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Atomically dispersed Fe‑N4 sites on g‑C3N4 enable highly selective CO2‑to‑CO electrocatalysis g‑C3N4上原子分散的Fe‑N4位点实现了高选择性的CO2 - to - CO电催化
IF 8.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-11 DOI: 10.1016/j.cclet.2025.112096
Yongliang Ban , Meng Zhang , Jianya He , Chunfeng Shao , Zhongliao Wang , Wei Zhao , Kai Dai
The development of efficient and cost-effective non-precious-metal single-atom catalysts (SACs) is crucial for advancing the practical application of electrocatalytic CO2 reduction (CO2RR). However, identifying highly active metal atoms and designing catalysts with uniform active center structures remain significant challenges. To address this, we developed a generic pyrolysis method to synthesize a series of transition metal-based SACs with atomically dispersed metal anchored on carbon nitride support (M-C3N4, M = Fe, Ni, Cu). Benefiting from the unique electronic structure of the Fe-N4 sites supported on C3N4, the Fe-C3N4 catalyst demonstrated exceptional performance, achieving a CO Faradaic efficiency of 99.6 % and maintaining excellent stability. Theoretical calculations indicate that the Fe site exhibits a relatively stronger interaction with the *COOH intermediate, thereby helping to lower the energy barrier of the CO2 protonation process. This study provides valuable theoretical insights and practical synthesis strategies for designing high-performance non-precious-metal SACs for CO2RR.
开发高效、经济的非贵金属单原子催化剂对于推进电催化CO2还原(CO2RR)的实际应用至关重要。然而,鉴定高活性金属原子和设计具有均匀活性中心结构的催化剂仍然是一个重大挑战。为了解决这个问题,我们开发了一种通用的热解方法来合成一系列过渡金属基SACs,这些SACs将原子分散的金属锚定在氮化碳载体上(M- c3n4, M = Fe, Ni, Cu)。得益于C3N4上Fe-N4位独特的电子结构,Fe-C3N4催化剂表现出优异的性能,CO法拉第效率达到99.6 %,并保持了优异的稳定性。理论计算表明,Fe位点与*COOH中间体的相互作用相对较强,从而有助于降低CO2质子化过程的能垒。该研究为设计高性能的CO2RR非贵金属sac提供了有价值的理论见解和实用的合成策略。
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引用次数: 0
Rise of colloidal silver bismuth sulfide nanocrystals solar cells 胶体硫化银铋纳米晶太阳能电池的兴起
IF 8.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-04 DOI: 10.1016/j.cclet.2025.112054
Yongqiang Ji , Donglin Jia , Fan Xu , Zhengwei Li , Lin Zhang , Le Li , Hengwei Qiu
In recent years, AgBiS2 nanocrystals (NCs) have emerged as a research hotspot in the field of solar cells due to their excellent optoelectronic properties and environmentally friendly characteristics. Although the theoretical power conversion efficiency (PCE) of AgBiS2 NC solar cells can reach up to 26%, the current best device only achieved a PCE of 10.84%. Such an enormous efficiency gap is primarily caused by the complex surface defects, severe carrier recombination, and undesirable energy-level mismatches. Therefore, this review comprehensively summarizes recent advancements in AgBiS2 NCs, including their crystal structures, optoelectronic properties, synthesis methods, ligand engineering, and device optimization. By fine-tuning synthesis conditions (e.g., temperature, precursor ratios) and employing ligand exchange strategies (solid-state/liquid-state), significant improvements in material performance have been realized. Furthermore, device structure optimization (e.g., transport layer selection, interface modification) and energy-level alignment engineering have further enhanced efficiency. Despite decent stabilities of AgBiS2 NCs, several challenges such as large-area uniformity and long-term device durability remain unraveled, which may be the major obstacles for their further commercialization. Future advancements in defect control, the development of novel ligands, and encapsulation technologies are expected to expand the applications of AgBiS2 NCs in flexible electronics, aerospace, and wearable devices.
