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Surfactant-Mediated Porous MOF-5 for High-Performance Triboelectric Nanogenerators 高性能摩擦电纳米发电机用表面活性剂介导的多孔MOF-5
IF 6.7 3区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-12 DOI: 10.1039/d5nr04950d
Amaal Romih, Carmen Abuoudah, Andreas Schiffer, Vincent Chan, Lianxi Zheng
In this study, high-performance triboelectric nanogenerators (TENGs) are developed by incorporating porous metal-organic frameworks (MOFs) into the device structure. The highly porous MOF-5 was prepared via a surfactant-mediated process, and was employed as the positive triboelectric layer of the TENG device. Several characterization techniques including scanning electron microscopy, Fourier transform infrared spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy, and the Brunauer–Emmett–Teller method were employed to investigate the structural and morphological properties and the influences of the surfactant. The surfactant-mediated MOF-5 exhibits well-defined crystalline structures, enhanced porosity, and a high specific surface area of ~601.5 m2/g. Consequently, the TENG device derived from such a porous material achieved a short circuit current (ISC) of 100 µA, an open circuit voltage (VOC) of 250 V, and a maximum power output (Pmax) of 6250 µW. This TENG device also demonstrated effective sensing function with outstanding sensitivity when used as a flexible pressure sensor, offering promising potential for self-powered sensing in applications such as human motion detection, personal healthcare monitoring, and electronic skins.
在本研究中,通过将多孔金属有机框架(mof)结合到器件结构中,开发了高性能摩擦电纳米发电机(TENGs)。通过表面活性剂介导法制备了高孔MOF-5,并将其作为TENG器件的正摩擦电层。利用扫描电镜、傅里叶变换红外光谱、x射线衍射、x射线光电子能谱和brunauer - emmet - teller方法等表征技术研究了表面活性剂的结构和形态特性以及对表面活性剂的影响。表面活性剂介导的MOF-5晶体结构清晰,孔隙率增强,比表面积高达~601.5 m2/g。因此,由这种多孔材料制成的TENG器件的短路电流(ISC)为100µa,开路电压(VOC)为250 V,最大输出功率(Pmax)为6250µW。当用作柔性压力传感器时,该TENG设备还展示了有效的传感功能,具有出色的灵敏度,在人体运动检测、个人医疗监测和电子皮肤等应用中具有自供电传感的潜力。
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引用次数: 0
Noble-metal-free recyclable electronic nanoinks for wireless wearable sensors. 用于无线可穿戴传感器的无贵金属可回收电子纳米墨水。
IF 5.1 3区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-12 DOI: 10.1039/d5nr04828a
Naimul Arefin, Kwame Afrifa Obeng Ofori, Curtis Borden, Nishat Paul, Thomas Jones, Nicolas Constantinides, Kai Wu, Minxiang Zeng

Inappropriate disposal of electronic waste (e-waste) can pollute ecosystems and deplete mineral resources, highlighting the urgency to develop sustainable and recyclable electronics. While various metal nanoparticles have been tested in literature regarding built-in recyclability for electronics, it remains unclear on how recycling processes affect their properties, since oxidation and contamination of recycled nanomaterials may compromise the functional and reliable performance of remanufactured devices. This study aims to fill this knowledge gap by systematically investigating the behaviors of metal particles at different remanufacturing stages and by developing an effective, printing-enabled, remanufacturing route using fully recyclable, noble-metal-free, conductive inks. Recyclability of the printed conductors is investigated in terms of electrical properties across multiple reuse cycles, achieving ∼90% recovery of electrical conductivity after 3 reuse cycles (at least 1 order of magnitude higher than the regular "mill-to-print" approach). As proof of concept, a wireless strain-sensing platform is designed for real-time monitoring of small strains generated by the human body, highlighting potential for wearable human-machine interface applications.

