结构化学最新文献

英文中文

Addressing agricultural (micro)plastics pollution: The promises and perspectives of framework-based photocatalysis 解决农业（微）塑料污染：基于框架的光催化的前景和前景

IF 10.3 4区化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR

结构化学

Pub Date : 2025-12-01 DOI: 10.1016/j.cjsc.2025.100752

Shuyu Li , Ning Gong , Zhi-Hao Lin , Jing Chen , Ge Chen , Jun Lv , Guangyang Liu , Yi Niu , Liao-Yuan Yao , Donghui Xu , Lin Qin

Plastics, renowned for their flexibility, stability, and cost-effectiveness, have become indispensable materials in modern life. However, their extensive use has led to a global environmental and health crisis. Especially, plastic products infiltrate agroecosystems through atmospheric deposition, irrigation water, soil contamination, and the degradation of plastic mulch films, posing significant risks to vegetable quality and safety. Traditional disposal methods, such as incineration and landfilling, are energy-intensive and ecologically harmful, necessitating the development and application of innovative technologies for plastic removal. This paper reviews representative advanced (micro)plastic removal technologies, with a particular focus on frameworks-containing photocatalysis as a promising green method for processing (micro)plastics. First, we analyze and compare traditional, then discuss emerging removal technologies. Next, we elaborate on the principles of photocatalytic degradation of plastic products, discuss key influencing factors, and classify various photocatalysts. Additionally, we highlight the limitations of conventional photocatalysts, such as TiO₂ and ZnO, and emphasize the advantages of framework materials (e.g., MOFs, COFs, ZIFs) in photocatalytic degradation, including their structural tunability and development potential. Finally, based on the current progress and applications of framework photocatalysts, we identify existing limitations and propose future research directions. This review provides a theoretical foundation and innovative technological insights to address the global challenge of plastic pollution.

塑料以其柔韧性、稳定性和性价比而闻名，已成为现代生活中不可或缺的材料。然而，它们的广泛使用导致了全球环境和健康危机。特别是，塑料制品通过大气沉降、灌溉水、土壤污染、地膜降解等途径渗入农业生态系统，对蔬菜质量安全构成重大威胁。传统的处理方法，如焚烧和堆填，是能源密集和生态有害的，需要开发和应用创新的技术来清除塑料。本文综述了具有代表性的先进（微）塑料去除技术，重点介绍了含框架光催化作为处理（微）塑料的一种有前途的绿色方法。首先，我们分析和比较了传统的去除技术，然后讨论了新兴的去除技术。接下来，我们阐述了光催化降解塑料制品的原理，讨论了关键的影响因素，并对各种光催化剂进行了分类。此外，我们强调了传统光催化剂（如TiO2和ZnO）的局限性，并强调了框架材料（如mof， COFs, zif）在光催化降解中的优势，包括它们的结构可调性和发展潜力。最后，根据目前框架光催化剂的研究进展和应用情况，指出了存在的局限性，并提出了未来的研究方向。这一综述为解决塑料污染的全球性挑战提供了理论基础和创新的技术见解。

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引用次数: 0

Fluorescence enhancement of perylene diimide: Design strategy and application 苝二亚胺的荧光增强：设计策略及应用

IF 10.3 4区化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR

结构化学

Pub Date : 2025-12-01 DOI: 10.1016/j.cjsc.2025.100756

Ya-Ru Qu , Kai-Li Tian , Han-Jun Huang , Jia-Jun Tu , Ai-Hao Chen , Hai-Jun Sun , Maxim V. Bermeshev , Shao-Jie Wang , Wen-Bin Li , Xiang-Kui Ren

Perylene diimide (PDI) derivatives have emerged as a class of important organic fluorescent materials owing to their high extinction coefficient, excellent thermal and photostability, and versatile structural tunability. However, due to its intrinsic rigid planar structure, π-π stacking is easy to occur, resulting in aggregation-caused quenching (ACQ). In recent years, extensive efforts have been devoted to overcome this challenge and enhance the fluorescence performance of PDIs. This review systematically summarizes representative strategies from three major perspectives: (i) Rational molecular design, including the introduction of bulky aromatic substituents, dendritic or polyhedral oligomeric silsesquioxane (POSS) units to provide steric hindrance, as well as the activation of aggregation-induced emission (AIE); (ii) Polymer-based regulation strategies, including physical blending with polymer hosts and covalent integration into polymer backbones, which provide spatial isolation and structural robustness; and (iii) Supramolecular assembly, where host-guest inclusion and self-assembly pathways precisely tune intermolecular packing and excitonic coupling. These strategies have enabled significant improvements in fluorescence quantum yield (FLQY) across solution, aggregate, and solid states. Furthermore, highly emissive perylene diimide (PDI) derivatives have demonstrated broad applicability in biomedicine, sensing and anti-counterfeiting, and optoelectronic devices such as organic light-emitting diodes (OLEDs). This review highlights the fundamental design principles, performance optimization strategies, and emerging application frontiers of PDI-based luminescent materials, providing guidance for their further development toward multifunctional and sustainable optoelectronic technologies.