近年来,AgBiS2纳米晶体(NCs)因其优异的光电性能和环保特性成为太阳能电池领域的研究热点。虽然AgBiS2 NC太阳能电池的理论功率转换效率(PCE)可以达到26%,但目前最好的器件的PCE仅达到10.84%。这种巨大的效率差距主要是由复杂的表面缺陷、严重的载流子复合和不理想的能级不匹配造成的。因此,本文综述了AgBiS2纳米材料的晶体结构、光电性能、合成方法、配体工程和器件优化等方面的最新进展。通过微调合成条件(如温度、前驱体比例)和采用配体交换策略(固态/液态),实现了材料性能的显著改善。此外,器件结构优化(如传输层选择、接口修改)和能级对齐工程进一步提高了效率。尽管AgBiS2 NCs具有良好的稳定性,但诸如大面积均匀性和长期设备耐用性等几个挑战仍未解决,这可能是其进一步商业化的主要障碍。未来在缺陷控制、新型配体和封装技术方面的进步有望扩大AgBiS2 NCs在柔性电子、航空航天和可穿戴设备中的应用。
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引用次数: 0
Metal-organic framework materials for encapsulation, release and delivery of essential oils: Engineering strategies and challenges 用于精油封装、释放和输送的金属有机框架材料:工程策略和挑战
IF 8.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-01 DOI: 10.1016/j.cclet.2025.112049
Junfeng Huang , Hongxin Chen , Yan Liao , Xiaowen Zhang , Zengzhu Zhang , Xiaoyu Su , Zihong Xie , Biao Li , Baode Shen , Pengfei Yue
Essential oils (EOs) are widely present in aromatic plants and possess a wide range of significant pharmacological activities such as antibacterial, antioxidant and anti-tumor properties. They have broad application prospects in medical care, food, agriculture and other fields. However, their poor stability poses substantial challenges that significantly hinder their development and practical application. Metal-organic framework materials (MOFs), characterized by highly controllable structures, large specific surface areas, and stimuli-responsive release properties, have been extensively utilized in various fields such as drug delivery and food preservation. Due to their capacity to encapsulate and deliver EOs, MOFs have garnered considerable attention. In this review, we systematically summarize the structural features, types, and characteristics of MOFs, as well as the recent advancements in their application for controlled EO release. Furthermore, we focus on discussing engineering strategies aimed at enhancing the encapsulation, release, and delivery of EOs using MOFs. Finally, we briefly outline the existing challenges in the delivery of EOs using MOFs and present well-reasoned insights into prospective directions for future research.
精油广泛存在于芳香植物中,具有抗菌、抗氧化、抗肿瘤等药理活性。在医疗、食品、农业等领域有着广阔的应用前景。然而,它们的稳定性差带来了重大挑战,严重阻碍了它们的发展和实际应用。金属-有机骨架材料(MOFs)具有结构高度可控、比表面积大、刺激响应释放等特点,在药物递送、食品保鲜等领域得到了广泛的应用。由于它们封装和交付EOs的能力,mof已经引起了相当大的关注。本文系统地综述了MOFs的结构特点、类型和特点,以及其在可控EO释放中的应用进展。此外,我们将重点讨论旨在增强使用mof的EOs的封装、发布和交付的工程策略。最后,我们简要概述了使用mof提供EOs的现有挑战,并对未来研究的预期方向提出了合理的见解。
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引用次数: 0
Dovetail joint strategy for constructing giant multi-propeller supramolecular architectures 巨型多螺旋桨超分子结构的燕尾连接策略
IF 8.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-10-31 DOI: 10.1016/j.cclet.2025.112051
He Zhao , Qiangqiang Dong , Fengxue Liu , Ning Wang , Lijun Wang , Mingzhao Chen , Zhilong Jiang , Die Liu , Jun Wang , Pingshan Wang , Yiming Li
The structural principles of traditional Chinese mortise-and-tenon joints have inspired breakthroughs in supramolecular engineering. Nevertheless, substantial challenges remain in constructing nanoscale supramolecular architectures with precisely controlled giant dimensions. Herein, we report a precision-guided synthetic strategy for constructing giant 2D and 3D supramolecular architectures with rhomboidal motifs, which was achieved through a dovetail joint strategy. Initial assembly of bis-mortise ligand L1 with dovetail tenon ligand L2 in the presence of Cd2+ ions yielded the fundamental bis-rhombic supramolecule R1. Subsequent structural elaboration of the dovetail tenon motif enabled the development of multitopic ligands L3 and L4, which facilitated the construction of expanded architectures of the giant bis-propeller supramolecule R2 and tris-propeller supramolecule R3. The synthesized supramolecules R1–R3 were fully characterized multidimensional NMR spectroscopy, electrospray ionization mass spectrometry (ESI-MS), traveling wave ion mobility mass spectrometry (TWIM-MS), transmission electron microscopy (TEM), and atomic force microscopy (AFM). This work develops an innovative dovetail-joint assembly strategy for constructing rigid giant supramolecular architectures, establishing a new paradigm for precision engineering of complex 3D molecular systems.