电子废物处置不当会污染生态系统并耗尽矿产资源,这凸显了开发可持续和可回收电子产品的紧迫性。虽然各种金属纳米颗粒已经在文献中进行了关于电子产品内置可回收性的测试,但回收过程如何影响其性能仍不清楚,因为再生纳米材料的氧化和污染可能会损害再制造设备的功能和可靠性能。本研究旨在通过系统地研究金属颗粒在不同再制造阶段的行为,并通过开发一种有效的、可打印的、使用完全可回收的、无贵金属的导电油墨的再制造路线来填补这一知识空白。根据多个重复使用周期的电性能,研究了印刷导体的可回收性,在3个重复使用周期后实现了~ 90%的电导率恢复(至少比常规的“从工厂到印刷”方法高1个数量级)。作为概念验证,设计了一种无线应变传感平台,用于实时监测人体产生的小应变,突出了可穿戴人机界面应用的潜力。
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引用次数: 0
Large-scale synthesis of zinc oxide-supported indium single-atom catalysts for efficient electrocatalytic CO2 reduction reaction. 大规模合成氧化锌负载铟单原子高效电催化CO2还原反应催化剂。
IF 5.1 3区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-12 DOI: 10.1039/d5nr04922a
Wenzhao Duan, Tianrui Lu, Qiuyue Xiang, Heng Chen, Xi Yu, Ge Meng, Zheng-Jun Wang, Hailong Zhang, Lilong Zhang, Huile Jin, Shun Wang, Jing-Jing Lv

Electrocatalytic CO2 reduction reaction (eCO2RR) represents a pivotal technology for converting CO2 into fuels and chemicals using renewable electricity, with formic acid being a highly valued product. This work reports the large-scale synthesis of zinc oxide-supported indium single-atom catalysts (ZnO@In-SACs) by a modified micro-impinging stream synthesis method and investigates its performance for eCO2RR. We demonstrate that the reconstructed ZnO nanosheet support optimally tunes the electronic configuration of In single-atom sites during electrolysis, leading to a remarkable enhancement in catalytic activity. Optimized ZnO@In-SACs exhibit exceptional selectivity toward formate and outstanding stability in an alkaline flow electrolyzer for eCO2RR, with a high faradaic efficiency of 85% and a decent durability of 40 hours at a current density of 100 mA cm-2, surpassing most reported single-atom catalysts. This work provides an efficient large-scale strategy for fabricating catalysts to be utilized in different electrochemical reactions.

电催化二氧化碳还原反应(eCO2RR)是利用可再生电力将二氧化碳转化为燃料和化学品的关键技术,甲酸是一种非常有价值的产品。本文报道了采用改进的微碰撞流合成方法大规模合成氧化锌负载的铟单原子催化剂(ZnO@In-SACs),并研究了其在eCO2RR上的性能。我们证明了重建的ZnO纳米片支持在电解过程中优化了In单原子位的电子构型,从而显著提高了催化活性。优化后的ZnO@In-SACs对甲酸盐表现出优异的选择性,eCO2RR在碱性流动电解槽中表现出优异的稳定性,法拉第效率高达85%,在100 mA cm-2的电流密度下具有40小时的耐久性,超过了大多数报道的单原子催化剂。这项工作为大规模制备用于不同电化学反应的催化剂提供了一种有效的策略。
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引用次数: 0
Catalytic Applications of Carbon Nanotubes in Energy and Environmental Remediation: Multifunctional Roles and Design Strategies 碳纳米管在能源和环境修复中的催化应用:多功能作用和设计策略
IF 6.7 3区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-12 DOI: 10.1039/d5nr05306d
Placidus B. Amama, Samson A Adeoye
Carbon nanotubes (CNTs) have emerged as highly multifunctional nanomaterials capable of addressing pressing challenges in energy conversion and environmental remediation. Their catalytic role has evolved from passive conductive supports to active, tunable catalytic platforms enabled by good control over nanotube structure, defect chemistry, and electronic properties. Across energy and environmental applications, catalytic performance is governed by unified nanoscale principles, including electronic structure modulation through heteroatom doping, nano-confinement-induced stabilization of active species, and strong interfacial interactions that facilitate efficient charge transfer and dynamic redox processes. Recent advances have demonstrated that CNTs are efficient and durable electrocatalysts and thermally stable supports for hydrocarbon reforming, in which confinement suppresses carbon accumulation. In environmental remediation, CNTs serve as efficient electron acceptors in hybrid photocatalysts, thereby suppressing electron-hole recombination and promoting the degradation of persistent pollutants and inactivation of pathogens. This review critically examines the advances in CNT-based catalysts and the emerging catalytic role of CNTs in these applications. It clarifies the structure-property-function relationships that define CNT catalytic behavior and identifies key challenges and future directions necessary to translate CNT-based catalysts into sustainable energy and environmental technologies.
