Chinese Chemical Letters最新文献

英文中文

F/N interface engineering of nonflammable polymer electrolyte for wide-temperature quasi-solid-state Li metal batteries 宽温准固态锂金属电池用不燃聚合物电解质的F/N界面工程

IF 8.9 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2025-09-09 DOI: 10.1016/j.cclet.2025.111815

Lisi Xu , Maosheng Li , Anqi He , Haijiao Xie , Kuirong Deng

Polymer-electrolyte-based solid-state Li metal batteries with high-voltage Ni-rich cathodes are promising energy storage technologies owing to their favorable security and high energy densities. However, operating in wide temperature range and at high voltage is a tough challenge for them. Herein, F/N donating fluorinated-amide-based plasticizers regulated polymer electrolyte capable of enabling high-voltage Li||LiNi_0.8Co_0.1Mn_0.1O₂ (NCM811) batteries with excellent performance in wide temperature range is developed. F/N donating fluorinated-amide-based plasticizers significantly improve ionic conductivity (1.52 mS/cm at 30 °C), enhance oxidation stability (5.0 V vs. Li⁺/Li) and fabricate robust LiF/Li₃N-rich electrode-electrolyte interphases, which significantly improve the interface stability of Li metal anode and NCM811 cathode. The designed polymer electrolyte is nonflammable and has excellent dimensional stability at 200 °C. Capitalizing on these advantageous attributes, the Li||NCM811 cells show excellent cycle stability and rate capability from −20 °C to 60 °C at high voltages (∼4.6 V), and under high-loading full cell condition, which display impressive capacity retention of 84.4 % after 1000 cycles and ultrahigh capacity of 154.8 mAh/g at 10 C. This work provides a rational design strategy of polymer electrolytes for wide-temperature high-energy solid-state Li metal batteries.

具有高电压富镍阴极的聚合物电解质固态锂金属电池具有良好的安全性和高能量密度，是一种很有前途的储能技术。然而，在宽温度范围和高电压下工作对他们来说是一个艰巨的挑战。本文研制了F/N供氟化酰胺基增塑剂调控聚合物电解质，可使高压Li||LiNi0.8Co0.1Mn0.1O2 （NCM811）电池在宽温度范围内具有优异的性能。F/N给体氟酰胺基增塑剂显著提高了离子电导率（30 °C时为1.52 mS/cm），增强了氧化稳定性（5.0 V vs. Li+/Li），制备了坚固的富LiF/ li3n电极-电解质界面，显著提高了Li金属阳极和NCM811阴极的界面稳定性。所设计的聚合物电解质不易燃，在200 °C时具有优异的尺寸稳定性。利用这些优势，Li||NCM811电池在高电压（~ 4.6 V）和高负载满电池条件下，在- 20 °C至60 °C范围内表现出优异的循环稳定性和倍率能力，在1000次循环后的容量保持率为84.4 %，在10℃时的超高容量为154.8 mAh/g。这项工作为宽温高能固态锂金属电池的聚合物电解质设计提供了合理的策略。

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引用次数: 0

Ligand-bridged nanoassemblies boost the peroxidase-mimicking activity of gold nanoclusters 配体桥接纳米组件提高了金纳米团簇的过氧化物酶模拟活性

IF 8.9 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2025-09-09 DOI: 10.1016/j.cclet.2025.111806

Jin-Ao Li , Nana Pan , Li Lu , Yifan Wei , Wenchang Hu , Zhiyang Zhang , Houda Amrani , Fang Huang , Xiaojuan Wang

