CCS Chemistry最新文献_第8页

Synergistic Enhancement of Thermopower and Conductance in Single-Molecule Junctions via Inter-Channel Quantum Interference 通道间量子干涉对单分子结热电和电导的协同增强

IF 11.2 1区化学

CCS Chemistry Pub Date : 2026-06-26 DOI: 10.31635/ccschem.026.202607839

Chao Fang, Mingchen Liang, Zhouyi Yu, Di Shan Chooi, Dongdong Wang, Xuejun Dong, Ning Cao, Jia Shi, Hongliang Chen, Junyang Liu, Wenjing Hong

{"title":"Synergistic Enhancement of Thermopower and Conductance in Single-Molecule Junctions via Inter-Channel Quantum Interference","authors":"Chao Fang, Mingchen Liang, Zhouyi Yu, Di Shan Chooi, Dongdong Wang, Xuejun Dong, Ning Cao, Jia Shi, Hongliang Chen, Junyang Liu, Wenjing Hong","doi":"10.31635/ccschem.026.202607839","DOIUrl":"https://doi.org/10.31635/ccschem.026.202607839","url":null,"abstract":"Molecular thermoelectric devices provides a promising route for nanoscale energy harvesting. However, its potential is often limited by a fundamental trade-off, where improvements in thermopower are typically accompanied by a suppressed electrical conductance, or vice versa. Here, we demonstrate that inter-channel quantum interference (QI) in cyclophane-based single-molecule junctions with two conducting channels enables synergistic enhancement of both thermopower and electrical conductance. Tight-binding modeling shows that tuning the energy or phase difference between the two conducting channels can induce constructive or destructive quantum interference, leading to a pronounced enhancement of both the transmission and its energy derivative within specific energy windows, thereby enabling synergistic increases in electrical conductance and the Seebeck coefficient. Measurements of single-molecule thermovoltage combined with current-voltage (I-V) analyses, using scanning tunneling microscope break-junction (STM-BJ) with a thermoelectric module, revealed that the two-channel molecular junction achieves an over two orders of magnitude enhancement of power factor compared to their single-channel counterparts, which confirms this hypothesis. This work establishes the inter-channel QI as a general molecular design principle to overcome the thermopower-conductance trade-off, which highlights the potential of macrocyclic and supramolecular architectures for realizing high-performance thermoelectric devices.","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"314 1","pages":""},"PeriodicalIF":11.2,"publicationDate":"2026-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148322876","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Non-thermal Plasma mediated Photocatalysis for Efficient Cascade Nitrogen Transformation to Oxime 非热等离子体介导的光催化高效级联氮转化为肟

IF 11.2 1区化学

CCS Chemistry Pub Date : 2026-06-26 DOI: 10.31635/ccschem.026.202607595

Lei Zou, Duan-hui Si, Shuai-long Yang, Zi-ao Chen, Yuan-biao Huang, Rong Cao

{"title":"Non-thermal Plasma mediated Photocatalysis for Efficient Cascade Nitrogen Transformation to Oxime","authors":"Lei Zou, Duan-hui Si, Shuai-long Yang, Zi-ao Chen, Yuan-biao Huang, Rong Cao","doi":"10.31635/ccschem.026.202607595","DOIUrl":"https://doi.org/10.31635/ccschem.026.202607595","url":null,"abstract":"Artificial nitrogen (N2) transformation is a crucial technology for modern industrialized societies. However, conventional methods for N2 transformation are highly energy-intensive and environmentally unsustainable. Herein, we developed a non-thermal plasma (NTP) mediated photocatalytic system for the cascade conversion of N2 into oxime. In this system, NTP facilitates the N2 activation, while photocatalysis realizes subsequent transformation of active N species into oxime through a C–N coupling process with an organic substrate. In-situ characterizations demonstrate that photo-reduced hydroxylamine from N2 is the key intermediate for the oxime production. Using lactic acid as a model substrate, it is first photo-oxidized to pyruvic acid, which then couples with hydroxylamine to form pyruvic oxime (PO). The representative cobalt-incorporated cadmium sulfide (CdS-Co) exhibits remarkably high PO productivity, achieving a maximum yield of 11.88 ± 0.51 mmol·g⁻1 within 2 hours, which is approximately twice that of pure CdS. This enhancement is attributed to efficient charge separation at the CdS-Co interface during photocatalysis, as confirmed by photoelectron kinetics measurements. This work proposes a new avenue for the conversion of inert gas molecules into value-added chemicals.","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"1 1","pages":""},"PeriodicalIF":11.2,"publicationDate":"2026-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148348834","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Construction of electron-donating bulwark in Methylene blue to overcoming biological reduction for improved photodynamic therapy 亚甲基蓝供电子壁垒的构建以克服生物还原改进光动力疗法