苝酰二亚胺（PDI）衍生物因其高消光系数、优异的热稳定性和光稳定性以及多种结构可调性而成为一类重要的有机荧光材料。然而，由于其固有的刚性平面结构，π-π堆积容易发生，导致聚集引起的猝灭（ACQ）。近年来，人们一直在努力克服这一挑战，提高pdi的荧光性能。本文从三个主要方面系统总结了具有代表性的策略：(1)合理的分子设计，包括引入大体积芳香取代基、树突或多面体低聚硅氧烷（POSS）单元来提供空间位阻，以及激活聚集诱导发射（AIE）；㈡基于聚合物的调节策略，包括与聚合物宿主的物理共混和共价整合到聚合物骨架中，从而提供空间隔离和结构坚固性；（iii）超分子组装，其中主-客体包涵和自组装途径精确调节分子间包装和激子耦合。这些策略使荧光量子产率（FLQY）在溶液、聚集体和固体状态有了显著的提高。此外，高发射度的苝二亚胺（PDI）衍生物在生物医学、传感和防伪以及光电器件（如有机发光二极管（oled））中已被证明具有广泛的适用性。本文综述了pdi基发光材料的基本设计原理、性能优化策略和新兴应用领域，为pdi基发光材料向多功能和可持续光电技术的进一步发展提供了指导。

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引用次数: 0

Solvent-coordination directed control of electron transfer dynamics in photoactive complexes 光活性配合物中电子转移动力学的溶剂配位定向控制

IF 10.3 4区化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR

结构化学

Pub Date : 2025-12-01 DOI: 10.1016/j.cjsc.2025.100753

Yan-Rui Zhao, Jin Zhang, Shi-Kun Yan, Guang-Zhi Zhou, Ya-Hui Wang, Qi-Yue Xin, Ji-Xiang Hu

Photochromic materials attract significant attention for their applications in anticounterfeiting devices, optical switches and molecular sensors. However, the influence of solvent molecules, particularly coordinated solvents, on electron transfer (ET) photochromic systems remains poorly understood. In this study, we synthesized a series of isostructural metal-organic complexes (MOCs), [Mn(ADC)(L)]_n (ADC = 9,10-anthracenedicarboxylic acid, L = DMF for 1, DMA for 2, MEA for 3, and DMSO for 4) to investigate the solvent-chromic behavior. All these MOCs exhibit typical radical-induced chromism upon illumination with a xenon lamp at room temperature. It is worth noting that coordination solvent molecules significantly modulate the photochromic response rate. Among the compounds studied, compound 1 exhibits the fastest response, while compound 3 shows the slowest. This variation in rate correlates with differences in the optimal ET path length within their structures. Specifically, solvent molecules regulate the C–H···π interaction distance through their steric hindrance and electronic properties. Shorter C–H···π paths facilitate more efficient ET upon photoexcitation, thus leading to faster photochromic response rates. Furthermore, illumination actuates magnetic couplings between photogenerated radicals and Mn²⁺ centers, resulting in a significant increase in room-temperature magnetization, demonstrating a photomagnetic response. This study demonstrates that coordinating solvent selection effectively controls photoinduced ET behavior, providing new insights for designing advanced photoactive materials.

光致变色材料在防伪器件、光开关和分子传感器等方面的应用备受关注。然而，溶剂分子，特别是配位溶剂，对电子转移（ET）光致变色系统的影响仍然知之甚少。在本研究中，我们合成了一系列同结构金属-有机配合物（MOCs）， [Mn(ADC)(L)]n （ADC = 9,10-蒽二羧酸，L = DMF为1，DMA为2，MEA为3，DMSO为4）来研究其溶剂-变色行为。这些MOCs在室温氙灯照射下均表现出典型的自由基致变色现象。值得注意的是，配位溶剂分子显著调节光致变色反应速率。在所研究的化合物中，化合物1的反应最快，而化合物3的反应最慢。这种速率的变化与它们结构内最佳ET路径长度的差异有关。溶剂分子通过空间位阻和电子性质调节C-H··π相互作用距离。更短的C-H··π路径有助于光激发时更有效的ET，从而导致更快的光致变色响应速率。此外，光照激发了光生成自由基和Mn2+中心之间的磁耦合，导致室温磁化强度显著增加，显示出光磁响应。本研究表明，协调溶剂选择有效地控制了光致ET行为，为设计先进的光活性材料提供了新的见解。

