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Integrating Machine Learning and DFT Descriptors for Screening Dual Metal‐Site Catalysts for CO 2 Reduction to C 2 Products 结合机器学习和DFT描述符筛选CO 2还原为c2产物的双金属位催化剂
IF 13.3 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-19 DOI: 10.1002/smll.202513368
Mukaddar Sk, Arupjyoti Pathak, Ranjit Thapa
The electrochemical reduction of CO 2 (CO 2 RR) offers a sustainable route to generate multi‐carbon products (C 2 ), but achieving high activity and selectivity remains a challenge. Dual metal‐site catalysts (DMSCs), composed of two adjacent metal sites, provide unique active centers that enable simultaneous CO adsorption, a key step for C─C coupling. Here, we systematically investigated 156 DMSCs supported on nitrogen‐doped carbon to identify promising candidates for CO 2 RR. Stability screening revealed that 8 DMSCs are unstable, while hydrogen adsorption calculations excluded 6 additional systems due to strong * H binding. Among the remaining catalysts, 33 DMSCs exhibit CO dimerization energies (∆G *CO dimer‐2*CO ) below 0.75 eV, indicating favorable activity toward C 2 products. To explain these trends, we performed a linear correlation analysis of CO dimerization energy against 71 electronic parameters, which revealed that the occupancy of the dz 2 ↓ orbital (denoted O‐dz 2 ↓) exhibits the highest correlation (R 2 = 0.69). This suggested that combinations of electronic parameters could further improve the correlation and accurately predict CO 2 RR toward C 2 products. To achieve this, multiple machine learning models were trained, with the random forest regressor (RFR) achieving superior performance (R 2 = 0.98 for training and 0.96 for testing), demonstrating its suitability for predicting CO dimerization energy. Furthermore, the overpotential for C 2 production of the 33 DMSCs was correlated with electronic descriptors, revealing that O‐dz 2 ↓ exhibited the highest correlation (R 2 = 0.87), attributable to the substantial population of dz 2 ↓ states near the Fermi level (E F ), thereby underscoring its significance as a key descriptor. Overall, we emphasize the importance of using a multi‐descriptor predictive model to accurately estimate CO dimerization energies, and we identify key electronic parameters of DMSCs that can predict the overpotential for C 2 products. These insights offer a valuable framework for the rapid screening of low‐cost materials with high selectivity toward C 2 products.
电化学还原co2 (co2 RR)为生成多碳产物(co2)提供了一条可持续的途径,但实现高活性和选择性仍然是一个挑战。双金属位催化剂(DMSCs)由两个相邻的金属位组成,提供独特的活性中心,可以同时吸附CO,这是C─C偶联的关键步骤。在这里,我们系统地研究了156个氮掺杂碳负载的DMSCs,以确定有希望的CO 2 RR候选材料。稳定性筛选显示8个DMSCs是不稳定的,而氢吸附计算排除了6个由于强* H结合的附加体系。在其余催化剂中,33种DMSCs的CO二聚化能(∆G *CO二聚体‐2*CO)低于0.75 eV,表明其对c2产物具有良好的活性。为了解释这些趋势,我们对CO二聚化能与71个电子参数进行了线性相关分析,结果表明,dz 2↓轨道(表示为O‐dz 2↓)的占据率具有最高的相关性(r2 = 0.69)。这表明电子参数的组合可以进一步提高相关性,准确预测co2对co2产物的RR。为了实现这一目标,对多个机器学习模型进行了训练,随机森林回归器(RFR)取得了优异的性能(训练r2 = 0.98,测试r2 = 0.96),证明了其预测CO二聚化能的适用性。此外,33个DMSCs产生c2的过电位与电子描述子相关,表明O‐dz 2↓表现出最高的相关性(r2 = 0.87),这归因于大量dz 2↓状态接近费米能级(E F),从而强调了其作为关键描述子的重要性。总之,我们强调了使用多描述子预测模型来准确估计CO二聚化能的重要性,并确定了DMSCs的关键电子参数,这些参数可以预测二氧化碳产物的过电位。这些见解为快速筛选具有高选择性的低成本材料提供了有价值的框架。
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引用次数: 0
Continuous Phase Transition Enables Piezoelectric Thermal Stability in KNN-Based Multilayer Textured Ceramics 连续相变使knn基多层织构陶瓷具有压电热稳定性
IF 13.3 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-19 DOI: 10.1002/smll.73175
Caixia Zhu, Huirong Yang, Jin Qian, Luomeng Tang, Peng Li, Xiaoqian Wu, Cheng Shi, Guohui Li, Guanglong Ge, Bo Shen, Jiwei Zhai