IF 11.2 1区化学

CCS Chemistry Pub Date : 2026-06-26 DOI: 10.31635/ccschem.026.202607598

Yingchao Chen, Tao Xiong, Yingnan Wu, Lei Wang, Mingle Li, Xiaoqiang Chen, Jiangli Fan, Xiaojun Peng

{"title":"Construction of electron-donating bulwark in Methylene blue to overcoming biological reduction for improved photodynamic therapy","authors":"Yingchao Chen, Tao Xiong, Yingnan Wu, Lei Wang, Mingle Li, Xiaoqiang Chen, Jiangli Fan, Xiaojun Peng","doi":"10.31635/ccschem.026.202607598","DOIUrl":"https://doi.org/10.31635/ccschem.026.202607598","url":null,"abstract":"Methylene blue (MB) is a promising photosensitizer for photodynamic therapy (PDT), yet its therapeutic efficacy is compromised by NAD(P)H-mediated reduction to leuco-MB, leading to suboptimal in vivo outcomes. To harness the phototherapeutic potential of MB, we developed an electron-donating bulwark strategy that circumvents biological reduction constraints, thereby substantially enhancing its reactive oxygen species (ROS) generation capacity. This anti-reduction property arises from augmented electron donation by molecular side chains, which mitigates electron deficiency of sulfur atom in MB and attenuates NAD(P)H-mediated reductive impact. Transient spectroscopy and electrochemical analysis revealed that electron-donating substituents decrease the reduction potential of MB, suppressing electron transfer between MB3⁺ and NADH while curbing ROS quenching in biological systems. Notably, bilateral ethyl-substituted MB-dEt demonstrated exceptional NADH resistance, producing ∼5.2-fold more ROS than MB under NADH exposure. Importantly, MB-dEt exhibited enhanced lipophilicity, enabling rapid cellular internalization within 10 minutes. Compared to MB, this minimally modified derivative showed a markedly reduced IC₅₀ for tumor cell cytotoxicity and achieved 90% tumor suppression in vivo. These findings establish a new paradigm for optimizing MB-based photosensitizers.","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"6 1","pages":""},"PeriodicalIF":11.2,"publicationDate":"2026-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148322611","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

OrgAIcat: Leveraging Literature Data for Enantioselectivity Prediction and Rapid Optimization in Organocatalysis 有机：利用文献数据对映体选择性预测和快速优化有机催化