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引用次数: 0

NaAg3Ga8S14: A new diamond-like framework infrared nonlinear optical material derived from AgGaS2 NaAg3Ga8S14：由AgGaS2衍生的新型类金刚石框架红外非线性光学材料

IF 10.3 4区化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR

结构化学

Pub Date : 2025-12-01 DOI: 10.1016/j.cjsc.2025.100757

Hongshan Wang , Zhenglong Li , Ran An , Zhenyou Wang , Juanjuan Lu , Guansong Zheng , Zhihua Yang , Yu Chu , Junjie Li

Diamond-like AgGaS₂ (DL AGS), as the typical infrared nonlinear optical (IR NLO) material, has suffered from its intrinsic drawbacks like narrow band gap (E_g) and low laser-induced damage threshold (LIDT). In this work, by first introducing [NaS₈] polyhedral unit into the

A_{2}^{I} Q^{VI}

-Ag₂Q^VI-

C_{2}^{III} Q_{3}^{VI}

system, a new Ag-based sulfide NaAg₃Ga₈S₁₄ with diamond-like framework (DLF) has been successfully synthesized via a high-temperature solid-state method in experiment. The compound shows a wide E_g (∼3.0 eV), high LIDT (3.0 × AGS) and moderate phase-matching NLO response (∼0.7 × AGS), effectively balancing the E_g (≥ 3.0 eV) and NLO response (≥ 0.5 × AGS), demonstrating its promise for IR NLO applications. Theoretical calculations elucidate the orbital hybridization between Na 3s, Ag 4d5s and S 3p enhances E_g, and the aligned NLO-active units ([AgS₄] and [GaS₄]) induce moderate NLO response in the compound. These findings not only expand the chemical and structural diversities of Ag-based chalcogenides, but also provide effective strategies for designing DLF functional materials derived from diamond-like structures.

类金刚石AgGaS2 （DL AGS）作为典型的红外非线性光学（IR NLO）材料，存在窄带隙（Eg）和低激光损伤阈值（LIDT）等固有缺陷。本文首次在A2IQVI-Ag2QVI-C2IIIQ3VI体系中引入[NaS8]多面体单元，在实验中通过高温固相法成功合成了一种新型类金刚石骨架（DLF） ag基硫化物NaAg3Ga8S14。该化合物具有宽Eg （~ 3.0 eV）、高LIDT （3.0 × AGS）和中等相位匹配NLO响应（~ 0.7 × AGS），有效地平衡了Eg（≥3.0 eV）和NLO响应（≥0.5 × AGS），显示了其在红外NLO应用中的前景。理论计算表明Na 3s， Ag 4d5s和s3p之间的轨道杂化增强了Eg，并且排列的NLO活性单元（[AgS4]和[GaS4]）在化合物中诱导适度的NLO响应。这些发现不仅扩大了银基硫族化合物的化学和结构多样性，而且为设计类金刚石结构衍生的DLF功能材料提供了有效的策略。

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引用次数: 0

CO2 valorization to amides via S-scheme photocatalysis with tandem carbonylation 串联羰基化s -方案光催化CO2价化生成酰胺

IF 10.3 4区化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR

结构化学

Pub Date : 2025-12-01 DOI: 10.1016/j.cjsc.2025.100718

Weikang Wang , Lele Wang , Qinqin Liu

引用次数: 0

A stereochemically stable double-helical trinuclear bis(tridipyrrin) complex exhibiting near-infrared chiroptical properties 一种立体化学稳定的双螺旋三核二（三吡啶）配合物，具有近红外热学性质

IF 10.3 4区化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR

结构化学

Pub Date : 2025-12-01 DOI: 10.1016/j.cjsc.2025.100722

Yingjian Shang , Xuefeng Zhao , Tao Wu , Yanhui He , Xing Guo , Hongwei Si , Lijuan Jiao , Erhong Hao , Wei Miao

A novel double-stranded trinuclear bis(tridipyrrin) zinc(II) complex, constructed from a linear π-conjugated tridipyrrin ligand, was synthesized and characterized. The complex featuring six directly linked dipyrrin units exhibits a stable double-helical structure with two non-superimposable P and M enantiomers, as confirmed by X-ray crystallography. Chirality was further demonstrated through HPLC separation and mirror-image circular dichroism (CD) spectra. The complex shows strong near-infrared (NIR) absorption and excellent solubility in various solvents, attributed to its sterically hindered structure. Spectroscopic, electrochemical, and theoretical studies revealed its unique electronic properties and redox behavior. This work advances the design of chiral NIR-active metallo-supramolecular systems and highlights potential applications in chiroptical materials.