Overcoming the trade-off between multiphase coexistence and phase transformation in piezoelectrics remains a critical challenge for achieving high and stable piezoelectric performance over a broad temperature range. Here, we resolve this long-standing dilemma by constructing a continuous phase transition through multilayer ceramic texture engineering. Specifically, two types of (K,Na)NbO3-based piezoelectric ceramics with distinct polymorphic phase boundary (PPB) features are physically composed. The composite ceramics exhibit hierarchic phase and domain structures, particularly a continuous phase transition, enabling outstanding piezoelectric performance and thermal stability across a wide temperature range. As a result, the multilayer composite ceramics prepared in this work demonstrate excellent room-temperature piezoelectric properties, with a piezoelectric coefficient (d33) ∼ 420 pC N−1 and an inverse piezoelectric coefficient (d33*) ∼ 600 pm V−1. More importantly, within the temperature range of 25°C–100°C, the variation in d33 and d33* values is merely 2%. This work establishes a continuous phase transition-driven paradigm for enhancing piezoelectric thermal stability, demonstrating universal potential to decouple the constraints imposed by multiphase coexistence and phase transformation in next-generation piezoelectric materials.
克服压电材料中多相共存和相变之间的权衡仍然是在宽温度范围内实现高稳定压电性能的关键挑战。在这里,我们通过多层陶瓷织构工程构建连续相变来解决这个长期存在的难题。具体而言,物理合成了两种具有不同多晶相边界(PPB)特征的(K,Na) nbo3基压电陶瓷。复合陶瓷具有分层相和畴结构,特别是连续相变,在很宽的温度范围内具有出色的压电性能和热稳定性。因此,在这项工作中制备的多层复合陶瓷表现出优异的室温压电性能,压电系数(d33) ~ 420 pC N−1和逆压电系数(d33*) ~ 600 pm V−1。更重要的是,在25℃- 100℃的温度范围内,d33和d33*值的变化仅为2%。这项工作为增强压电热稳定性建立了一个连续相变驱动的范例,展示了在下一代压电材料中解耦多相共存和相变所施加的约束的普遍潜力。
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引用次数: 0
Chemical Functionalization of 2D Materials 二维材料的化学功能化
IF 13.3 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-19 DOI: 10.1002/smll.73110
Xiaoyan Zhang, Nikos Tagmatarchis, Zhong‐Shuai Wu, Nazario Martín
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引用次数: 0
Measures for Mitigating Ionic Concentration Polarization During Osmotic Energy Conversion 缓解渗透能转换过程中离子浓度极化的措施
IF 13.3 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-19 DOI: 10.1002/smll.202514089
Boyou Wang, Wenxia Xu, Man Zhang, Jing Pan, Cong Wang, Qitao Zhou, Fan Xia
The recovery of osmotic energy through nanochannel membrane materials offers advantages such as zero CO 2 emissions and high resistance to weather and other external factors. Therefore, it holds great promise as a potential renewable energy source in the context of carbon neutrality. However, there are still numerous challenges before the relevant technology can be practically applied. Among them, large‐area and reproducible fabrication of membrane materials and overcoming the performance degradation caused by the ionic concentration polarization (ICP) effect at the interface between the membrane material and salt solution during system operation are key research focuses. Existing reviews primarily focus on the latest advancements in the field of material preparation. This review, however, starts from the approaches to mitigate the ICP effect. It categorizes the existing methods for ICP mitigating into physical means and material design strategies. Furthermore, it summarizes the matching patterns among nanopore size, charge characteristics during material design, and concentration gradients during operation. We believe that this review can offer valuable guidance to relevant researchers and facilitate the progression of osmotic energy conversion technology toward practical applications.
