic polymer (PPA) for the sustainable transformation of CO2 into dimethyl carbonate (DMC). The PPA-wrapped CA/CuZn can capture CO2 to form active intermediates. Through photo-induced charge transfer under visible light illumination, the CA/CuZn@PPA system achieves 100% selectivity for DMC production at room temperature and low CO2 pressure.
直接从阳光驱动的二氧化碳中生产增值化学品,为解决环境和经济挑战提供了一种可持续的方法。然而,二氧化碳固有的化学稳定性对实现高活性和选择性的二氧化碳转化提出了巨大的挑战。在此,我们开发了一种生物杂交半人工光合系统,该系统将碳酸酐酶(CA)和CuZn纳米酶光敏剂与树突聚合物(PPA)结合在一起,用于将二氧化碳可持续地转化为碳酸二甲酯(DMC)。ppa包裹的CA/CuZn可以捕获CO2形成活性中间体。通过可见光照明下的光诱导电荷转移,CA/CuZn@PPA体系在室温和低CO2压力下实现了100%的DMC生产选择性。
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引用次数: 0
Ferroelectric Transistors: from Materials Innovation to Intelligent Electronic Systems 铁电晶体管:从材料创新到智能电子系统
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-18 DOI: 10.1002/adma.202515480
Enlong Li, Wunan Wang, Yu Liu, Ruixue Wang, Chunlai Luo, Hongmiao Zhou, Shuo Chen, Shuxin Chen, Zhaoren Xie, Kaichen Zhu, Wenwu Li, Junhao Chu
The explosive growth of artificial intelligence, big data, and the Internet of Things is driving an unprecedented demand for computing power and energy efficiency. However, conventional von Neumann architectures are increasingly constrained by the physical and economic limits of transistor scaling in the post‐Moore era. Ferroelectric transistors (FeFETs) are far more than a novel memory technology and instead represent a revolutionary platform that seamlessly integrates nonvolatile storage, in‐memory computation, and multi‐modal sensing into a single, energy‐efficient device, overcoming the bottlenecks of traditional computing architectures. This review provides a comprehensive overview of ferroelectric materials, including perovskite oxides, hafnium‐based compounds, organics, and emerging 2D systems, emphasizing their polarization original mechanisms and structureproperty relationships. This study focuses on the device physics and engineering of three terminal FeFETs, with particular attention to the current issues, optimization strategies, and contrasting operation principles of ferroelectric dielectric and semiconductor‐based designs. Finally, the expanding applications of FeFETs in nonvolatile memory, neuromorphic computing, and artificial intelligence hardware from device to system integration is discussed, and an outlook toward scalable, low‐power, and multifunctional electronics driven by ferroelectric innovation is presented.
人工智能、大数据和物联网的爆炸式增长正在推动对计算能力和能源效率的前所未有的需求。然而,在后摩尔时代,传统的冯·诺伊曼架构越来越受到晶体管缩放的物理和经济限制。铁电晶体管(fefet)不仅仅是一种新颖的存储技术,而是一个革命性的平台,它将非易失性存储、内存计算和多模态传感无缝集成到一个单一的节能设备中,克服了传统计算架构的瓶颈。本文综述了铁电材料,包括钙钛矿氧化物、铪基化合物、有机物和新兴的二维系统,强调了它们的极化原始机制和结构性质关系。本研究的重点是三端场效应管的器件物理和工程,特别关注当前的问题,优化策略,以及基于铁电介质和半导体设计的对比工作原理。最后,讨论了fefet在非易失性存储器、神经形态计算和人工智能硬件从器件到系统集成方面的扩展应用,并展望了由铁电创新驱动的可扩展、低功耗和多功能电子产品的前景。
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引用次数: 0
Bulk Fabrication of Space‐Confined CsPbI 3 Nanocrystal Films Toward Efficient and Bright Deep‐Red LEDs 面向高效、明亮的深红色led的空间受限CsPbI - 3纳米晶体薄膜的批量制备
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-18 DOI: 10.1002/adma.202518255
Wenji Zhan, Haifei Wang, Jiahao Guo, Yugang Liang, Yanming Wang, Jixin Wu, Zhengzheng Dang, Ni Zhang, Jingjing Cao, Yingping Fan, Yu Zou, Bowei Li, Yao Wang, Yuetian Chen, Yanfeng Miao, Yixin Zhao
Deep‐red light‐emitting diodes (LEDs) with 690−710 nm emission show high significance in optical, agricultural, and biomedical applications. As primary candidates for deep‐red emitters, all‐inorganic CsPbI 3 films suffer from fused large grains with abundant trap states, leading to inferior performance of deep‐red perovskite LEDs (PeLEDs). Here we report CsPbI 3 nanocrystal films with strong space confinement and notable performance at ∼700 nm of deep‐red emission via bulk fabrication. The dual roles of diaza‐18‐crown‐6 dihydriodide additive as crystallization regulator and Lewis base ligand trigger more nucleation sites, retarded grain growth and passivated trap states, ensuring the crystallization of high‐quality space‐confined CsPbI 3 nanocrystal films. This approach establishes a record‐high external quantum efficiency (EQE) of 23.4% for deep‐red PeLEDs, and achieves a maximum luminance of 10152 cd m −2 . Low roll‐off is also demonstrated that EQE maintain over 20% under a high current density of 900 mA cm −2 , which is superior to state‐of‐the‐art deep‐red organic and quantum‐dot LEDs. The T 50 operating lifetime is estimated to be 234 h at an initial radiance of 6.3 W sr −1 m −2 . This work provides an effectual strategy to accelerate radiative recombination and enhance the performance of CsPbI 3 ‐based deep‐red PeLEDs.