合成了一种新型的双链三核双（三吡啶）锌（II）配合物，该配合物是由线性π共轭三吡啶配体构成的。x射线晶体学证实，该配合物具有六个直接相连的二吡啶单元，具有两个不重叠的P和M对映体，具有稳定的双螺旋结构。通过HPLC分离和镜像圆二色光谱进一步证实了手性。由于其位阻结构，该配合物在各种溶剂中具有较强的近红外吸收和良好的溶解度。光谱、电化学和理论研究揭示了其独特的电子性质和氧化还原行为。这项工作推进了手性nir活性金属超分子体系的设计，并强调了手性nir活性金属超分子体系在手性材料中的潜在应用。

引用次数: 0

Accelerated discovery of stable and extra-large-pore nano zeolites: A paradigm shift in catalytic materials 加速发现稳定和超大孔径纳米沸石：催化材料的范式转变

IF 10.3 4区化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR

结构化学

Pub Date : 2025-12-01 DOI: 10.1016/j.cjsc.2025.100720

Basem E. Keshta , Lingyao Wang , Yuanbin Zhang

引用次数: 0

Fine-tuning of Hofmann-type metal-organic frameworks for highly efficient separation of C4 olefins 用于高效分离C4烯烃的hofmann型金属-有机骨架的微调

IF 10.3 4区化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR

结构化学

Pub Date : 2025-12-01 DOI: 10.1016/j.cjsc.2025.100744

Jun-Xian Chen , Xian-Xian Xiao , Libo Li , Jinping Li , Rui-Biao Lin , Xiao-Ming Chen

Separation of ternary C₄ olefins (n-butene, iso-butene and 1,3-butadiene) is very challenging but crucial in the petrol-chemical industry due to their similar molecular sizes and properties. Herein, to optimize the separation efficiency for separation of C₄ olefins, a new Hofmann-type MOF, [Ni(piz)Ni(CN)₄] (piz = piperazine)—isostructural to the typical one [Ni(pyz)Ni(CN)₄] (pyz = pyrazine), has been synthesized by a facile method from aqueous solution. The pore size reduction of [Ni(piz)Ni(CN)₄] (3.62 Å, in contrast to 3.85 Å in [Ni(pyz)Ni(CN)₄]) results in negligible iso-butene (i-C₄H₈) uptake (from 2.92 to 0.04 mmol g⁻¹) whereas retaining significant uptake for 1,3-butadiene (1,3-C₄H₆, 1.96 mmol g⁻¹) and n-butene (n-C₄H₈, 1.47 mmol g⁻¹), showing much higher uptake ratios of 1,3-C₄H₆/i-C₄H₈ (47) and n-C₄H₈/i-C₄H₈ (35) that outperform most of the benchmark porous materials for separating C₄ olefins. Breakthrough experiments demonstrate successful separation of high-purity (99.9999%) i-C₄H₈ and 1,3-C₄H₆ from equimolar 1,3-C₄H₆/i-C₄H₈, n-C₄H₈/i-C₄H₈ and 1,3-C₄H₆/n-C₄H₈/i-C₄H₈ mixtures.

三元C4烯烃（正丁烯、异丁烯和1,3-丁二烯）的分离是非常具有挑战性的，但由于它们的分子大小和性质相似，在石油化工工业中至关重要。为了优化C4烯烃的分离效率，在水溶液中采用易溶法合成了与典型的[Ni(pyz)Ni(CN)4] （pyz = pyrazine）结构相同的新型hofmann型MOF [Ni(pyz)Ni(CN)4] （pyz = pyrazine）。[Ni(pyz)Ni(CN)4]的孔径减小(3.62 Å，而[Ni（pyz)Ni(CN)4]的孔径减小为3.85 Å）导致异丁烯（i-C4H8）的吸收率可以忽略（从2.92到0.04 mmol g−1），而对1,3-丁二烯（1,3- c4h6, 1.96 mmol g−1）和正丁烯（n-C4H8, 1.47 mmol g−1）的吸收率保持显著，显示出更高的吸收率1,3- c4h6 /i-C4H8（47）和n-C4H8/i-C4H8(35)，优于大多数分离C4烯烃的基准多孔材料。突破性实验表明，从等摩尔的1,3- c4h6 /i-C4H8、n-C4H8/i-C4H8和1,3- c4h6 /n-C4H8/i-C4H8混合物中成功分离出高纯度（99.9999%）的i-C4H8和1,3- c4h6 /n-C4H8/i-C4H8混合物。

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引用次数: 0

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