通过纳米通道膜材料回收渗透能具有零二氧化碳排放和对天气等外界因素的高抗性等优点。因此,在碳中和的背景下,它作为一种潜在的可再生能源具有很大的前景。然而,相关技术在实际应用前仍面临诸多挑战。其中,膜材料的大面积和可重复性制备以及克服系统运行过程中膜材料与盐溶液界面离子浓度极化(ICP)效应导致的性能下降是研究的重点。现有的评论主要集中在材料制备领域的最新进展。然而,本综述从减轻ICP影响的方法开始。它将现有的ICP缓解方法分为物理手段和材料设计策略。此外,总结了纳米孔尺寸、材料设计时的电荷特性和运行时的浓度梯度之间的匹配规律。我们相信本文的综述可以为相关研究人员提供有价值的指导,促进渗透能转换技术向实际应用的发展。
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引用次数: 0
Ferrate‐Crosslinked Polybenzimidazole‐Derived Carbon Molecular Sieve Membranes for Enhanced H 2 /CO 2 Separation 高铁酸盐-交联多苯并咪唑-衍生碳分子筛膜增强h2 / co2分离
IF 13.3 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-19 DOI: 10.1002/smll.202514458
Jianyu Guan, Zeyuan Gao, Lu Bai, Fangxu Fan, Tianyou Li, Hongjin Li, Fake Sun, Yijun Liu, Gaohong He, Canghai Ma
The fabrication of carbon molecular sieve (CMS) membranes via pyrolysis of crosslinked polymeric precursors has proven highly effective for hydrogen purification, offering unparalleled molecular sieving capabilities. However, conventional approaches typically require pyrolysis temperatures above 800°C to achieve precise H 2 /CO 2 discrimination, posing substantial challenges to industrial scalability and cost‐effectiveness. In this study, an oxidative crosslinking strategy employing potassium ferrate (K 2 FeO 4 ) is introduced to synergistically integrate proton transfer, hydrogen bonding, and covalent crosslinking, enabling the formation of a highly selective CMS membrane at a significantly reduced pyrolysis temperature of 650°C. The optimized FeO 4 2− ‐PBI‐12 h CMS@650°C membrane demonstrated remarkable gas transport performance, elevating H 2 permeability from 3.4 Barrer to 66 Barrer and H 2 /CO 2 selectivity from 14.4 to 75.3 under industrially relevant conditions (11 atm, 100°C), compared to its polymer precursor. These metrics transcend the 2008 Robeson upper bound and rank among the highest reported for H 2 /CO 2 separation. This work establishes an energy‐efficient pathway for producing high‐performance CMS membranes, offering a promising pathway toward more economically viable hydrogen purification.