碳纳米管作为一种高度多功能的纳米材料,能够解决能源转换和环境修复方面的紧迫挑战。通过对纳米管结构、缺陷化学和电子特性的良好控制,它们的催化作用已经从被动的导电支撑演变为主动的、可调的催化平台。在能源和环境应用中,催化性能由统一的纳米级原理控制,包括通过杂原子掺杂调制电子结构,纳米束缚诱导活性物质稳定,以及促进有效电荷转移和动态氧化还原过程的强界面相互作用。最近的研究表明,碳纳米管是高效、耐用的电催化剂和热稳定的烃类重整载体,其中约束抑制了碳的积累。在环境修复中,碳纳米管在杂化光催化剂中作为高效的电子受体,从而抑制电子-空穴复合,促进持久性污染物的降解和病原体的失活。本文综述了碳纳米管催化剂的研究进展以及碳纳米管在这些应用中的催化作用。它阐明了定义碳纳米管催化行为的结构-性能-功能关系,并确定了将碳纳米管催化剂转化为可持续能源和环境技术所需的关键挑战和未来方向。
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引用次数: 0
Rational design of self-assembled monolayer composition for efficient perovskite/Si tandem solar cells. 高效钙钛矿/硅串联太阳能电池自组装单层结构的合理设计。
IF 6.7 3区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-12 DOI: 10.1039/d5nr04517g
Min Sup Kim,So Jeong Park,Geon Pyo Hong,Jin Young Kim
Efficient charge extraction at the interface is essential for achieving high-performance perovskite/Si tandem solar cells. Here, we demonstrate a highly efficient wide-bandgap perovskite single-junction solar cell using a co-adsorption strategy of commercial self-assembled monolayers (SAMs), specifically MeO-4PACz and Br-4PACz. Mixed-SAMs, with electron-withdrawing Br functional groups, induce a larger dipole moment and a downward shift in the HOMO level, thereby promoting favorable energy level alignment with a wide-bandgap perovskite. It further passivates interfacial defects, suppressing non-radiative recombination. This combined effect enables effective hole transport at the SAM/perovskite interface, enhancing the open-circuit voltage and fill factor of the perovskite device. Accordingly, the optimal single-junction perovskite solar cell exhibits an efficiency of 19.72%. By integrating this cell with a Si bottom cell, we achieve a tandem solar cell efficiency of 28.02%. This study provides a universal strategy to design SAM-based interfacial layers in p-i-n perovskite and tandem solar cells.
高效的界面电荷提取是实现高性能钙钛矿/硅串联太阳能电池的关键。在这里,我们展示了一种高效的宽带隙钙钛矿单结太阳能电池,使用商业自组装单层(sam)的共吸附策略,特别是MeO-4PACz和Br-4PACz。具有吸电子Br官能团的混合sams诱导了更大的偶极矩和HOMO能级的向下移动,从而促进了与宽带隙钙钛矿的有利能级排列。它进一步钝化界面缺陷,抑制非辐射复合。这种综合效应使SAM/钙钛矿界面上的空穴传输有效,提高了钙钛矿器件的开路电压和填充系数。因此,最佳单结钙钛矿太阳能电池的效率为19.72%。通过将该电池与硅底电池集成,我们实现了28.02%的串联太阳能电池效率。本研究提供了一种通用策略来设计基于sam的p-i-n钙钛矿和串联太阳能电池的界面层。
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引用次数: 0
Multifunctional ruthenium-based complexes for chronic wound therapy: from ligand engineering to intelligent microenvironment remodeling. 用于慢性伤口治疗的多功能钌基复合物:从配体工程到智能微环境重塑。
IF 5.1 3区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-12 DOI: 10.1039/d5nr05441a
Yulong Lan, Jianliang Shen, Lifeng Tan

Chronic wounds form a self-perpetuating vicious cycle driven by oxidative stress, immune dysregulation, and biofilm infections. Traditional monotherapies yield limited efficacy, posing significant clinical challenges. Ruthenium-based complexes (RuBCs), as an emerging therapeutic platform, offer breakthrough opportunities in this field due to their inherent multi-enzyme mimetic activity, superior photophysical properties, and high tunability achieved through ligand engineering. This review systematically elucidates how intelligent ligand design transforms ruthenium-based biomaterials from passive drugs into smart diagnostic-therapeutic integrated systems capable of sensing and responding to pathological wound microenvironments (such as abnormal pH, elevated reactive oxygen species, and specific enzymes). Initially, we analyze the chronic wound microenvironment to establish precise therapeutic targets. We subsequently detail the fundamental properties of ruthenium-based nanomaterials and complexes, along with ligand design principles, to construct a multifunctional toolkit. The core section systematically integrates multiple advanced design strategies, including environmentally responsive drug release, targeted cellular or bacterial delivery, and the synergistic integration of catalytic, phototherapeutic, and immunomodulatory functions. Furthermore, we explore how to combine real-time phosphorescence diagnostics with therapy to establish closed-loop feedback systems. Despite promising prospects, RuBCs still face significant challenges such as long-term biosafety, large-scale preparation, and in vivo efficacy validation. The conclusion outlines future directions: developing multi-stimulus-responsive systems, synergizing with advanced biomaterials, and leveraging AI-assisted design. These efforts aim to provide systematic, forward-looking theoretical and technical guidance for developing smart RuBCs for chronic wound treatment.

