Pub Date : 2025-10-24DOI: 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.
{"title":"Recent advances in machine learning-driven discovery of alloy electrocatalysts for hydrogen evolution reaction","authors":"Na Qin , Wenxin Guo , Fangxiu Li , Houfeng Zhang , Hong Liu , Chang Zhang , Lipiao Bao , Lei Liu , Muneerah Alomar , Siqi Zhao , Jian Zhang , Xing Lu","doi":"10.1016/j.cclet.2025.112021","DOIUrl":"10.1016/j.cclet.2025.112021","url":null,"abstract":"<div><div>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.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"37 3","pages":"Article 112021"},"PeriodicalIF":8.9,"publicationDate":"2025-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145735451","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}
Pub Date : 2025-10-24DOI: 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.
{"title":"Scalable and rapid liquid synthesis of PtNi electrocatalyst for hydrogen evolution reaction","authors":"Liming Li , Yanchang Liu , Peng Kang , Donghui Feng , Yuguang Zhang , Hangxing Ren , Jianrong Zeng , He Zhu , Qiang Li , Xiaoya Cui","doi":"10.1016/j.cclet.2025.112022","DOIUrl":"10.1016/j.cclet.2025.112022","url":null,"abstract":"<div><div>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/cm<sup>2</sup>, 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.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"37 2","pages":"Article 112022"},"PeriodicalIF":8.9,"publicationDate":"2025-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145622132","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}
Pub Date : 2025-10-22DOI: 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 %.
{"title":"Carbonylation of C(sp3)–H bonds with CO2: Facile synthesis of 2,4-quinolinediones and related luminescent materials","authors":"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","doi":"10.1016/j.cclet.2025.112003","DOIUrl":"10.1016/j.cclet.2025.112003","url":null,"abstract":"<div><div>A novel method for carbonylation of tertiary C(sp<sup>3</sup>)–H bonds in 2-aminophenyl-alkyl methanones with CO<sub>2</sub> 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 CO<sub>2</sub> 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 %.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"37 3","pages":"Article 112003"},"PeriodicalIF":8.9,"publicationDate":"2025-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145735368","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}
Pub Date : 2025-10-22DOI: 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。
{"title":"Monochromophore-tunable supramolecular fluorescence-phosphorescence dual light-harvesting NIR emission for multi-dimensional information encryption","authors":"Siwei Wang , Fanxu Zeng , Yuan Yan , Jinghai Liu , Wei-Lei Zhou , Yong Chen","doi":"10.1016/j.cclet.2025.112002","DOIUrl":"10.1016/j.cclet.2025.112002","url":null,"abstract":"<div><div>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 <strong>G</strong>/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, <em>y</em> = 0.31, 0.33) was realized. Utilizing this LP to promote the supramolecular full-color FPRET assembly of single fluorophore <strong>G</strong> 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.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"37 4","pages":"Article 112002"},"PeriodicalIF":8.9,"publicationDate":"2025-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145975308","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}
Pub Date : 2025-10-22DOI: 10.1016/j.cclet.2025.112018
Hongjin Xu , Jinghua Wu , Hui Wang , Huanfeng Jiang , Zhiqiang Ma
The α,β-butenolide moiety serves as a valuable electrophile in Michael additions and cycloadditions, enabling the direct and atom-economical construction of γ-butyrolactones—a unique structural motif prevalent in natural products. However, its susceptibility to aromatization limits its applications in complex natural products synthesis. Herein, we report the asymmetric synthesis of (–)-14‑epi-sinugyrosanolide A, a stereoisomer of the natural product sinugyrosanolide A, in which the aromatization of α,β-butenolide moiety was inhibited. A mild acid-promoted intramolecular [5 + 2] cycloaddition could rapidly assemble the synthetically challenging 5,5,7,6 core found in several Sinularia diterpenoids. The key cycloaddition precursor was prepared through an unconventional sequence involving an aldol reaction of dihydropyranone acetal derivatives and aldehyde, followed by ring-closing metathesis (RCM). This research not only accomplishes the asymmetric synthesis of (–)-14‑epi-sinugyrosanolide A, but also shows its potential for synthesizing other cembranoid and norcembranoid natural products. More importantly, it establishes an alternative approach toward synthesizing structurally complex molecules containing γ-butyrolactone moiety.