通过热解交联聚合物前体制备碳分子筛(CMS)膜已被证明对氢净化非常有效,具有无与伦比的分子筛分能力。然而,传统方法通常需要800°C以上的热解温度才能实现精确的h2 /CO 2区分,这对工业可扩展性和成本效益构成了重大挑战。在本研究中,采用高铁酸钾(k2feo4)氧化交联策略,协同整合质子转移、氢键和共价交联,在显著降低的650℃热解温度下形成了高选择性的CMS膜。优化后的feo4 2−‐PBI‐12 h CMS@650°C膜具有显著的气体输送性能,在工业相关条件下(11 atm, 100°C),与聚合物前驱体相比,h2渗透率从3.4 Barrer提高到66 Barrer, h2 /CO 2选择性从14.4提高到75.3。这些指标超越了2008年罗布森上限,并跻身于h2 /CO 2分离的最高报告之列。这项工作为生产高性能的CMS膜建立了一个节能的途径,为更经济可行的氢净化提供了一条有希望的途径。
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引用次数: 0
Solution‐Processed Ambipolar Thin Film Transistors‐Based Inverters for Circuit Applications 基于电路应用的溶液处理双极性薄膜晶体管的逆变器
IF 13.3 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-19 DOI: 10.1002/smll.202514974
Min Ki Kim, Swarup Biswas, Yongju Lee, Dong Hyun Nam, Sein Chung, Byeong Jin Kim, Kilwon Cho, Hyeok Kim
Fully solution‐processed ambipolar organic thin‐film transistors (OTFTs) are attractive for flexible, large‐area, and low‐cost electronics; however, their circuit‐level implementation has remained limited by mobility imbalance, trap‐induced instability, and complex fabrication. This study employs bulk‐heterojunction blends of the benchmark n‐type polymer N2200 and the high‐mobility donor polymer DPP‐DTT as a single active semiconductor platform for ambipolar OTFTs and complementary‐like logic. Systematically tuning the DPP‐DTT:N2200 composition enables balanced electron and hole transport, high on/off current ratios of ∼10 5 , and threshold voltages suitable for rail‐to‐rail operation, with the 5:95 blend providing the optimal compromise between mobility symmetry and operational stability. The optimized ambipolar behavior is attributed to a semi‐intermixed morphology with bi‐continuous percolation pathways and controlled crystallinity, as confirmed by correlated optical, energetic, and structural characterizations. Using a simple top‐gate device architecture and geometry‐scaled channel widths, all‐polymer ambipolar inverters exhibited sharp switching voltage‐transfer characteristics and high small‐signal gains of up to 19 at an optimized width ratio of 2:1. This study establishes a manufacturing‐compatible strategy for co‐engineering blend composition, microstructure, and device geometry, enabling scalable printed organic logic using a single bulk heterojunction semiconductor rather than separate p‐type and n‐type materials.
完全溶液处理的双极性有机薄膜晶体管(OTFTs)对于柔性、大面积和低成本电子产品具有吸引力;然而,它们的电路级实现仍然受到迁移率不平衡,陷阱诱导的不稳定性和复杂的制造的限制。本研究采用基准n型聚合物N2200和高迁移率供体聚合物DPP - DTT的体异质结共混物作为双极性otft和互补类逻辑的单一有源半导体平台。系统地调整DPP - DTT:N2200组成可实现平衡的电子和空穴输运,高开/关电流比约10.5,以及适合轨对轨运行的阈值电压,5:95混合提供了迁移率对称性和运行稳定性之间的最佳折衷。优化的双极性行为归因于具有双连续渗透途径和可控结晶度的半混合形态,相关光学,能量和结构表征证实了这一点。采用简单的顶栅极器件结构和几何缩放的通道宽度,全聚合物双极性逆变器在优化宽度比为2:1的情况下,具有锐利的开关电压转移特性和高达19的高小信号增益。本研究建立了一种制造兼容策略,用于共同工程混合成分,微观结构和器件几何形状,使可扩展的印刷有机逻辑使用单个异质结半导体,而不是单独的p型和n型材料。
