Chinese Chemical Letters最新文献

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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

Chinese Chemical Letters

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

Chinese Chemical Letters

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

Chinese Chemical Letters

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

Nanodelivery strategies modulating tumor stromal cells for reverting the immunosuppressive tumor microenvironment 纳米递送策略调节肿瘤基质细胞以恢复免疫抑制肿瘤微环境

IF 8.9 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2025-10-30 DOI: 10.1016/j.cclet.2025.112036

Jiayi Sun , Luyao Huang , Wenfeng Jia , Yitong Liu , Li Xiang , Xing Yang , Fan Tong , Xiaobo Wang , Huile Gao , Yi Zhang

In contrast to conventional cancer treatment modalities, cancer immunotherapy has increasingly emerged as one of the most promising therapeutic approaches for cancer, owing to its capacity to elicit long-lasting immune memory and its favorable safety profile. However, the immunosuppressive tumor microenvironment (ITME) significantly hinders its progression. While tumor stromal cells play a crucial role in the formation of the ITME, they also offer several potential targets for interventions aimed at reshaping this suppressive milieu. In clinical practice, the modulating of tumor stromal cells overcomes resistance mechanisms, exhibits broader therapeutic potential, and allows for more manageable toxicity profiles. Owing to the capacity of nanodrug delivery systems (nano-DDS) to facilitate accurate targeting and integrate multiple functions, a growing number of researchers are employing nano-DDS in the immunotherapy modulated to tumor stromal cells. This review begins by elucidating the roles played by different tumor stromal cells in the formation of the ITME. Subsequently, we provide the nanodelivery strategies modulating distinct tumor stromal cells. Finally, we propose the current challenges and discuss potential future development directions in this field.

与传统的癌症治疗方式相比，癌症免疫疗法已日益成为最有前途的癌症治疗方法之一，因为它能够引发持久的免疫记忆，并且具有良好的安全性。然而，免疫抑制肿瘤微环境（ITME）显著阻碍其进展。虽然肿瘤基质细胞在ITME的形成中起着至关重要的作用，但它们也为旨在重塑这种抑制环境的干预措施提供了几个潜在的靶点。在临床实践中，调节肿瘤基质细胞克服了耐药机制，显示出更广泛的治疗潜力，并允许更可控的毒性谱。由于纳米药物递送系统（nano-DDS）具有精确靶向和多种功能整合的能力，越来越多的研究人员将纳米药物递送系统应用于肿瘤基质细胞的免疫治疗。本文首先阐述了不同肿瘤基质细胞在ITME形成中的作用。随后，我们提供了调节不同肿瘤基质细胞的纳米递送策略。最后，我们提出了当前面临的挑战，并讨论了该领域未来可能的发展方向。

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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

Chinese Chemical Letters

Pub Date : 2025-10-29 DOI: 10.1016/j.cclet.2025.112037

Yang Liu, Zi-Xi Wang, Fu-Gen Wu

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

Chinese Chemical Letters

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

Scalable and rapid liquid synthesis of PtNi electrocatalyst for hydrogen evolution reaction 可伸缩、快速液相合成析氢反应用PtNi电催化剂

IF 8.9 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2025-10-24 DOI: 10.1016/j.cclet.2025.112022

Liming Li , Yanchang Liu , Peng Kang , Donghui Feng , Yuguang Zhang , Hangxing Ren , Jianrong Zeng , He Zhu , Qiang Li , Xiaoya Cui

Structural engineering of Pt-based nanoalloys is crucial for the rational design and manufacturing of high-performance and low-cost electrocatalysts for hydrogen evolution reaction (HER). Here, we reported PtNi nanoparticles with a refined size of 2.71 nm and regular strains loaded on carbon black, synthesized using the high-temperature liquid shock (HTLS) method. This approach offers significant advantages over conventional synthesis methods, including high scalability, rapid reaction rates, and precise control over the size and shape of nanocrystals. Importantly, the synthesized PtNi electrocatalysts demonstrate outstanding catalytic activity and long-term stability for HER, achieving low overpotentials of 19 and 203 mV at current densities of 10 and 1000 mA/cm², respectively. The superior performance can be attributed to the combination of a refined particle size, lattice strains, and synergistic effects between Pt and Ni. This rapid liquid-state synthesis demonstrated here holds great potential for scalable and industrial manufacturing of micro-/nano- catalysts.

pt基纳米合金的结构工程对于合理设计和制造高性能、低成本的析氢反应电催化剂至关重要。本文采用高温液体冲击（HTLS）法制备了尺寸为2.71 nm的PtNi纳米颗粒，并将其加载在炭黑上。与传统的合成方法相比，这种方法具有显著的优势，包括高可扩展性，快速的反应速率，以及对纳米晶体大小和形状的精确控制。重要的是，合成的PtNi电催化剂对HER表现出出色的催化活性和长期稳定性，在电流密度为10和1000 mA/cm2时分别实现了19和203 mV的低过电位。优异的性能可归因于精细粒度、晶格应变以及Pt和Ni之间的协同效应的结合。这种快速液相合成方法在微/纳米催化剂的规模化和工业化制造方面具有巨大的潜力。