慢性伤口形成了一个由氧化应激、免疫失调和生物膜感染驱动的自我延续的恶性循环。传统的单一疗法疗效有限,给临床带来了重大挑战。钌基配合物(RuBCs)作为一种新兴的治疗平台,由于其固有的多酶模拟活性、优越的光物理性质以及通过配体工程实现的高度可调性,为该领域提供了突破性的机会。这篇综述系统地阐述了智能配体设计如何将基于钌的生物材料从被动药物转变为能够感知和响应病理性伤口微环境(如异常pH值、活性氧含量升高和特定酶)的智能诊断-治疗集成系统。首先,我们分析慢性伤口微环境以建立精确的治疗靶点。我们随后详细介绍了钌基纳米材料和配合物的基本性质,以及配体设计原则,以构建一个多功能工具包。核心部分系统地整合了多种先进的设计策略,包括环境响应性药物释放、靶向细胞或细菌递送,以及催化、光疗和免疫调节功能的协同整合。此外,我们探索如何将实时磷光诊断与治疗相结合,建立闭环反馈系统。尽管前景看好,但RuBCs仍面临着长期生物安全性、大规模制备和体内疗效验证等重大挑战。结论概述了未来的发展方向:开发多刺激响应系统,与先进的生物材料协同,并利用人工智能辅助设计。这些努力旨在为开发用于慢性伤口治疗的智能RuBCs提供系统的、前瞻性的理论和技术指导。
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引用次数: 0
A Dual-nanograting perovskite structure for photodetectors with enhanced light trapping. 一种用于光探测器的双纳米光栅钙钛矿结构。
IF 6.7 3区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-11 DOI: 10.1039/d5nr04907e
Rui Wei,Hongyi Zhao,Qiyang Wang,Jiren Liang,Mingzhong Lü,Weiting Weng,Shun-Xin Li
Perovskite crystals show great potential for application in photodetectors due to their superior optoelectronic properties. However, their smooth surfaces cause strong reflection and poor light trapping, limiting performance. To address this, a nanograting was engineered on both crystal surfaces to suppress reflection and enhance absorption. Experiments and simulations confirm that the structure induces strong optical field localization, improving light-harvesting efficiency and reducing optical losses. A photodetector based on the Dual-nanograting achieves 200% responsivity compared with the Planar reference device. An optical information processing system based on this structure further demonstrates potential for application in optical communication and intelligent sensing.
钙钛矿晶体由于其优越的光电性能在光电探测器中显示出巨大的应用潜力。然而,它们光滑的表面会引起强烈的反射和较差的光捕获,从而限制了性能。为了解决这个问题,在两个晶体表面都设计了纳米光栅来抑制反射和增强吸收。实验和仿真结果表明,该结构可诱导强光场定位,提高光捕获效率,降低光损耗。与Planar基准器件相比,基于双纳米光栅的光电探测器的响应率达到200%。基于该结构的光信息处理系统进一步显示了在光通信和智能传感领域的应用潜力。
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引用次数: 0
Design and Fabrication of Plasmonic Hedgehog-Shaped Covalent Organic Framework Nanocomposites for Indirect SERS-based Ultradetection of Water Contaminant Terbutryn 用于水污染物Terbutryn间接sers超检测的等离子体刺猬形共价有机框架纳米复合材料的设计与制备
IF 6.7 3区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-11 DOI: 10.1039/d5nr02476e
Tolga Zorlu, Maedeh Anisi, Mónica Quarato, Ana Vieira, Jesús Giráldez-Martínez, Carlos Gonçalves, Aitor Alvarez, Tania Prieto, T. Medina-Tautz, Lucas V. Besteiro, Miguel A. Correa-Duarte, Begoña Espiña, Laura M. Salonen, Laura Rodriguez-Lorenzo
Surface-enhanced Raman scattering (SERS) spectroscopy is an ultrasensitive analytical technique, the efficiency of which can be enhanced by developing plasmonic nanostructured substrates and sieving elements to capture target analytes close to the plasmonic surface. This study reports the development of a plasmonic hedgehog-shaped colloidal covalent organic framework (SiO2@Au@ COFHedgehog) composite as an efficient SERS substrate. First, hedgehog-shaped COF particles were synthesized, fully characterized, and their development was studied over time to gain insight into their formation. Then, SiO2@Au@COFHedgehog composite was prepared, retaining the characteristics of the crystalline COF and the hedgehog-type morphology. The composite exhibited significantly enhanced SERS intensity for 4-nitrothiophenol (4-NTP), which has a strong affinity for the Au surface via