发光波长为690 ~ 710 nm的深红色发光二极管(led)在光学、农业和生物医学领域具有重要的应用价值。作为深红色发光材料的主要候选材料,全无机CsPbI - 3薄膜存在熔融大晶粒和丰富的陷阱态,导致深红色钙钛矿led (PeLEDs)的性能较差。在这里,我们报道了CsPbI - 3纳米晶体薄膜具有很强的空间约束和显著的性能,在~ 700 nm的深红色发射。diaza - 18 - crown - 6二氢化物添加剂作为结晶调节剂和Lewis碱配体的双重作用引发了更多的成核位点,延缓了晶粒的生长和钝化了陷阱状态,确保了高质量的空间受限CsPbI - 3纳米晶体膜的结晶。该方法为深红色pled创造了创纪录的23.4%的外量子效率(EQE),并实现了10152 cd m−2的最大亮度。低滚降也证明了在900毫安厘米−2的高电流密度下,EQE保持在20%以上,这优于目前最先进的深红色有机和量子点led。t50的工作寿命估计为234小时,初始辐射强度为6.3 W sr−1 m−2。这项工作为加速辐射复合和提高基于CsPbI - 3的深红色pled的性能提供了一种有效的策略。
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引用次数: 0
Control of Covalent Bond Enables Efficient Magnetic Cooling 共价键的控制,使有效的磁冷却
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-18 DOI: 10.1002/adma.202514295
Xin Tang, Yoshio Miura, Noriki Terada, Enda Xiao, Shintaro Kobayashi, Allan Döring, Terumasa Tadano, Andres Martin‐Cid, Takuo Ohkochi, Shogo Kawaguchi, Yoshitaka Matsushita, Tadakatsu Ohkubo, Tetsuya Nakamura, Konstantin Skokov, Oliver Gutfleisch, Kazuhiro Hono, Hossein Sepehri‐Amin
Magnetic cooling, harnessing the temperature change in matter when exposed to a magnetic field, presents an energy‐efficient and climate‐friendly alternative to traditional vapor‐compression refrigeration systems, with a significantly lower global warming potential. The advancement of this technology would be accelerated if irreversible losses arising from hysteresis in magnetocaloric materials are minimized. Despite extensive efforts to manipulate crystal lattice constants at the unit‐cell level, mitigating hysteresis often compromises cooling performance. Herein, we address this persistent challenge by forming Sn(Ge) 3 −Sn(Ge) 3 bonds within the unit cell of the Gd 5 Ge 4 compound. This approach enables an energetically favorable phase transition, leading to the elimination of thermal hysteresis. Consequently, we achieve a synergistic improvement of two key magnetocaloric figures of merit: a larger magnetic entropy change and a twofold increase in the reversible adiabatic temperature change (from 3.8 to 8 K) in the Gd 5 Sn 2 Ge 2 compound. Such synergies can be extended over a wide temperature range of 40–160 K. This study demonstrates a paradigm shift in mastering hysteresis toward simultaneously achieving exceptional magnetocaloric metrics and opens up promising avenues for gas liquefaction applications in the longstanding pursuit of sustainable energy solutions.
磁冷却,利用物质在暴露于磁场时的温度变化,提供了传统蒸汽压缩制冷系统的节能和气候友好型替代方案,具有显着降低全球变暖的潜力。如果能将磁致热材料中由磁滞引起的不可逆损耗降至最低,将加速该技术的发展。尽管在单位晶胞水平上对晶格常数进行了大量的研究,但减少迟滞往往会影响冷却性能。在这里,我们通过在Gd 5 ge4化合物的胞内形成Sn(Ge) 3−Sn(Ge) 3键来解决这一持续的挑战。这种方法可以实现能量上有利的相变,从而消除热滞后。因此,我们实现了两个关键的磁热学指标的协同改进:更大的磁熵变化和Gd 5 Sn 2 ge2化合物的可逆绝热温度变化(从3.8 K到8 K)增加了两倍。这种协同效应可以在40-160 K的宽温度范围内扩展。这项研究展示了在控制滞后的同时实现卓越的磁热指标的范式转变,并为长期追求可持续能源解决方案的天然气液化应用开辟了有希望的途径。
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引用次数: 0
Pressure‐Adaptive Artificial Synapses with High Linearity for Intelligent Computing in Extreme Environments 用于极端环境下智能计算的高线性压力自适应人工突触
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-18 DOI: 10.1002/adma.202516053
Yang Wang, Chen‐Yang Zhang, Shun‐Xin Li, Guanjun Xiao, Bo Zou
The ongoing exploration of the physical world has intensified the demand for intelligent computing in extreme environments. However, intelligent devices operating under extreme high‐pressure conditions are limited by the pressure tolerance of the materials used for intelligent computing. A pressure‐adaptive artificial synapse (PAAS) using VO 2 (M 1 ) nanoparticles is developed, leveraging the increased lattice rigidity during the M 1 ‐to‐M 1 ’ phase transition (1 atm to 15.1 GPa), which causes the photoinduced insulator‐to‐metal transition to be Mott dominated. The PAAS demonstrated a stable operating current, a superior biomimetic plasticity (maximum paired‐pulse facilitation index from 109.6% to 155.4%), and an improved postsynaptic current linearity (Pearson's r from 0.64 to 0.97) from 1 atm to 15.1 GPa. Furthermore, an artificial neural network mapped by PAAS under high pressure achieved a validation accuracy of 95%–97% in handwritten digit recognition. The PAAS is also applied to a convolutional autoencoder for denoising reconstruction of color images.