{"title":"Asymmetric total synthesis of (–)-14-epi-sinugyrosanolide A","authors":"Hongjin Xu , Jinghua Wu , Hui Wang , Huanfeng Jiang , Zhiqiang Ma","doi":"10.1016/j.cclet.2025.112018","DOIUrl":"10.1016/j.cclet.2025.112018","url":null,"abstract":"<div><div>The <em>α,β</em>-butenolide moiety serves as a valuable electrophile in Michael additions and cycloadditions, enabling the direct and atom-economical construction of <em>γ</em>-butyrolactones—a unique structural motif prevalent in natural products. However, its susceptibility to aromatization limits its applications in complex natural products synthesis. Herein, we report the asymmetric synthesis of (–)-14‑<em>epi</em>-sinugyrosanolide A, a stereoisomer of the natural product sinugyrosanolide A, in which the aromatization of <em>α,β</em>-butenolide moiety was inhibited. A mild acid-promoted intramolecular [5 + 2] cycloaddition could rapidly assemble the synthetically challenging 5,5,7,6 core found in several <em>Sinularia</em> diterpenoids. The key cycloaddition precursor was prepared through an unconventional sequence involving an aldol reaction of dihydropyranone acetal derivatives and aldehyde, followed by ring-closing metathesis (RCM). This research not only accomplishes the asymmetric synthesis of (–)-14‑<em>epi</em>-sinugyrosanolide A, but also shows its potential for synthesizing other cembranoid and norcembranoid natural products. More importantly, it establishes an alternative approach toward synthesizing structurally complex molecules containing <em>γ</em>-butyrolactone moiety.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"37 3","pages":"Article 112018"},"PeriodicalIF":8.9,"publicationDate":"2025-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145735369","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}
In 2024, the MOE Key Laboratory of Macromolecular Synthesis and Functionalization at Zhejiang University continued its impactful researches across five core areas. In controllable catalytic polymerization, organoboron catalysts were developed for CO₂ copolymerization and novel photoresist materials. Studies in microstructure and rheology elucidated universal deformation modes in graphene-based 2D membranes and improved graphene fiber properties through shear alignment engineering, defect control, and enhanced interlayer entanglement. For separating functional polymers, Janus membranes and channels were created for multiphase separation, liquid-phase molecular layer-by-layer deposition technique was developed to fabricate aromatic polyamide nanofilms, and the harmonic amide bond density was established as a valuable parameter for polyamide structural analysis. In biomedical functional polymers, a sustainable carboxyl-ester transesterification strategy was proposed for upcycling poly(ethylene terephthalate) (PET) waste into biodegradable plastics. Additionally, immunocompatible biomaterials were designed utilizing zwitterionic polypeptides and albumin-derived coatings, and Cu2+-phenolic nanoflower was designed to combat fungal infections by combining cuproptosis and cell wall digestion. Further, the researchers developed a gelatin-DOPA-knob/fibrinogen hydrogel to achieve rapid and robust hemostatic sealing, utilized a double-network polyelectrolyte-coated hydrogel for enhancing endothelialization of left atrial appendage (LAA) occluders, and the researchers also demonstrated that image-guided high-intensity focused ultrasound enables manipulation of shape-memory polymers. Finally, in the realm of photo-electro-magnetic functional polymers, precise control of through-space conjugation was shown to enhance organic luminescence. Topologically structured hydrogels were revealed to exhibit autonomous actuation. Also, solar-driven photothermal ion pumps were developed for selective lithium extraction from seawater, and high-performance non-solvated C60 single-crystal films were prepared via facile bar coating. Lastly, the researchers demonstrated outstanding dielectric properties of polyethylene (PE) lamellar single crystals. The relevant works are reviewed in this paper.
{"title":"Key progresses of MOE Key laboratory of macromolecular synthesis and functionalization in 2024","authors":"Kangyuan Xie, Tianxiang Fang, Qingli Zhu, Qingyang Xu, Boyu Peng, Guangpeng Wu, Chao Gao, Haocheng Yang, Liping Zhu, Hongqing Liang, Weipu Zhu, Peng Zhang, Qiao Jin, Zhengwei Mao, Kefeng Ren, Yang Zhu, Haoke Zhang, Ziliang Wu, Chao Zhang, Hanying Li","doi":"10.1016/j.cclet.2025.111990","DOIUrl":"10.1016/j.cclet.2025.111990","url":null,"abstract":"<div><div>In 2024, the MOE Key Laboratory of Macromolecular Synthesis and Functionalization at Zhejiang University continued its impactful researches across five core areas. In controllable catalytic polymerization, organoboron catalysts were developed for CO₂ copolymerization and novel photoresist materials. Studies in microstructure and rheology elucidated universal deformation modes in graphene-based 2D membranes and improved graphene fiber properties through shear alignment engineering, defect control, and enhanced interlayer entanglement. For separating functional polymers, Janus membranes and channels were created for multiphase separation, liquid-phase molecular layer-by-layer deposition technique was developed to fabricate aromatic polyamide nanofilms, and the harmonic amide bond density was established as a valuable parameter for polyamide structural analysis. In biomedical functional polymers, a sustainable carboxyl-ester transesterification strategy was proposed for upcycling poly(ethylene terephthalate) (PET) waste into biodegradable plastics. Additionally, immunocompatible biomaterials were designed utilizing zwitterionic polypeptides and albumin-derived coatings, and Cu<sup>2+</sup>-phenolic nanoflower was designed to combat fungal infections by combining cuproptosis and cell wall digestion. Further, the researchers developed a gelatin-DOPA-knob/fibrinogen hydrogel to achieve rapid and robust hemostatic sealing, utilized a double-network polyelectrolyte-coated hydrogel for enhancing endothelialization of left atrial appendage (LAA) occluders, and the researchers also demonstrated that image-guided high-intensity focused ultrasound enables manipulation of shape-memory polymers. Finally, in the realm of photo-electro-magnetic functional polymers, precise control of through-space conjugation was shown to enhance organic luminescence. Topologically structured hydrogels were revealed to exhibit autonomous actuation. Also, solar-driven photothermal ion pumps were developed for selective lithium extraction from seawater, and high-performance non-solvated C<sub>60</sub> single-crystal films were prepared <em>via</em> facile bar coating. Lastly, the researchers demonstrated outstanding dielectric properties of polyethylene (PE) lamellar single crystals. The relevant works are reviewed in this paper.