IF 11.2 1区化学

CCS Chemistry Pub Date : 2026-06-26 DOI: 10.31635/ccschem.026.202607900

Qi Yang, Yidi Liu, Wenxuan Zhang, Long Zhang, Yufei Chen, Sanzhong Luo

{"title":"OrgAIcat: Leveraging Literature Data for Enantioselectivity Prediction and Rapid Optimization in Organocatalysis","authors":"Qi Yang, Yidi Liu, Wenxuan Zhang, Long Zhang, Yufei Chen, Sanzhong Luo","doi":"10.31635/ccschem.026.202607900","DOIUrl":"https://doi.org/10.31635/ccschem.026.202607900","url":null,"abstract":"Published reaction literature is heterogeneous and biased, yet it remains the largest practical record of asymmetric catalysis. Here we ask whether carefully curated literature data can nevertheless support useful enantioselectivity prediction in organocatalysis. We present OrgAIcat, a machine-learning workflow built on iSynth, a manually curated dataset of over 22,000 Aldol reactions and Michael additions collected from 844 publications. Using R-SPOC, a chemically informed reaction representation that combines catalyst, transformation, and condition descriptors without quantum-mechanical calculations, OrgAIcat achieves R2 values of 0.716 and 0.774 and mean absolute errors (MAE) of 0.282 and 0.265 kcal/mol for the Aldol reactions and Michael additions, respectively. External tests on recent literature and in-house reactions show that the model performs well in related organocatalytic systems. In a human-guided closed-loop workflow, OrgAIcat was used to prioritize catalysts for a challenging Aldol reaction, after which Bayesian optimization improved the enantiomeric excess (ee) from 41% to 96% in 12 experiments. These results indicate that curated literature data, despite their biases, can provide a practical basis for enantioselectivity prediction, catalyst prioritization, and rapid optimization in organocatalysis.","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"29 1","pages":""},"PeriodicalIF":11.2,"publicationDate":"2026-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148336022","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Degradation and Recycling of Polyamides via Nitrosation Strategy 聚酰胺的亚硝化降解与再循环

IF 11.2 1区化学

CCS Chemistry Pub Date : 2026-06-26 DOI: 10.31635/ccschem.026.202607643

Rehemuhali Hajiayi, Xinde Wang, Yichen Sun, Binzhi Zhao, Teng Wang, Ning Jiao

{"title":"Degradation and Recycling of Polyamides via Nitrosation Strategy","authors":"Rehemuhali Hajiayi, Xinde Wang, Yichen Sun, Binzhi Zhao, Teng Wang, Ning Jiao","doi":"10.31635/ccschem.026.202607643","DOIUrl":"https://doi.org/10.31635/ccschem.026.202607643","url":null,"abstract":"Polyamides are among the most widely produced engineering plastics (annual production >8 million tonnes) owing to their outstanding thermal and mechanical stability. However, their resistance to chemical degradation renders existing recycling strategies energy-intensive, typically requiring temperatures above 250 °C, elevated pressures, or noble-metal catalysts. Here we report a nitrosative depolymerization strategy that proceeds under mild conditions. Selective N–H nitrosation followed by backbone rearrangement disrupts hydrogen-bonding networks and cleaves otherwise inert amide linkages, enabling degradation of diverse nylons (e.g., nylon-6 and nylon-66) at 70 °C within 30 min, affording up to 61% yield of monomeric carboxylic acid derivatives. Substitution of sodium nitrite with tert-butyl nitrite (TBN) further enabled the direct one-step conversion of nylon-6 waste into 6-(nitrooxy)hexanoic acid, a key intermediate for the nitric oxide–donating prostaglandin analogue NCX-470, an intraocular-pressure-lowering agent. The method is applicable to commercial polyamide products, including gears, yarns, and cable ties. This work establishes a general platform for polyamide upcycling under mild conditions, expanding the scope of depolymerization beyond conventional acid- or base-driven approaches.","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"29 1","pages":""},"PeriodicalIF":11.2,"publicationDate":"2026-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148322875","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Heteroatom Engineering of Hemicyanine Chromophores Enables Tunable Imaging and Precision Photothermal Therapy for Bacterial Keratitis 半花青碱发色团的杂原子工程实现细菌性角膜炎的可调成像和精确光热治疗

IF 11.2 1区化学

CCS Chemistry Pub Date : 2026-06-22 DOI: 10.31635/ccschem.026.202507194

Di Fan, Jiawei Zhang, Jingjing Ye, Pengcheng Wang, Mengya Li, Haoliang Shi, Yufan Ling, Jian Yan, Houyu Wang