对物理世界的不断探索加剧了对极端环境下智能计算的需求。然而,在极端高压条件下运行的智能设备受到用于智能计算的材料的耐压能力的限制。利用VO 2 (m1)纳米颗粒开发了一种压力自适应人工突触(PAAS),利用在m1 - to - m1 '相变(1 atm至15.1 GPa)期间增加的晶格刚度,导致光诱导绝缘体- to -金属转变为Mott主导。PAAS表现出稳定的工作电流,优越的仿生可塑性(最大配对脉冲促进指数从109.6%到155.4%),以及从1 atm到15.1 GPa改善的突触后电流线性(Pearson's r从0.64到0.97)。此外,高压下PAAS映射的人工神经网络在手写体数字识别中获得了95% ~ 97%的验证准确率。该方法还应用于卷积自编码器,用于彩色图像的去噪重建。
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引用次数: 0
Designing Synergistic Lewis Acid‐Base Pairs in Compressed Bismuth‐Copper Oxide for Selective CO 2 ‐to‐Formate Electrosynthesis 设计压缩铋-铜氧化物中协同Lewis酸碱对用于选择性CO 2 - to -甲酸盐电合成
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-18 DOI: 10.1002/adma.202519866
Yi Cheng, Lijuan Yang, Xiaoli Zhao, Lulu Li, Jian Yang, Tao Liu, Feng Li, Ming Huang
Electrocatalytic carbon dioxide reduction (CO 2 RR) to formate represents a sustainable pathway for carbon utilization, yet its industrial deployment remains hindered by insufficient current density and stability of the electrocatalysts. While lattice strain engineering can modulate catalytic performance by altering electronic structures, a major challenge is the lack of a clear mechanistic understanding connecting the induced strain to the activity enhancement. Herein, by precisely engineering lattice strain in an atomically integrated catalytic system, we establish a definitive intrinsic structure‐activity relationship, moving beyond conventional correlations with apparent properties. Combined experimental and theoretical investigations demonstrate that compressive strain effectively modulates the electronic structure of the Cu d‐orbital and the local electronic states of oxygen vacancies, thereby enhancing the cooperation within the Lewis acid–base pairs. This mechanism facilitates CO 2 adsorption and activation, stabilizes the key * HCOO intermediate, and significantly lowers the reaction energy barrier. Consequently, the catalyst exhibits high formate Faradaic efficiency (>95%) over a broad current density range (−100 to −700 mA cm −2 ), achieving 96.1% at −576.8 mA cm −2 . This research not only elucidates the synergistic Lewis acid‐base catalytic mechanism at the molecular level but also provides universal design principles for the sustainable electro‐synthesis of value‐added formate.
电催化二氧化碳还原(CO 2 RR)生成甲酸是碳利用的一种可持续途径,但其工业应用仍受到电催化剂电流密度和稳定性不足的阻碍。虽然晶格应变工程可以通过改变电子结构来调节催化性能,但主要的挑战是缺乏将诱导应变与活性增强联系起来的明确机制理解。在此,通过精确地设计原子集成催化系统中的晶格应变,我们建立了确定的内在结构-活性关系,超越了与表观性质的传统相关性。结合实验和理论研究表明,压缩应变有效地调节了Cu d轨道的电子结构和氧空位的局部电子态,从而增强了Lewis酸碱对内部的合作。该机制有利于CO 2的吸附和活化,稳定了关键* HCOO中间体,显著降低了反应能垒。因此,该催化剂在较宽的电流密度范围内(- 100至- 700 mA cm - 2)表现出较高的甲酸法拉第效率(>95%),在- 576.8 mA cm - 2时达到96.1%。本研究不仅在分子水平上阐明了Lewis酸碱协同催化机理,而且为可持续电合成增值甲酸酯提供了通用的设计原则。
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引用次数: 0
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Advanced Materials
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