S-Au bond formation, achieving a limit of detection (LoD) of 10–10 M. This demonstrated that molecules with high affinity for the Au surface and smaller than the COF pore size (< 3 nm) can diffuse easily through the pore. Furthermore, an indirect SERS strategy for the detection of the toxic herbicide terbutryn was designed based on the reduction of the nitro group in 4-NTP to form 4,4-dimercaptoazobenzene (DMAB) when terbutryn molecules were placed close to 4-NTP-coated AuNPs, thanks to the high adsorption efficiency of the porous anisotropic COF shell by this herbicide (>50%), revealing a strong correlation between the SERS intensity ratios of specific peaks with an impressive LoD of 10–9 M (220 ng/L). Overall, these findings underscore the potential of plasmonic hedgehog-shaped COF composites as innovative nanomaterials for SERS-based detection, highlighting the exciting possibilities for developing sensitive and selective sensors for various target molecules, with implications in environmental analysis, biomedicine, and fields requiring ultrasensitive analytical techniques
表面增强拉曼散射(SERS)是一种超灵敏的分析技术,可以通过开发等离子体纳米结构衬底和筛分元件来捕获靠近等离子体表面的目标分析物来提高分析效率。本研究报道了一种等离子体刺猬状胶体共价有机框架(SiO2@Au@ COFHedgehog)复合材料作为高效SERS底物的开发。首先,合成了刺猬形状的COF颗粒,充分表征了它们的特征,并随着时间的推移研究了它们的发育,以深入了解它们的形成。然后制备SiO2@Au@COFHedgehog复合材料,该复合材料保留了晶体COF的特征和刺猬型形态。该复合材料对4-亚基噻吩(4-NTP)的SERS强度显著增强,4-亚基噻吩(4-NTP)通过S-Au键形成对Au表面具有很强的亲和力,检测限(LoD)为10-10 m。这表明对Au表面具有高亲和力且小于COF孔径(< 3nm)的分子可以很容易地通过孔扩散。此外,由于terbutryn的多孔各向异性COF壳具有较高的吸附效率(>50%),当terbutryn分子靠近4- ntp包覆的AuNPs时,将4- ntp分子中的硝基还原为4,4-二巯基偶氮苯(DMAB),设计了一种间接SERS检测策略,揭示了特定峰的SERS强度比之间具有很强的相关性,LoD高达10-9 M (220 ng/L)。总的来说,这些发现强调了等离子体刺猬形COF复合材料作为基于sers检测的创新纳米材料的潜力,突出了为各种目标分子开发敏感和选择性传感器的令人兴奋的可能性,这在环境分析、生物医学和需要超灵敏分析技术的领域具有重要意义
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引用次数: 0
Activity of ice-binding proteins can be markedly enhanced by protein tags. 蛋白标签可以显著增强冰结合蛋白的活性。
IF 6.7 3区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-11 DOI: 10.1039/d5nr04805b
Daniëlle van den Broek,Sanne N Giezen,Tim P Hogervorst,Renko de Vries,Ilja K Voets
Ice-binding proteins (IBPs) are crucial for the survival of cold-adapted organisms, as they regulate ice crystal formation and growth. To understand their molecular mode of action, fluorescence microscopy of IBPs bound to ice-crystal surfaces has been shown to be very helpful, although it is unknown whether the (fluorescent) tags typically used in these studies affect the activities of the IBPs. Here, we evaluate the impact of mEos3.2, SNAP-tag, and HaloTag on the ice-recrystallization inhibition (IRI) activity of IBPs. We find that most tags, in most orientations, do not affect the IRI activity of IBPs. These tags are promising candidates for investigating the binding mechanisms of IBPs in their native form with fluorescence microscopy. A surprising exception is the N-terminal attachment of HaloTag to QAE, an isoform of AFP type III: for this case, we find an order of magnitude higher IRI activity. Additionally, we show that HaloTag also has moderate IRI activity by itself and induces the formation of ice crystals with hexagonal prism morphology, suggesting binding affinity for the primary prism plane of ice. Our findings indicate that moderately IRI-active proteins may synergistically enhance the IRI activity of IBPs, when attached in the proper orientation.