Rational design of nanozymes with enhanced catalytic efficiency remains a central challenge in the development of artificial enzymes. Herein, we report the construction of ultrasmall gold nanocluster-based nanoassemblies (Dp-AuNCs@Fe²⁺) through the coordination of Fe²⁺ ions by a dopa-containing peptidomimetic ligand (DpCDp). This nanoarchitecture simultaneously integrates catalytically active gold cores and redox-active Fe²⁺ centers, bridged by DpCDp to facilitate directional electron transfer. Comprehensive spectroscopic and kinetic analyses reveal that DpCDp promotes efficient charge migration from the Au core to surface-bound Fe²⁺, significantly enhancing H₂O₂-mediated peroxidase-like activity. Compared to bare Dp-AuNCs, Dp-AuNCs@Fe²⁺ display a 4.3-fold improvement in detection sensitivity, a 6.7-fold increase in catalytic efficiency, and markedly stronger hydroxyl radical generation. Mechanistically, this activity stems from a synergistic triad: direct H₂O₂ oxidation at gold surfaces, radical generation at Fe²⁺ sites, and DpCDp-facilitated electron shuttling. This work presents a robust strategy for nanozyme enhancement via electronic and structural co-engineering, offering valuable insights for the future design of bioinspired catalytic systems.

合理设计具有高催化效率的纳米酶仍然是人工酶发展的核心挑战。在此，我们报道了通过含多巴的拟肽配体（DpCDp）配位Fe2+离子构建超小金纳米团簇纳米组件（Dp-AuNCs@Fe2+）。这种纳米结构同时集成了催化活性金核和氧化还原活性Fe2+中心，由DpCDp桥接以促进定向电子转移。综合光谱和动力学分析表明，DpCDp促进了电荷从Au核向表面结合的Fe2+的有效迁移，显著增强了h2o2介导的过氧化物酶样活性。与裸Dp-AuNCs相比，Dp-AuNCs@Fe2+的检测灵敏度提高了4.3倍，催化效率提高了6.7倍，羟基自由基的生成明显增强。从机制上讲，这种活性源于三个协同作用：H2O2在金表面的直接氧化，Fe2+位点的自由基生成，以及dpcdp促进的电子穿梭。这项工作提出了一种通过电子和结构协同工程增强纳米酶的强大策略，为未来设计生物激发催化系统提供了有价值的见解。

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引用次数: 0

Supramolecular catalysis enabled by chiral molecular cages with anion-π interaction capability 具有阴离子-π相互作用能力的手性分子笼实现了超分子催化

IF 8.9 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2025-09-06 DOI: 10.1016/j.cclet.2025.111796

Jinchen Li , Tangxin Xiao , Kai Diao , Zhouyu Wang , Leyong Wang

引用次数: 0

Linear paired electrolysis enables redox-neutral benzylation of N-heteroarenes with benzyl halides using ion resin as the recyclable electrolyte 采用离子树脂作为可循环电解质，实现了n -杂芳烃与卤苄的氧化还原-中性苄基化反应

IF 8.9 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2025-09-06 DOI: 10.1016/j.cclet.2025.111795

Yan-Cui Wen , Jia-Cheng Hou , Qian Zhou , Sheng-Hua Wang , Jun Jiang , Zi Yang , Hai-Tao Zhu , Zu-Li Wang , Wei-Min He

Herein, we have developed a sustainable linear paired electrolysis strategy for the redox-neutral benzylation of N-heteroarenes with benzyl halides using solid ion resin as the recyclable electrolyte. This method sufficiently utilizes both cathodic and anodic reactions to produce a variety of benzylated N-heteroarenes, features high atom- and step-economy, excellent energy efficiency, operational simplicity, good functional group tolerance, mild conditions and no requirement of sacrifice reagent and base additive. Importantly, the inexpensive and commercially available solid ion resin electrolyte was validated in both gram-scale synthesis and electrolyte cycling experiment. We hope this strategy not only provides a sustainable synthetic strategy for benzylated compounds but also develops the further utilization of ion resin in electrosynthesis as well as linear paired electrolysis.