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引用次数: 0

IFC - Editorial Board/ Publication info IFC -编辑委员会/出版信息

IF 8.9 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2025-10-23 DOI: 10.1016/S1001-8417(25)00940-4

引用次数: 0

Carbonylation of C(sp3)–H bonds with CO2: Facile synthesis of 2,4-quinolinediones and related luminescent materials C(sp3) -H键与CO2的羰基化：2,4-喹啉二酮及其发光材料的简易合成

IF 8.9 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2025-10-22 DOI: 10.1016/j.cclet.2025.112003

Xiu-Mei Xie , Hongyang Zhang , Shao-Xuan Gong , Hong-Xia Sun , Yu-Ting Liu , Xue-Ling Chen , Shuming Chen , Tian-Yu Gao , Wai-Yeung Wong , Zhen Zhang , Da-Gang Yu

A novel method for carbonylation of tertiary C(sp³)–H bonds in 2-aminophenyl-alkyl methanones with CO₂ has been developed, enabling the synthesis of 2,4-quinolinediones featuring quaternary carbon centres. Building on this approach, a promising iridium(III) complex involving carbon from CO₂ was designed and synthesized. This complex, exhibiting a high photoluminescent quantum yield, was successfully applied in organic light-emitting diodes (OLEDs), achieving a high maximum luminance up to 12,010 cd/m² and a maximum external quantum efficiency (EQE) of 13.95 %.

本文提出了用CO2羰基化2-氨基苯基烷基甲烷的叔碳(sp3) -H键，合成具有季碳中心的2,4-喹啉二酮的新方法。在这种方法的基础上，设计并合成了一种有前途的铱（III）配合物，该配合物涉及二氧化碳中的碳。该配合物具有较高的光致发光量子产率，成功地应用于有机发光二极管（oled）中，最大亮度高达12010 cd/m²，最大外量子效率（EQE）为13.95 %。

引用次数: 0

Monochromophore-tunable supramolecular fluorescence-phosphorescence dual light-harvesting NIR emission for multi-dimensional information encryption 用于多维信息加密的单色可调超分子荧光-磷光双捕光近红外发射

IF 8.9 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2025-10-22 DOI: 10.1016/j.cclet.2025.112002

Siwei Wang , Fanxu Zeng , Yuan Yan , Jinghai Liu , Wei-Lei Zhou , Yong Chen

Organic fluorescence-phosphorescence dual-emitting materials based on tunable single chromophores have attracted much attention for their broad application prospects in information technology, display media and other fields due to their high luminescence stability, simple preparation process and excellent reproducibility. Herein, we constructed a novel LP-activated fluorescence-phosphorescence dual-light-harvesting (FPRET) supramolecular assembly based on LP with orthogonal charges, the phosphorescent molecule G and the NIR dye NIB through a supramolecular non-covalent strategy. The energy transfer efficiency of fluorescence is 54.68 % when the molar ratio of G/LP to NIB is 10:1, while the energy transfer efficiency and antenna effect of phosphorescence are 48.75 % and 241.43 respectively when the molar ratio of G/LP to NIB is 50:1. In addition, by co-assembling with carbon dots (CDs) and adjusting the ratio of donor to acceptor components, the full-color spectral regulation including white light (CIE chromaticity coordinates x, y = 0.31, 0.33) was realized. Utilizing this LP to promote the supramolecular full-color FPRET assembly of single fluorophore G and showing the multi-level anti-counterfeiting of intelligent logic gates through pattern, time, and color editing, it provides a new insight and direction for the development of a new generation of high-performance optical functional materials.

基于可调单发色团的有机荧光-磷光双发射材料因其发光稳定性高、制备工艺简单、重现性好等优点，在信息技术、显示媒体等领域具有广阔的应用前景而备受关注。本文采用非共价超分子策略，构建了一种基于正交电荷LP、磷光分子G和近红外染料NIB的新型LP激活荧光-磷光双捕光（FPRET）超分子组装体。当G/LP与NIB的摩尔比为10:1时，荧光的能量转移效率为54.68 %，而当G/LP与NIB的摩尔比为50:1时，荧光的能量转移效率为48.75 %，天线效应为241.43。此外，通过与碳点（CDs）共组装和调节供体与受体组分的比例，实现了包括白光在内的全彩色光谱调节（CIE色度坐标x， y = 0.31,0.33）。利用该LP推进单荧光团G的超分子全彩FPRET组装，通过图案、时间、色彩编辑展现智能逻辑门的多层次防伪，为新一代高性能光学功能材料的开发提供了新的见解和方向。

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