中国传统榫卯连接的结构原理激发了超分子工程的突破。然而,构建具有精确控制的巨大尺寸的纳米级超分子结构仍然存在重大挑战。在此,我们报告了一种精确制导的合成策略,用于构建具有菱形基序的巨型二维和三维超分子结构,该策略通过燕尾连接策略实现。在Cd2+离子存在下,双榫配体L1与燕尾榫配体L2的初始组装产生了基本的双斜方超分子R1。随后对燕尾榫基序的结构细化使多主题配体L3和L4的发展成为可能,从而促进了巨型双螺旋桨超分子R2和三螺旋桨超分子R3的扩展结构的构建。对合成的超分子R1-R3进行了多维核磁共振谱、电喷雾电离质谱(ESI-MS)、行波离子迁移率质谱(TWIM-MS)、透射电子显微镜(TEM)和原子力显微镜(AFM)等表征。本工作开发了一种用于构建刚性巨型超分子结构的创新燕尾连接装配策略,为复杂3D分子系统的精密工程建立了新的范例。
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引用次数: 0
Lithium-bond chemistry enlightens 600 Wh/kg solid-state batteries 锂键化学启发600 Wh/kg固态电池
IF 8.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-10-30 DOI: 10.1016/j.cclet.2025.112045
Hong-Li Long, Hong-Jie Peng
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引用次数: 0
Rigid urea-based structures drive analysis of chiral amino acids 刚性脲基结构驱动手性氨基酸的分析
IF 8.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-10-30 DOI: 10.1016/j.cclet.2025.112039
Yanhui Zhong , Peisi Xie , Chengyi Xie , Lei Guo , Weiwei Chen , Shuyi Wang , Xiaoxiao Wang , Fuyue Wang , Zian Lin , Gongke Li , Zongwei Cai
Chiral amino acids (AAs) serve as essential building blocks of proteins and play vital physiological roles in living organisms. To achieve accurate, rapid, and high-throughput analysis of chiral AAs, this work proposed a methylbenzyl isocyanate (MBIC) derivatization strategy coupled with ultra-high performance liquid chromatography-mass spectrometry or trapped ion mobility spectrometry-mass spectrometry. The integration of a chiral carbon atom with a rigid urea-based structure can significantly enhance the separation of chiral MBIC-labeled AA enantiomers. This phenomenon can be attributed to the labeled l-AAs allow the carboxyl group to form intramolecular hydrogen bonds with the amino group in the rigid urea-based structure, whereas labeled d-AAs are unable to form such bonds. The method based on MBIC derivatization coupled with ultra-performance liquid chromatography-tandem mass spectrometry achieved simultaneous separation of 19 pairs of chiral AAs using only a C18 column within 30 min, enabling quantitatively detect twelve types of chiral AAs in the serum of healthy humans and Parkinson's patients. The distribution of twenty-four chiral AAs is observed in mouse brain using MBIC labeling-based matrix-assisted laser desorption/ionization-trapped ion mobility spectrometry-mass spectrometry imaging without prior separation. Our work elucidates the principles governing the separation of chiral AAs using derivatization methods, providing valuable guidance for the separation of chiral compounds.