在此，我们开发了一种可持续的线性配对电解策略，用于n -杂芳烃与苄基卤化物的氧化还原-中性苄基化，使用固体离子树脂作为可回收电解质。该方法充分利用阴极和阳极反应制备多种苄基化n -杂芳烃，具有原子经济性和阶梯经济性高、能源效率优异、操作简单、官能团耐受性好、条件温和、不需要牺牲试剂和碱添加剂等特点。重要的是，廉价且可商用的固体离子树脂电解质在克级合成和电解质循环实验中得到了验证。我们希望这一策略不仅为苯基化化合物的可持续合成提供了一种策略，而且也为离子树脂在电合成和线性配对电解中的进一步利用提供了途径。

引用次数: 0

Asymmetric catalysis for the synthesis of planar chiral ferrocene derivatives 平面手性二茂铁衍生物的不对称催化合成

IF 8.9 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2025-09-05 DOI: 10.1016/j.cclet.2025.111793

Haitao Liu, Youlin Deng, Dan Ling, Lingzhu Chen, Zhichao Jin

The asymmetric catalytic synthesis of planar chiral ferrocene derivatives has received dramatic attention in recent years. Transition metal-catalyzed asymmetric cross-coupling reactions and CH functionalization reactions have played significant roles in the stereoselective construction of planar chiral ferrocene derivatives. Transition metals such as copper, palladium, rhodium, iridium, gold, and platinum have been adopted as the effective catalysts in combination with various chiral ligands to achieve satisfactory yields and stereoselectivity. Organic catalysts have also shown great potential in the synthesis of planar chiral ferrocenes. Chiral amines and N-heterocyclic carbenes (NHCs) have been the key catalysts for facile access to multi-functional ferrocene derivatives. Some of the planar chiral ferrocene molecules obtained from the above methods have demonstrated promising applications in the development of novel ligands for asymmetric synthesis and pesticides for plant protection. This review provides an overview on the key progresses in the catalytic synthesis of planar chiral ferrocene derivatives using transition metal catalysts and organic catalysts. The merits, challenges and potential directions in the future development within this highly active research field are also discussed at the end of this review.

不对称催化合成平面手性二茂铁衍生物是近年来研究的热点。过渡金属催化的不对称交叉偶联反应和CH功能化反应在平面手性二茂铁衍生物的立体选择性构建中起着重要作用。铜、钯、铑、铱、金、铂等过渡金属与各种手性配体结合作为有效催化剂，获得了满意的产率和立体选择性。有机催化剂在平面手性二茂铁的合成中也显示出巨大的潜力。手性胺和n -杂环碳烯是制备多功能二茂铁衍生物的关键催化剂。通过上述方法获得的一些平面手性二茂铁分子在开发新型不对称合成配体和植物保护用农药方面具有广阔的应用前景。综述了过渡金属催化剂和有机催化剂催化合成平面手性二茂铁衍生物的研究进展。最后对这一活跃研究领域的优点、面临的挑战和未来发展的潜在方向进行了讨论。

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引用次数: 0

Enhancing photovoltaic performance via γ-positioned side-chains engineering of Y-series non-fullerene acceptors 通过y系列非富勒烯受体的γ定位侧链工程提高光伏性能

IF 8.9 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2025-09-05 DOI: 10.1016/j.cclet.2025.111787

Ruixiang Fang , Yilan Zhai , Huijuan Bi , Caixuan Wang , Ailing Tang , Shiming Zhang , Zhixiang Wei , Kun Lu

In the field of organic solar cells (OSCs), side-chain engineering is a key strategy for developing high-performance non-fullerene small molecule acceptors (SMAs), which could adjust the material solubility and modulate the intermolecular stacking properties, profoundly impacting the film morphology and thus acting on the final power conversion efficiency (PCE) of the materials. In this study, two asymmetric acceptor molecules, Qx-PhBr-BO and Qx-PhBr-X, were synthesized by migrating the branching site of the outer side chain from the β-site to the γ-site. The branching site located at the γ-site could reduce the steric-hindrance effect and enhance the molecular aggregation behavior, giving rise to redshifted absorption and tight π-π stacking. Morphology analysis shows that the Qx-PhBr-X-based devices have smoother surfaces and a phase-separated structure, which is more favorable for charge transport and extraction. The Qx-PhBr-X-based devices exhibit balanced hole-electron mobility, efficient exciton dissociation, and low charge recombination. As a result, Qx-PhBr-X with γ-site branching exhibits superior photovoltaic performance with a PCE of 17.16 %, which is significantly higher than that of Qx-PhBr-BO at 16.28 %. These results highlight the importance of side-chain modifications for optimizing OSC efficiency and provide an important reference for precise tuning of side-chain structures in future molecular design.