{"title":"Heteroatom Engineering of Hemicyanine Chromophores Enables Tunable Imaging and Precision Photothermal Therapy for Bacterial Keratitis","authors":"Di Fan, Jiawei Zhang, Jingjing Ye, Pengcheng Wang, Mengya Li, Haoliang Shi, Yufan Ling, Jian Yan, Houyu Wang","doi":"10.31635/ccschem.026.202507194","DOIUrl":"https://doi.org/10.31635/ccschem.026.202507194","url":null,"abstract":"Photothermal therapy offers a non-antibiotic strategy to eradicate drug-resistant bacterial keratitis, but its practical deployment is hindered by two intrinsic limitations: the low photothermal efficiency of organic small-molecule agents and the lack of spatially confined activation. Here we systematically modulated the bridging heteroatom (O, S, Se) within a hemicyanine scaffold to elucidate how spin–orbit coupling governs nonradiative relaxation and heat generation. Sulfur incorporation markedly enhanced internal conversion, yielding a 2.49-fold improvement in photothermal efficiency over the O-bridged analogue. Building on this optimized photothermal core, we introduced a β-lactamase (βla)–cleavable linker to construct enzyme-activatable probes (Pro-OCyOH and Pro-SCyOH). These probes remain quiescent in healthy ocular tissue but undergo rapid enzymatic cleavage in the presence of bacterial βla, releasing the active hemicyanine chromophore for site-specific fluorescence imaging and controlled photothermal ablation. In vitro and in vivo studies demonstrate that Pro-SCyOH achieves potent, spatially restricted eradication of multidrug-resistant pathogens while minimizing collateral corneal damage. This work defines a heteroatom-guided strategy to tune hemicyanine excited-state behavior and delivers an enzyme-activated small-molecule platform for precision therapy of drug-resistant bacterial keratitis.","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"436 1","pages":""},"PeriodicalIF":11.2,"publicationDate":"2026-06-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148322539","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Programmable Artificial K⁺-Cl− Cotransporters Harness K⁺ Flux to Drive Secondary Active Chloride Transport 可编程人工K + -Cl - Cotransporters利用K +通量驱动二次活性氯离子传输

IF 11.2 1区化学

CCS Chemistry Pub Date : 2026-06-22 DOI: 10.31635/ccschem.026.202607940

Xinxin Zhang, Mingju Luo, Jianru Wang, Wenju Chang, Jie Shen, Huaqiang Zeng

{"title":"Programmable Artificial K⁺-Cl− Cotransporters Harness K⁺ Flux to Drive Secondary Active Chloride Transport","authors":"Xinxin Zhang, Mingju Luo, Jianru Wang, Wenju Chang, Jie Shen, Huaqiang Zeng","doi":"10.31635/ccschem.026.202607940","DOIUrl":"https://doi.org/10.31635/ccschem.026.202607940","url":null,"abstract":"Natural K+-Cl− cotransporters (KCCs) are secondary active transporters that move Cl− against its transmembrane concentration gradient by harnessing the electrochemical gradient of K+. Faithfully replicating this secondary active transport function synthetically requires precisely balanced control of K+/Cl− ion selectivity. Here, we report a novel class of artificial K+-Cl− cotransporter (AKCC) system capable of such a secondary active transport, enabled by a dual-channel strategy that provides controllable bidirectional tuning of K+/Cl− selectivity within a single structural framework. The system features a modular, amino acid–derived H-bonded backbone that assembles into a one-dimensional array, positioning crown ether units on one side for K+ transport while hydrocarbon chains on the opposite side form anion-conducting pores. Independent variation of crown ether size and alkyl chain length enables fine control of transport properties, favoring K+ over Cl− without excessive selectivity and thereby allowing passive K+ flux to drive uphill Cl− transport in an unprecedented manner. The top-performing AKCC, <b xmlns:bkstg=\"http://www.atypon.com/backstage-ns\" xmlns:fn=\"http://www.w3.org/2005/xpath-functions\" xmlns:pxje=\"java:com.atypon.frontend.services.impl.PassportXslJavaExtentions\" xmlns:urlutil=\"java:com.atypon.literatum.customization.UrlUtil\" xmlns:xlink=\"http://www.w3.org/1999/xlink\">6F12, exhibits a balanced K+/Cl− selectivity ratio of 2.48 and enables robust K+-driven secondary active Cl− transport in a simulated cardiomyocyte environment. This work establishes a versatile design paradigm for controllable secondary active transport of Cl− anions, bridging a critical gap between biological inspiration and functional biomimetic materials.","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"2 1","pages":""},"PeriodicalIF":11.2,"publicationDate":"2026-06-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148322537","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Stabilizing Propylene Recognition via Molecular Clamps for Propylene/Propane Sieving under Challenging Conditions 在具有挑战性的条件下，通过分子钳稳定丙烯/丙烷筛分的丙烯识别