冰结合蛋白(IBPs)对冷适应生物的生存至关重要,因为它们调节冰晶的形成和生长。为了了解它们的分子作用模式,结合在冰晶表面的IBPs的荧光显微镜已被证明是非常有用的,尽管尚不清楚这些研究中通常使用的(荧光)标签是否会影响IBPs的活性。在这里,我们评估了mEos3.2、SNAP-tag和HaloTag对IBPs冰重结晶抑制(IRI)活性的影响。我们发现大多数标签,在大多数方向上,不影响IBPs的IRI活性。这些标签是用荧光显微镜研究IBPs天然形式结合机制的有希望的候选者。一个令人惊讶的例外是HaloTag的n端附着到QAE上,这是AFP III型的一种异构体:在这种情况下,我们发现IRI活性高一个数量级。此外,我们发现HaloTag本身也具有中等的IRI活性,并诱导形成具有六棱柱形态的冰晶,这表明它与冰的主棱柱面具有结合亲和力。我们的研究结果表明,适度的IRI活性蛋白可以协同增强IBPs的IRI活性,当以适当的方向附着时。
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引用次数: 0
Catalytic Tango in Diatomic Catalysts: From Precision-Guided Pair Construction to Machine-Learning-Driven Identification and Design 双原子催化剂中的催化探戈:从精确引导的对构建到机器学习驱动的识别和设计
IF 6.7 3区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-11 DOI: 10.1039/d5nr05121e
Bowen Jiang, Jishui Huang, Kuibo Yin, Litao Sun
Diatomic catalysts (DACs) are composed of two neighboring metal centers, each stabilized by its own coordination environment, that extend single-atom precision into a cooperative two-site manifold. By programmably tuning composition, geometry, and local microenvironment, DACs bridge the gap between isolated single-atom sites and extended clusters, and can enable cross-site electronic coupling, dual-site adsorption motifs, and short-range relay pathways that are difficult to realize on mononuclear sites, effectively creating a catalytic “tango” in which two adjacent centers cooperate through shared electronic structure and intermediates. This Review first highlights strategies for precision-guided pair construction, including probability-controlled density generators that increase the likelihood of forming adjacent sites, ordered coordination networks (MOFs, COFs, and related 2D frameworks) that pre-organize metal nodes at defined separations, and multinuclear metal–organic complexes that offer molecular blueprints for well-defined dimers and higher oligomers. These platforms are then used to discuss representative modes of intersite cooperativity: charge redistribution and orbital hybridization between neighboring metals, distance- and orientation-dependent co-adsorption and transition states on dual sites, and sequential reaction pathways in which different elementary steps are preferentially accommodated by different atoms in the pair. Finally, the Review surveys how atomic-resolution electron microscopy and related correlative imaging are beginning to be combined with machine-learning workflows for automatic identification, classification, and screening of neighboring metal sites, sketching an emerging and promising route toward machine-learning-assisted identification and design of diatomic motifs.
双原子催化剂(DACs)由两个相邻的金属中心组成,每个中心都由自己的配位环境稳定,将单原子精度扩展到合作的二元流形。通过可编程地调整组成、几何形状和局部微环境,dac弥合了孤立的单原子位点和扩展簇之间的差距,并且可以实现在单个核位点上难以实现的跨位点电子耦合、双位点吸附基序和短程中继途径,有效地创建了催化“探戈”,其中两个相邻中心通过共享电子结构和中间体进行合作。本综述首先强调了精确引导对构建的策略,包括概率控制密度生成器,增加形成相邻位点的可能性,有序配位网络(mof, COFs和相关的2D框架),在定义的分离处预先组织金属节点,以及多核金属有机配合物,为定义明确的二聚体和高级低聚物提供分子蓝图。然后,这些平台被用来讨论具有代表性的位点间协同作用模式:相邻金属之间的电荷重分配和轨道杂化,依赖于距离和取向的双位点共吸附和过渡态,以及不同基本步骤优先被不同原子容纳的顺序反应途径。最后,综述调查了原子分辨率电子显微镜和相关成像如何开始与机器学习工作流程相结合,用于自动识别,分类和筛选邻近金属位点,概述了机器学习辅助识别和设计双原子基序的新兴和有前途的路线。
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引用次数: 0
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Nanoscale
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