手性氨基酸(AAs)作为蛋白质的基本组成部分,在生物体中起着重要的生理作用。为了实现准确、快速、高通量的手性原子吸收光谱分析,本研究提出了异氰酸甲酯(MBIC)衍生化策略与超高性能液相色谱-质谱或捕获离子迁移率谱-质谱联用。手性碳原子与刚性脲基结构的整合可以显著增强mbic标记的手性AA对映体的分离。这一现象可归因于标记的l- aa允许羧基与刚性脲基结构中的氨基形成分子内氢键,而标记的d- aa则不能形成这种键。基于MBIC衍生化-超高效液相色谱-串联质谱联用的方法在30 min内仅用C18色谱柱即可同时分离19对手性原子吸收剂,可定量检测健康人及帕金森病患者血清中的12种手性原子吸收剂。采用基于MBIC标记的基质辅助激光解吸/电离捕获离子迁移谱-质谱成像技术,在不预先分离的情况下,观察了24种手性原子吸收剂在小鼠脑内的分布。本研究阐明了衍生化方法分离手性原子吸收剂的原理,为手性化合物的分离提供了有价值的指导。
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引用次数: 0
Slow photons effect amplifying photo/photothermocatalytic solar fuel production 放大光/光热催化太阳能燃料生产的慢光子效应
IF 8.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-10-30 DOI: 10.1016/j.cclet.2025.112040
Yang Ding , Shuzeng Zhang , Zhixue Li , Guoxiang Yang , Runtian Zheng , Ning Han , Chunhua Wang
Transforming sunlight into renewable energy sources like hydrogen and methane through photocatalytic water splitting and the CO2 conversion presents a promising prospect to tackle energy scarcity and environmental pollution caused by burning fossil fuels. As the core of the photocatalytic technique, photocatalysts design is most significant for acquiring the desirable catalytic performance and target products. Photonic crystals, also denoted as inverse opals and three-dimensionally ordered macroporous materials (3DOM), have been extensively applied in photocatalytic fields due to their distinct advantages. Specifically, photonic crystal possesses slow photons effect, rich reactive sites, and well-interconnected inner channels. Among the above advantages, the slow photons effect contributes the most essential role for accelerating photocatalytic reaction. However, how to design materials with maximized slow photons effect upon specific wavelength illumination is still in the infancy. Although some reviews about 3DOM photocatalysts have been published, a critical review focusing on tunable slow photons effects for efficient photocatalysis is still lacking. In this review, we highlighted recent advances in slow photons effect in boosting solar energy conversion. Meanwhile, the relevant mechanism and fundamentals of the slow photons effect are discussed. Finally, we present our vision of the future developments and challenges in this exciting research field.
通过光催化水分解和二氧化碳转化,将太阳光转化为氢气和甲烷等可再生能源,为解决化石燃料燃烧造成的能源短缺和环境污染提供了广阔的前景。光催化剂作为光催化技术的核心,其设计对于获得理想的催化性能和目标产物至关重要。光子晶体也被称为逆蛋白石和三维有序大孔材料(3DOM),由于其独特的优点,在光催化领域得到了广泛的应用。具体来说,光子晶体具有慢光子效应、丰富的反应位、内部通道连通良好等特点。在上述优点中,慢光子效应对加速光催化反应起着最重要的作用。然而,如何设计在特定波长照明下使慢光子效应最大化的材料仍处于起步阶段。虽然已经发表了一些关于3DOM光催化剂的评论,但关于可调慢光子效应用于高效光催化的批评性评论仍然缺乏。本文综述了近年来慢光子效应在促进太阳能转化方面的研究进展。同时,讨论了慢光子效应的相关机理和基本原理。最后,我们对这一令人兴奋的研究领域的未来发展和挑战提出了展望。
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引用次数: 0
Ion-equilibrated OECT inverters for neural-compatible ring oscillators 用于神经兼容环振荡器的离子平衡OECT逆变器
IF 8.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-10-30 DOI: 10.1016/j.cclet.2025.112042
Xiangyuan Mei , Yu Xiao , Chaoyi Yan , Lingxuan Jia , Gang Song , Runjie Zhang , Weijie Wang , Fengting Lv , Xiaojuan Dai , Liyao Liu , Ye Zou , Shu Wang , Chong-an Di , Daoben Zhu , Fengjiao Zhang
Organic electrochemical transistor (OECT)-based inverters hold great promise for neural-machine interfaces due to their low operating voltage and compatibility with aqueous environments. However, unbalanced p-/n-channel characteristics hinder the inverter’s voltage gain and fast switching. Here, a rational inverter design is presented, leveraging ion concentration to equilibrate p-n channel conductivity and kinetic doping in the OECT inverter, achieving an extremely high gain value of over 370 V/V under optimized driving conditions. Furthermore, a 3-stage ring oscillator constructed from these ion-equilibrated OECT inverters exhibits a rapid response time (stage delay < 0.6 ms) and a broad frequency response exceeding 300 Hz, matching the mechanoreceptor signals in human skin. The biocompatible output displays a sublinear reaction to static pressure pulses, indicating successful tactile recognition in live neurons. This work presents a practical strategy for constructing neural-compatible artificial logics through ion-concentration engineering, providing a platform for seamless neural-machine integration.