{"title":"Solution‐Processed Ambipolar Thin Film Transistors‐Based Inverters for Circuit Applications","authors":"Min Ki Kim, Swarup Biswas, Yongju Lee, Dong Hyun Nam, Sein Chung, Byeong Jin Kim, Kilwon Cho, Hyeok Kim","doi":"10.1002/smll.202514974","DOIUrl":"https://doi.org/10.1002/smll.202514974","url":null,"abstract":"Fully solution‐processed ambipolar organic thin‐film transistors (OTFTs) are attractive for flexible, large‐area, and low‐cost electronics; however, their circuit‐level implementation has remained limited by mobility imbalance, trap‐induced instability, and complex fabrication. This study employs bulk‐heterojunction blends of the benchmark n‐type polymer N2200 and the high‐mobility donor polymer DPP‐DTT as a single active semiconductor platform for ambipolar OTFTs and complementary‐like logic. Systematically tuning the DPP‐DTT:N2200 composition enables balanced electron and hole transport, high on/off current ratios of ∼10 <jats:sup>5</jats:sup> , and threshold voltages suitable for rail‐to‐rail operation, with the 5:95 blend providing the optimal compromise between mobility symmetry and operational stability. The optimized ambipolar behavior is attributed to a semi‐intermixed morphology with bi‐continuous percolation pathways and controlled crystallinity, as confirmed by correlated optical, energetic, and structural characterizations. Using a simple top‐gate device architecture and geometry‐scaled channel widths, all‐polymer ambipolar inverters exhibited sharp switching voltage‐transfer characteristics and high small‐signal gains of up to 19 at an optimized width ratio of 2:1. This study establishes a manufacturing‐compatible strategy for co‐engineering blend composition, microstructure, and device geometry, enabling scalable printed organic logic using a single bulk heterojunction semiconductor rather than separate p‐type and n‐type materials.","PeriodicalId":228,"journal":{"name":"Small","volume":"17 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2026-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147478440","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}
引用次数: 0
Switching the Channel Screening Effect of Metal–Organic Frameworks to Control the Selectivity of Furfural Hydrogenation 切换金属-有机骨架的通道筛选效应以控制糠醛加氢的选择性
IF 13.3 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-19 DOI: 10.1002/smll.202514192
Yuanxia Zhao, Yan Liang, Jin Hu, Zhiwei Chen, Hongru Zhou, Bo Jiang, Qianshuo Wang, Min Wang
The adsorption configuration regulation of molecules on the metal site is crucial in the targeted conversion of specific functional groups. Herein, we propose a strategy to adjust the adsorption configuration of substrate molecules by switching the channel screening effect of MOF, thereby achieving the targeted regulation of the selective hydrogenation pathway of furfural. Specifically, two Pd‐containing MOF with different Pd locations were fabricated, in which Pd nanoclusters are confined within the MOF cavities and Pd nanoparticles grow on the MOF external surface. Since furfural must pass through the MOF to contact with the Pd cluster, thus forcing furfural to present a linear adsorption configuration and selectively activates the C═O bonds. In contrast, surface Pd particles shield the channel effect, allowing furfural to adopt a thermodynamically stable planar adsorption mode, resulting in hydrogenation of both C═O and C═C bonds. This work provides insights into the adjustment of substrate adsorption configurations, and the proposed channel screening adsorption mechanism also provides ideas for designing catalysts with complex molecular orientation conversion.