IF 11.2 1区化学

CCS Chemistry Pub Date : 2026-06-18 DOI: 10.31635/ccschem.026.202607512

Yanhui Dai, Yang Chen, Jiamin Zhang, Yongheng Ren, Lu Zhang, Libo Li, Jinping Li

{"title":"Stabilizing Propylene Recognition via Molecular Clamps for Propylene/Propane Sieving under Challenging Conditions","authors":"Yanhui Dai, Yang Chen, Jiamin Zhang, Yongheng Ren, Lu Zhang, Libo Li, Jinping Li","doi":"10.31635/ccschem.026.202607512","DOIUrl":"https://doi.org/10.31635/ccschem.026.202607512","url":null,"abstract":"Adsorptive separation of C3H6/C3H8 represents a low-energy alternative to cryogenic distillation; however, the performance of leading metal-organic frameworks (MOFs) declines sharply in dilute streams at elevated temperatures. This limitation mainly originates from their reliance on weak host-guest interactions and simple size-sieving mechanisms. Therefore, recovering and separating propylene under elevated temperature and low concentration conditions is a very difficult challenge. Here, a molecular clamp strategy is developed within a robust framework, TYUT-9, enabling specific and thermally stable recognition of C3H6. The molecular clamp creates a structure-defined binding pocket, where multiple cooperative C–H···N interactions stabilize C3H6 adsorption and preserve size-selective discrimination. Gas-loaded single-crystal X-ray diffraction and molecular modeling validated this mechanism, endowing TYUT-9 with exceptional adsorption performance at challenging conditions. The C3H6 capacity of TYUT-9 at 333 K and 0.05 bar reaches 32.8 cm3 g−1, retaining 92% of its 298 K capacity, which is more than twice that of benchmarks. Breakthrough experiments using equimolar C3H6/C3H8 mixture verify its superior separation performance, with breakthrough times 2–6 times longer than benchmarks at 333 K. In addition, TYUT-9 shows excellent chemical and cycling stability. These findings demonstrate that stabilizing C3H6 recognition via molecular clamps is effective for C3H6/C3H8 separation under elevated temperature and dilute conditions.","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"19 1","pages":"1-21"},"PeriodicalIF":11.2,"publicationDate":"2026-06-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148290053","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Helicene-Based Chiral Macrocycle: Efficient Synthesis, Spontaneous Chiral Resolution, and Strong Circularly Polarized Luminescence 螺旋烯基手性大环：高效合成、自发手性分辨和强圆偏振发光

IF 11.2 1区化学

CCS Chemistry Pub Date : 2026-04-28 DOI: 10.31635/ccschem.026.202607463

Peipei Liu, Meng-Ling Yu, Meng-Xiang Wu, Xiao-Li Zhao, Gui-Fei Huo, Xueliang Shi & Hai-Bo YangShanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai 200062