基于有机电化学晶体管(OECT)的逆变器由于其低工作电压和与水环境的兼容性,在神经机器接口方面具有很大的前景。然而,不平衡的p /n通道特性阻碍了逆变器的电压增益和快速开关。本文提出了一种合理的逆变器设计,利用离子浓度平衡OECT逆变器中的p-n通道电导率和动力学掺杂,在优化的驱动条件下实现了370 V/V以上的极高增益值。此外,由这些离子平衡OECT逆变器构建的3级环形振荡器具有快速响应时间(级延迟<; 0.6 ms)和超过300 Hz的宽频率响应,与人体皮肤的机械感受器信号相匹配。生物相容性输出显示出对静压脉冲的亚线性反应,表明活神经元成功地进行了触觉识别。这项工作提出了一种通过离子浓度工程构建神经兼容人工逻辑的实用策略,为神经与机器的无缝集成提供了一个平台。
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引用次数: 0
Trapping extracellular vesicles from biofluids by hydrogels 用水凝胶捕获生物体液中的细胞外囊泡
IF 8.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-10-29 DOI: 10.1016/j.cclet.2025.112037
Yang Liu, Zi-Xi Wang, Fu-Gen Wu
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引用次数: 0
Recent advances in machine learning-driven discovery of alloy electrocatalysts for hydrogen evolution reaction 机器学习驱动下析氢反应合金电催化剂的新进展
IF 8.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-10-24 DOI: 10.1016/j.cclet.2025.112021
Na Qin , Wenxin Guo , Fangxiu Li , Houfeng Zhang , Hong Liu , Chang Zhang , Lipiao Bao , Lei Liu , Muneerah Alomar , Siqi Zhao , Jian Zhang , Xing Lu
The hydrogen evolution reaction (HER) is a pivotal process for clean energy conversion, yet the development of efficient and cost-effective electrocatalysts remains a major challenge. Alloy catalysts, with their tunable electronic properties and promising catalytic performance, have shown great potential for HER. However, the design of component types and ratios, along with structural optimization, has largely relied on traditional trial-and-error approaches, which are very complex and time-consuming. The rise of machine learning (ML) provides an efficient strategy for discovering and optimizing alloy catalysts by enabling rapid analysis of extensive experimental and simulation datasets. This review highlights the recent advances in applying ML techniques for the design and optimization of alloy electrocatalysts for HER, covering binary and multinary (ternary, quaternary and high-entropy alloys). In particular, by employing supervised learning and deep learning techniques, ML has achieved remarkable success in the rapid screening of alloy catalysts and in improving prediction accuracy. It also demonstrates the merit and capability of ML in accelerating this process. In the end, we discuss current challenges and future prospects for integrating ML into advanced HER catalysis, highlighting its potential to revolutionize catalyst development and promote sustainable hydrogen energy solutions.
析氢反应(HER)是清洁能源转化的关键过程,但开发高效、经济的电催化剂仍然是一个重大挑战。合金催化剂具有可调谐的电子特性和良好的催化性能,在HER中显示出巨大的潜力。然而,部件类型和比例的设计以及结构优化在很大程度上依赖于传统的试错方法,这种方法非常复杂且耗时。机器学习(ML)的兴起通过快速分析大量实验和模拟数据集,为发现和优化合金催化剂提供了一种有效的策略。本文综述了近年来应用ML技术设计和优化HER合金电催化剂的最新进展,包括二元和多元(三元、四元和高熵合金)。特别是,通过采用监督学习和深度学习技术,机器学习在合金催化剂的快速筛选和提高预测精度方面取得了显著的成功。这也证明了机器学习在加速这一过程中的优点和能力。最后,我们讨论了将ML整合到先进HER催化中的当前挑战和未来前景,强调了其在催化剂开发和促进可持续氢能解决方案方面的潜力。
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引用次数: 0
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Chinese Chemical Letters
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