分子在金属位点上的吸附构型调节对于特定官能团的靶向转化至关重要。本文提出一种策略,通过切换MOF的通道筛选效应来调整底物分子的吸附构型,从而实现对糠醛选择性加氢途径的靶向调控。具体来说,制备了两种具有不同Pd位置的含Pd MOF,其中Pd纳米团簇被限制在MOF腔内,Pd纳米颗粒生长在MOF外表面。由于糠醛必须通过MOF与Pd簇接触,从而迫使糠醛呈现线性吸附构型并选择性地激活C = O键。相反,表面Pd粒子屏蔽了通道效应,允许糠醛采用一种热力学稳定的平面吸附模式,导致C = O和C = C键的加氢。这项工作为调节底物吸附构型提供了新的思路,所提出的通道筛选吸附机制也为设计具有复杂分子取向转换的催化剂提供了思路。
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引用次数: 0
Fluorescent Supramolecular Gels Based on D‐Sorbitol Derivatives 基于D -山梨醇衍生物的荧光超分子凝胶
IF 13.3 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-19 DOI: 10.1002/smll.202511765
Emmanuel Odella, Miryam Criado‐Gonzalez, Rodrigo A. Ponzio, David Mecerreyes, Matías L. Picchio, Daniele Mantione
Supramolecular gels formed by low‐molecular‐weight gelators (LMWGs) are valuable soft materials due to their remarkable versatility and wide range of applications. Developing ambidextrous LMWGs that self‐assemble in diverse solvents remains challenging, as such versatility requires precise molecular engineering to ensure robust structuring across varying polarity and hydrogen‐bonding environments. Here, we present a family of sugar‐based molecules functionalized with naphthyl (DNapS), benzothiadiazole (DBTDS), and coumarin (MCumS) moieties, synthesized by a green, scalable method, which serve as fluorescent LMWGs. Their gelation abilities are evaluated in water, organic solvents of different polarities, and deep eutectic solvents (DES). Among them, MCumS forms gels in water, short‐chain alcohols, and terpene‐based hydrophobic DES, highlighting its potential as a rare example of an LMWG capable of gelation across chemically diverse environments. Morphological analysis of MCumS gels reveals fibrous network formation in water and distinct, solvent‐dependent architectures in eutectogels. Interestingly, supramolecular gels based on this LMWG and zwitterionic DES show superior viscoelastic behavior and injectability. These findings not only expand the library of fluorescent LMWGs but also contribute to the fundamental understanding of structure‐property relationships in versatile supramolecular gel systems.
由低分子量凝胶(lmwg)形成的超分子凝胶由于其卓越的通用性和广泛的应用范围而成为有价值的软材料。开发在不同溶剂中自组装的双灵巧lmwg仍然具有挑战性,因为这种多功能性需要精确的分子工程来确保在不同极性和氢键环境下的坚固结构。在这里,我们提出了一个以萘基(DNapS),苯并噻唑(DBTDS)和香豆素(MCumS)为功能化的糖基分子家族,通过绿色,可扩展的方法合成,可作为荧光LMWGs。在水、不同极性的有机溶剂和深共晶溶剂(DES)中评价了它们的凝胶能力。其中,mcum在水、短链醇和萜烯基疏水性DES中形成凝胶,突出了其作为一种罕见的LMWG能够在不同化学环境中形成凝胶的潜力。形态学分析揭示了MCumS凝胶在水中形成的纤维网络和共聚凝胶中独特的、依赖溶剂的结构。有趣的是,基于这种低分子聚合物和两性离子DES的超分子凝胶表现出优异的粘弹性和注射性。这些发现不仅扩大了荧光小分子蛋白的文库,而且有助于从根本上理解多用途超分子凝胶体系的结构-性质关系。
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引用次数: 0
A Review of Fiber‐Shape Rolled Dielectric Elastomer Actuators: A Pivotal Pathway in Advancing Bionic Actuation 纤维型卷绕介质弹性体致动器:推进仿生致动的关键途径
IF 13.3 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-19 DOI: 10.1002/smll.202513229
Ziqi Zhang, Wei Yu, Jianghua Zhao, Yingjie Li, Chuizhou Meng, Shijie Guo
Dielectric Elastomer Actuators (DEAs) demonstrate tremendous application potential in the field of flexible actuation due to their excellent actuation performance. Rolled Dielectric Elastomer Actuators (RDEAs) in the form of fibers, featuring a bionic actuation form that more closely mimics the biological motion, enable a more natural actuation mode. This review systematically elaborates on the typical physical configurations and core actuation mechanisms of RDEAs, and sorts out the key geometric parameters and output performance characteristics of RDEAs in existing research. Through practical examples, it showcases the application achievements of robot systems based on RDEAs in multiple fields, covering areas such as crawling robots, bionic robots, end‐effectors, and interactive devices. Finally, the paper conducts an in‐depth analysis of the key challenges currently faced by RDEAs, including the improvement of output performance, the optimization of preparation and integration technologies, and the adaptation to human‐robot collaboration scenarios. Based on this analysis, it proposes the key future development directions.