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"37 2","pages":"Article 111990"},"PeriodicalIF":8.9,"publicationDate":"2025-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145622098","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}
Pub Date : 2025-10-21DOI: 10.1016/j.cclet.2025.111989
Yue Li , Qianyu Ding , Wansheng Liu , Yimeng Sun , Liyao Liu , Ye Zou , Yutao Cui , Jia Zhu , Chongan Di , Daoben Zhu
Cyclo[n]Thiophenes (CnTs) are a distinctive class of π-conjugated macrocyclic molecules that have attracted growing attention owing to their structural aesthetics and organic electronic characteristics. However, the development of CnTs has been largely impeded by inefficient synthetic route. In this work, we employ a bridge strategy using bipyridine as bridge to link two quaterthiophene units resulting in Φ-shaped bicyclosystem. This strain-retaining approach improves the synthesis efficiency of the macrocycles. Two new macrocyclic molecules, (4T-2hexyl-2Me)2-DPBP and (4T-2hexyl)2-DPBP, were successfully synthesized in total yield 17 % and 16 %, respectively. Single-crystal structure of (4T-2hexyl-2Me)2-DPBP reveals that the bipyridine bridge is orthogonally strapped by two quaterthiophene units. Notably, both compounds exhibit aggregation-induced emission enhancement (AIEE) behavior-an unprecedented feature among CnT-based macrocycles. Theoretical calculations reveal that this AIE phenomenon originates from the restriction of intramolecular motion (RIM) in the aggregated state, which suppresses the non-radiative decay channels. These results demonstrate a generalized strategy for the synthesis of functional π-conjugated macrocyclic molecules based fluorescent materials.
{"title":"Bipyridine-bridged Φ-shaped cyclo[8]thiophene[2]pyrrole: Synthesis and fluorescence properties","authors":"Yue Li , Qianyu Ding , Wansheng Liu , Yimeng Sun , Liyao Liu , Ye Zou , Yutao Cui , Jia Zhu , Chongan Di , Daoben Zhu","doi":"10.1016/j.cclet.2025.111989","DOIUrl":"10.1016/j.cclet.2025.111989","url":null,"abstract":"<div><div>Cyclo[<em>n</em>]Thiophenes (C<em>n</em>Ts) are a distinctive class of <em>π</em>-conjugated macrocyclic molecules that have attracted growing attention owing to their structural aesthetics and organic electronic characteristics. However, the development of C<em>n</em>Ts has been largely impeded by inefficient synthetic route. In this work, we employ a bridge strategy using bipyridine as bridge to link two quaterthiophene units resulting in Φ-shaped bicyclosystem. This strain-retaining approach improves the synthesis efficiency of the macrocycles. Two new macrocyclic molecules, (4T-2hexyl-2Me)<sub>2</sub>-DPBP and (4T-2hexyl)<sub>2</sub>-DPBP, were successfully synthesized in total yield 17 % and 16 %, respectively. Single-crystal structure of (4T-2hexyl-2Me)<sub>2</sub>-DPBP reveals that the bipyridine bridge is orthogonally strapped by two quaterthiophene units. Notably, both compounds exhibit aggregation-induced emission enhancement (AIEE) behavior-an unprecedented feature among C<em>n</em>T-based macrocycles. Theoretical calculations reveal that this AIE phenomenon originates from the restriction of intramolecular motion (RIM) in the aggregated state, which suppresses the non-radiative decay channels. These results demonstrate a generalized strategy for the synthesis of functional <em>π</em>-conjugated macrocyclic molecules based fluorescent materials.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"37 2","pages":"Article 111989"},"PeriodicalIF":8.9,"publicationDate":"2025-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145622096","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}
Shape memory polymers used in 4D printing only had one permanent shape after molding, which limited their applications in requiring multiple reconstructions and multifunctional shapes. Furthermore, the inherent stability of the triazine ring structure within cyanate ester (CE) crosslinked networks after molding posed significant challenges for both recycling, repairing, and degradation of resin. To address these obstacles, dynamic thiocyanate ester (TCE) bonds and photocurable group were incorporated into CE, obtaining the recyclable and 3D printable CE covalent adaptable networks (CANs), denoted as PTCE1.5. This material exhibits a Young's modulus of 810 MPa and a tensile strength of 50.8 MPa. Notably, damaged printed PTCE1.5 objects can be readily repaired through reprinting and interface rejoining by thermal treatment. Leveraging the solid-state plasticity, PTCE1.5 also demonstrated attractive shape memory ability and permanent shape reconfigurability, enabling its reconfigurable 4D printing. The printed PTCE1.5 hinges and a main body were assembled into a deployable and retractable satellite model, validating its potential application as a controllable component in the aerospace field. Moreover, printed PTCE1.5 can be fully degraded into thiol-modified intermediate products. Overall, this material not only enriches the application range of CE resin, but also provides a reliable approach to addressing environmental issue.