在有机太阳能电池（OSCs）领域，侧链工程是开发高性能非富勒烯小分子受体（SMAs）的关键策略，它可以调节材料的溶解度和分子间的堆叠特性，深刻影响薄膜的形态，从而影响材料的最终功率转换效率（PCE）。本研究将Qx-PhBr-BO和Qx-PhBr-X两个不对称受体分子通过将外侧链的分支位点从β-位点迁移到γ-位点合成。位于γ-位点的支化位点降低了空间位阻效应，增强了分子的聚集行为，产生了红移吸收和紧密的π-π堆积。形貌分析表明，qx - phbr - x基器件表面光滑，具有相分离结构，更有利于电荷输运和萃取。基于qx - phbr - x的器件具有平衡的空穴电子迁移率，高效的激子解离和低电荷复合。结果表明，具有γ-位点支化的Qx-PhBr-X的PCE为17.16 %，显著高于Qx-PhBr-BO的16.28 %。这些结果突出了侧链修饰对优化盐碳效率的重要性，并为未来分子设计中侧链结构的精确调整提供了重要参考。

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引用次数: 0

Covalent organic framework ionomers enable synergistic efficient transport of protons and oxygen in medium-temperature proton exchange membrane fuel cells 共价有机骨架离聚体在中温质子交换膜燃料电池中实现了质子和氧的协同高效传输

IF 8.9 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2025-09-02 DOI: 10.1016/j.cclet.2025.111784

Zijie Lin, Qing Li

引用次数: 0

Enantioconvergent reductive amidation of benzyl ammonium salts for synthesis of α-chiral amides 苄基铵盐的对映收敛还原酰胺化合成α-手性酰胺

IF 8.9 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2025-09-01 DOI: 10.1016/j.cclet.2025.111779

Saima Perveen , Xicheng Wang , Tao Li , Linghua Wang , Shuai Zhang , Yizhao Ouyang , Xue Zhao , Liang Xu , Pengfei Li

α-Chiral amides are common in pharmaceuticals, agrochemicals, natural products, and peptides, prompting the need for new synthetic methods. Here, we introduce a nickel-catalyzed asymmetric reductive amidation method to synthesize α-chiral amides from benzyl ammonium salts and isocyanates. The key to success is using a chiral 2,2′-bipyridine ligand (-)-Ph-SBpy, enabling high yield (up to 95 %) and enantiomeric ratio (up to 98:2 er) under mild conditions. Addition of phenol prevents isocyanate polymerization by reversibly forming a carbamate intermediate, enhancing selectivity and efficiency. The synthetic utility is showcased through transformations of the enantioenriched amides, and the mechanism and enantioselectivity are supported by experimental and computational studies.

α-手性酰胺在医药、农用化学品、天然产物和多肽中都很常见，这促使人们需要新的合成方法。本文介绍了以苯基铵盐和异氰酸酯为原料，镍催化不对称还原酰胺化合成α-手性酰胺的方法。成功的关键是使用手性2,2 ' -联吡啶配体(-)- ph - sbpy，在温和的条件下实现高收率（高达95% %）和对映体比（高达98:2 er）。苯酚的加入通过可逆地形成氨基甲酸酯中间体来防止异氰酸酯聚合，提高了选择性和效率。通过对映体富集酰胺的转化，展示了其合成效用，并通过实验和计算研究支持了其机理和对映体选择性。

引用次数: 0

One-step synthesis of trimetallic PdCuNi porous nanoflowers for enhanced alcohol oxidation 一步法合成三金属PdCuNi多孔纳米花增强醇氧化

IF 8.9 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2025-08-26 DOI: 10.1016/j.cclet.2025.111756