{"title":"Helicene-Based Chiral Macrocycle: Efficient Synthesis, Spontaneous Chiral Resolution, and Strong Circularly Polarized Luminescence","authors":"Peipei Liu, Meng-Ling Yu, Meng-Xiang Wu, Xiao-Li Zhao, Gui-Fei Huo, Xueliang Shi & Hai-Bo YangShanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai 200062","doi":"10.31635/ccschem.026.202607463","DOIUrl":"https://doi.org/10.31635/ccschem.026.202607463","url":null,"abstract":"CCS Chemistry, Ahead of Print. Herein, we report the synthesis of a novel helicene-based chiral macrocycle featuring distinctive conglomerate crystallization and markedly enhanced photophysical and chiroptical properties. Chiral macrocycle 1, consisting of three helicene moieties, is efficiently constructed via Yamamoto coupling of a newly synthesized dichloro-[5]helicene 2. Notably, 1 predominantly adopted the PPM/MMP conformation rather than the more stable PPP/MMM. The structures of both macrocycle 1 and its precursor helicene 2 were unambiguously confirmed by single-crystal X-ray diffraction (XRD). Interestingly, an unusual spontaneous chiral resolution phenomenon was observed upon crystallization of 1, resulting in enantiomerically pure chiral crystals of 1-PPM and 1-MMP. Compared with helicene 2, the absorption of macrocycle 1 was significantly redshifted, and its molar extinction coefficient (ε), as well as the fluorescence quantum efficiency (ΦF), were also remarkably enhanced. Notably, 1 exhibited a superior luminescent asymmetry factor (|glum| = 2.85 × 10−2) and a very high circularly polarized luminescence (CPL) brightness (Bcpl = 1514 M−1 cm−1), which represents one of the best CPL performances among chiral organic molecules. We believe this work provides valuable insights and new perspectives for exploring novel helicene-based macrocycles with multiple conformations, enhanced (chir)optical properties, as well as valuable electronic and optoelectronic applications.","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"28 1","pages":""},"PeriodicalIF":11.2,"publicationDate":"2026-04-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147755046","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Chiral Copper Clusters as Artificial Light-Harvesting Antennas Enabling Sequential Circularly Polarized Förster Resonance Energy Transfer 手性铜簇作为人工光收集天线实现顺序圆极化Förster共振能量转移

IF 11.2 1区化学

CCS Chemistry Pub Date : 2026-04-28 DOI: 10.31635/ccschem.026.202607344

Tian-Li Gao, Qi-Xiang Cai, Xiao-Jie Xu, Shuai-Peng Chen, Li-Zhen Wang, Ying-Xue Yuan, & Shuang-Quan ZangHenan Key Laboratory of Crystalline Molecular Functional Materials, College of Chemistry, Zhengzhou University, Zhengzhou, 450001, Henan Province

{"title":"Chiral Copper Clusters as Artificial Light-Harvesting Antennas Enabling Sequential Circularly Polarized Förster Resonance Energy Transfer","authors":"Tian-Li Gao, Qi-Xiang Cai, Xiao-Jie Xu, Shuai-Peng Chen, Li-Zhen Wang, Ying-Xue Yuan, & Shuang-Quan ZangHenan Key Laboratory of Crystalline Molecular Functional Materials, College of Chemistry, Zhengzhou University, Zhengzhou, 450001, Henan Province","doi":"10.31635/ccschem.026.202607344","DOIUrl":"https://doi.org/10.31635/ccschem.026.202607344","url":null,"abstract":"CCS Chemistry, Ahead of Print. The continuous transmission and amplification of chirality is a fascinating feature in natural biological systems. However, achieving sequential transmission of circularly polarized luminescence (CPL) through multistep energy transfer remains a formidable challenge. Here, chiral N-heterocyclic carbene-protected Cu3 clusters (R/S-Cu3) were synthesized as light-harvesting antennas, self-assembling into blue-emitting nanospheres with considerable CPL-active. Coumarin 6 (C-6), a green emitter, was introduced as the key relay baton for both chirality and energy transmission. We constructed chiral light-harvesting systems (LHSs) through the coassembly of R/S-Cu3, C-6, and red-emitting Nile Red (NiR), enabling efficient two-step energy transfer with a maximum efficiency (ΦET, max) of 87.86%. Supramolecular engineering was employed to fabricate nanofiber bundles serving as film templates, which facilitated sequential CPL transmission from Cu3 to C-6 and subsequently to NiR. The sequential circularly polarized Förster resonance energy transfer (CP-FRET) was verified via CPL spectral comparisons, resulting in distinct amplification of the dissymmetry factor. This work develops metal cluster-driven sequential CPL and energy transmission in chiral LHSs and provides in-depth insights into CP-FRET mechanism.","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"23 1","pages":""},"PeriodicalIF":11.2,"publicationDate":"2026-04-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147755047","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0