介电弹性体作动器以其优异的作动性能在柔性作动领域显示出巨大的应用潜力。纤维形式的滚动介电弹性体致动器(rdea)具有更接近模拟生物运动的仿生致动形式,实现更自然的致动模式。本文系统阐述了rdea的典型物理构型和核心驱动机构,并对现有研究中rdea的关键几何参数和输出性能特征进行了梳理。通过实例展示了基于rdea的机器人系统在爬行机器人、仿生机器人、末端执行器和交互设备等多个领域的应用成果。最后,本文深入分析了rdea目前面临的主要挑战,包括输出性能的提高、制备和集成技术的优化以及对人机协作场景的适应。在此基础上,提出了未来的重点发展方向。
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引用次数: 0
Spatially Extended Interfacial Optimization via Holey‐Defect Architectures for Hydrogen Evolution Reaction 基于空穴缺陷结构的空间扩展界面析氢反应优化研究
IF 13.3 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-19 DOI: 10.1002/smll.202600032
Chengang Pei, Jaekyum Kim, Dong Zhang, Won Tae Hong, Jong Hun Kim, Xu Yu, Jongwook Park, Chan‐Hwa Chung, Byung‐Hyun Kim, Ho Seok Park, Jung Kyu Kim
Supported metal catalysts provide a highly effective route to achieving high‐performance water electrolysis with minimized noble‐metal usage, where precise engineering of the catalyst–support interface is crucial to unlock outstanding activity. Herein, we present a strategy to engineer catalyst interfaces by introducing holey defects for highly efficient hydrogen evolution reaction. The holey defects promote uniform dispersion of Pt nanoclusters across the basal planes, rather than the edge‐confined deposition observed on pristine ReS 2 (Pt‐hReS 2 ). Beyond geometric templating, the holey architecture enriches local electron density, stabilizes Pt–S interfacial bridge motifs, tunes the adsorption energy toward near‐thermoneutral values, and lowers the water‐dissociation barrier. These synergistic effects shift the catalytic regime, moving the rate‐determining step from dissociation to desorption, which is revealed in characterizations and density functional theory calculations. Consequently, Pt‐hReS 2 requires only 12 mV overpotential at 10 mA cm −2 , which outperforms commercial Pt/C while using substantially less Pt. In an anion‐exchange membrane water electrolyzer, a Pt‐hReS 2 cathode achieves 1.77 V at 0.5 A cm −2 and 1.99 V at 1.0 A cm −2 , with stable operation exceeding 100 h. This work establishes holey‐defect engineering as a powerful approach for interface optimization, opening new avenues for rational catalyst design in energy‐conversion applications.
负载型金属催化剂为实现高性能水电解提供了一种高效途径,同时最大限度地减少贵金属的使用,而催化剂-载体界面的精确设计对于释放出色的活性至关重要。在此,我们提出了一种通过引入孔洞缺陷来设计催化剂界面的策略,以实现高效的析氢反应。孔洞缺陷促进Pt纳米团簇在基面上均匀分散,而不是在原始ReS 2 (Pt - hReS 2)上观察到的边缘受限沉积。除了几何模板外,多孔结构丰富了局部电子密度,稳定了Pt-S界面桥基,将吸附能调整到接近热中性值,并降低了水解离势垒。这些协同效应改变了催化机制,将速率决定步骤从解离移动到解吸,这在表征和密度泛函理论计算中得到了揭示。因此,工党还是人力资源2只需要12 mV过电压马10厘米−2,优于商业Pt / C在使用Pt少得多。在一个阴离子交换膜水电解槽,一个Pt人力资源2阴极达到1.77 V 0.5厘米−2和1.99 V 1.0厘米−2,与稳定运行超过100 h。这项工作建立多洞的检测缺陷工程作为一个强大的方法界面优化,合理的催化剂设计开辟新途径的能源转换的应用程序。
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