Xinyu Gu , Jun Yu , Huiyu Sun , Nannan Zhang , Zhengying Wu , Yukou Du

The three-dimensional (3D) Pd-based nanoflower structures, assembled from two-dimensional (2D) nanosheets, are characterized by their stable and ordered configurations. These structures have been extensively designed as anode materials for fuel cells. However, the exploration of trimetallic nanoflowers with porous architectures remains limited. In this study, we present a straightforward one-step solvothermal method for the synthesis of trimetallic PdCuNi porous nanoflowers (PNFs). Leveraging several unique advantages, such as an open superstructure, high porosity, and enhanced electronic interactions among the trimetals, the resulting PdCuNi PNFs demonstrate significantly improved electrochemical performance, with mass activities reaching 5.94 and 10.14 A/mg for the ethanol oxidation reaction (EOR) and the ethylene glycol oxidation reaction (EGOR), respectively. Furthermore, the PdCuNi PNFs exhibit optimized d-band centers and the most negative onset oxidation potential, indicating enhanced antitoxicity and stability. This study not only provides a novel perspective on the synthesis of 3D porous nanomaterials but also highlights the potential application value of trimetallic nanoalloys in catalysis.

三维（3D）基于pd的纳米花结构，由二维（2D）纳米片组装而成，具有稳定有序的结构特征。这些结构已被广泛设计为燃料电池的阳极材料。然而，具有多孔结构的三金属纳米花的探索仍然有限。在这项研究中，我们提出了一种简单的一步溶剂热合成三金属PdCuNi多孔纳米花（PNFs）的方法。利用开放的上层结构、高孔隙度和增强的三金属之间的电子相互作用等独特优势，所制得的PdCuNi PNFs具有显著提高的电化学性能，在乙醇氧化反应（EOR）和乙二醇氧化反应（EGOR）中分别达到5.94和10.14 A/mg的质量活性。此外，PdCuNi PNFs具有优化的d波段中心和最负的氧化电位，表明其抗毒性和稳定性增强。该研究不仅为三维多孔纳米材料的合成提供了新的视角，而且突出了三金属纳米合金在催化方面的潜在应用价值。

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引用次数: 0

Surface dynamic reconstruction of Ni-based catalysts for electrooxidation reaction 镍基电氧化反应催化剂的表面动力学重构

IF 8.9 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2025-08-21 DOI: 10.1016/j.cclet.2025.111746

Cheng Wang , Li Zhou , Zhenghao Fei , Yanqing Wang , Yukou Du

Ni-based materials, widely recognized for their exceptional catalytic properties, experience structural transformations that profoundly influence their performance characteristics and operational stability. To deeply understand the reconstruction mechanism of Ni-based catalysts, this review systematically summarizes the advanced strategies tailoring the dynamic reconstruction process, including electrochemical activation, defect engineering, partial etching, ionic doping, and heterostructure construction. Furthermore, we discuss the implications of these surface transformations on catalytic activity, highlighting their role in optimizing reaction pathways and enhancing overall efficiency in various electrooxidation reactions, such as oxygen evolution reaction (OER), urea oxidation reaction (UOR), glycerol oxidation reaction (GOR), hydroxymethylfurfural oxidation reaction (HMFOR), and ammonia oxidation reaction (AOR). By summarizing recent research findings, this review aims to provide a systematical summary of how surface dynamics can be harnessed to improve the design of Ni-based catalysts for a variety of electrooxidation applications, paving the way for advancements in energy conversion and storage technologies.

镍基材料因其特殊的催化性能而被广泛认可，其结构转变深刻地影响了其性能特征和操作稳定性。为了深入了解镍基催化剂的重构机理，本文系统地总结了电化学活化、缺陷工程、局部刻蚀、离子掺杂和异质结构构建等适应动态重构过程的先进策略。此外，我们还讨论了这些表面转化对催化活性的影响，强调了它们在优化反应途径和提高各种电氧化反应(如析氧反应（OER）、尿素氧化反应（UOR）、甘油氧化反应（GOR）、羟甲基糠醛氧化反应（HMFOR）和氨氧化反应（AOR）中的总体效率方面的作用。通过总结最近的研究成果，本文旨在系统地总结如何利用表面动力学来改进用于各种电氧化应用的镍基催化剂的设计，为能量转换和存储技术的进步铺平道路。

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