{"title":"4D printing of reprocessable thiocyanate covalent adaptable networks with reconfigurable shape memory ability","authors":"Ting Xu, Kexiang Chen, Zhiyuan He, Chuanzhen Zhang, Xiaoyu Li, Ziyan Zhang, Wenbo Fan, Zhishen Ge, Chenhui Cui, Yanfeng Zhang","doi":"10.1016/j.cclet.2025.111959","DOIUrl":"10.1016/j.cclet.2025.111959","url":null,"abstract":"<div><div>Shape memory polymers used in 4D printing only had one permanent shape after molding, which limited their applications in requiring multiple reconstructions and multifunctional shapes. Furthermore, the inherent stability of the triazine ring structure within cyanate ester (CE) crosslinked networks after molding posed significant challenges for both recycling, repairing, and degradation of resin. To address these obstacles, dynamic thiocyanate ester (TCE) bonds and photocurable group were incorporated into CE, obtaining the recyclable and 3D printable CE covalent adaptable networks (CANs), denoted as PTCE1.5. This material exhibits a Young's modulus of 810 MPa and a tensile strength of 50.8 MPa. Notably, damaged printed PTCE1.5 objects can be readily repaired through reprinting and interface rejoining by thermal treatment. Leveraging the solid-state plasticity, PTCE1.5 also demonstrated attractive shape memory ability and permanent shape reconfigurability, enabling its reconfigurable 4D printing. The printed PTCE1.5 hinges and a main body were assembled into a deployable and retractable satellite model, validating its potential application as a controllable component in the aerospace field. Moreover, printed PTCE1.5 can be fully degraded into thiol-modified intermediate products. Overall, this material not only enriches the application range of CE resin, but also provides a reliable approach to addressing environmental issue.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"37 2","pages":"Article 111959"},"PeriodicalIF":8.9,"publicationDate":"2025-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145622058","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}
Pub Date : 2025-10-15DOI: 10.1016/j.cclet.2025.111960
Yuheng Wen , Zeyu Wang , Jingli Li , Chengyao Xue , Haobo Wang , Xingrui Li , Hao Zhang , Yang Lu , Yu Zhang , Qing Hou , Wenliang Song
The growing global demand for sustainable energy makes biodiesel an important renewable alternative to alleviate the energy crisis and reduce greenhouse gas emissions. Therefore, there is an urgent need to develop efficient, environmentally friendly and economically viable biodiesel production methods. Hypercrosslinked polymers (HCPs), as aromatic porous organic polymers, are solid frameworks that can be used as heterogeneous catalyst, and they are a promising platform for biodiesel catalytic conversion due to their low cost, highly accessible active site, tunable catalytic site types. In addition, innovative green synthesis strategies make environmentally begin production of HCPs possible. In recent years, HCPs has developed rapidly in the field of biomass catalysis. Unfortunately, to the best of our knowledge, there are no publications focusing on the green synthesis and application of HCPs-based materials for biodiesel production. This review provides an update on the synthesis and utilisation of green and efficient HCPs for catalytic biodiesel production. Initially, the green routes for HCPs synthesis are described, followed by a comprehensive summary of the various approaches to biodiesel production. The primary focus is on the utilisation of HCPs as carriers of active sites in the catalytic conversion of biodiesel, with particular emphasis on catalyst design, morphology control, and intelligent management in terms of application extension. Ultimately, thought-provoking recommendations are proposed to utilize improved green HCPs in combination with advanced production processes to achieve more efficient and sustainable development.
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