Junqing Ye , Mengyuan Ren , Junfeng Qian , Xibao Li , Qun Chen
{"title":"Advances in graphene quantum dots-based photocatalysts for enhanced charge transfer in photocatalytic reactions","authors":"Junqing Ye , Mengyuan Ren , Junfeng Qian , Xibao Li , Qun Chen","doi":"10.1016/j.cclet.2025.110857","DOIUrl":"10.1016/j.cclet.2025.110857","url":null,"abstract":"<div><div>The development of efficient green energy technology is imperative in the face of energy crises and environmental concerns. Photocatalysis, which utilizes solar energy for processes such as carbon dioxide (CO<sub>2</sub>) reduction, organic pollutants degradation, and hydrogen (H<sub>2</sub>) production through water splitting, is a promising approach. The key to high-efficiency photocatalysis lies in the design of superior photocatalysts. Graphene quantum dots (GQDs) have sparked significant interest in photocatalysis due to their exceptional up conversion photoluminescence (UCPL), strong light-capturing capability, and unique photoinduced charge transfer properties. However, their standalone use is limited by stability and activity. By integrating GQDs into composite photocatalysts, the separation of photogenerated electron-hole pairs is enhanced, boosting photocatalytic performance. This review provides the first overview and summary of the preparation methods of GQDs in photocatalysts, encompassing top-down and bottom-up strategy. Subsequently, a pioneering detailed summary was made on the applications of GQDs-semiconductor composites (metal organic frameworks, CdS, and bismuth-based oxides, <em>etc.</em>) in photocatalytic reactions such as CO<sub>2</sub> reduction, organic pollutant degradation, and H<sub>2</sub> generation. Furthermore, the corresponding representative examples and mechanisms are also elaborated and discussed respectively. Finally, the challenges and prospects for GQDs-based photocatalysts in the field of photocatalysis are proposed. This review provides inspiration and guidance for the development of efficient GQDs-based photocatalysts.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 9","pages":"Article 110857"},"PeriodicalIF":9.4,"publicationDate":"2025-01-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144569999","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}
Baoqi Wu , Rongzhi Tang , Zhi-Wei Li , Feng Lin , Zongyu Sun , Huanyu Xia , Lin Jiang , Yu Tan
{"title":"Selective encapsulation of azo compounds by tetracationic cyclophane in water and photo-controlled reversible release","authors":"Baoqi Wu , Rongzhi Tang , Zhi-Wei Li , Feng Lin , Zongyu Sun , Huanyu Xia , Lin Jiang , Yu Tan","doi":"10.1016/j.cclet.2025.110896","DOIUrl":"10.1016/j.cclet.2025.110896","url":null,"abstract":"<div><div>Many azo compounds and their intermediates are toxic and have been linked to various health issues, representing a growing global problem. Molecular engineering for selective encapsulation of azobenzene compounds is critical, given their significant use in smart materials and prevalence as environmental micropollutants released from the food and dye industries. However, the current host molecules catering to azobenzene compounds are mainly limited to cyclodextrins, pillar[<em>n</em>]arenes and cucurbit[<em>n</em>]urils, demonstrating a moderate affinity. This report describes that a novel 3,3′-bipyridinium-based cyclophane was capable of encapsulating anionic azobenzene compounds in water with high binding affinity and pH stability through electrostatic attraction-enhanced mechanism, surpassing the extensively reported supramolecular systems. 1D&2D NMR experiments, UV–vis spectrum, X-ray crystallography and computational modeling were carried out to understand the host-guest complexation. It's worth noting that the tetracationic cyclophane exhibited good selective and anti-interference encapsulation properties in binary, ternary and seawater systems. Furthermore, upon UV/white light irradiation, the reversible conversion between (<em>E</em>)-4,4′-azobisbenzoate and (<em>Z</em>)-4,4′-azobisbenzoate triggers the dissociation/recomplexation of the host-guest complex within 3 min. This reversible photo-switchable (<em>E</em>)-disodium 4,4′-azobisbenzoate-<strong>BPy-Box<sup>4+</sup></strong> supramolecular system holds promise for designing novel materials for extraction/release of azo compounds and other small smart materials.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 9","pages":"Article 110896"},"PeriodicalIF":9.4,"publicationDate":"2025-01-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144472012","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}
Zhongchao Zhou , Jian Song , Yinghao Xie , Yuqian Ma , Hong Hu , Hui Li , Lei Zhang , Charles H. Lawrie
{"title":"DFT calculation for organic semiconductor-based gas sensors: Sensing mechanism, dynamic response and sensing materials","authors":"Zhongchao Zhou , Jian Song , Yinghao Xie , Yuqian Ma , Hong Hu , Hui Li , Lei Zhang , Charles H. Lawrie","doi":"10.1016/j.cclet.2025.110906","DOIUrl":"10.1016/j.cclet.2025.110906","url":null,"abstract":"<div><div>Organic semiconductor materials have demonstrated extensive potential in the field of gas sensors due to the advantages including designable chemical structure, tunable physical and chemical properties. Through density functional theory (DFT) calculations, researchers can investigate gas sensing mechanisms, optimize, and predict the electronic structures and response characteristics of these materials, and thereby identify candidate materials with promising gas sensing applications for targeted design. This review concentrates on three primary applications of DFT technology in the realm of organic semiconductor-based gas sensors: (1) Investigating the sensing mechanisms by analyzing the interactions between gas molecules and sensing materials through DFT, (2) simulating the dynamic responses of gas molecules, which involves the behavior on the sensing interface using DFT combined with other computational methods to explore adsorption and diffusion processes, and (3) exploring and designing sensitive materials by employing DFT for screening and predicting chemical structures, thereby developing new sensing materials with exceptional performance. Furthermore, this review examines current research outcomes and anticipates the extensive application prospects of DFT technology in the domain of organic semiconductor-based gas sensors. These efforts are expected to provide valuable insights for further in-depth exploration of DFT applications in sensor technology, thereby fostering significant advancements and innovations in the field.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 6","pages":"Article 110906"},"PeriodicalIF":9.4,"publicationDate":"2025-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143704150","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}
Chao Chen , Wang Geng , Ke Li , Qiong Lei , Zhichao Jin , Xiuhai Gan
{"title":"Pyridazine: A privileged scaffold in the development of 21st-century pesticides","authors":"Chao Chen , Wang Geng , Ke Li , Qiong Lei , Zhichao Jin , Xiuhai Gan","doi":"10.1016/j.cclet.2025.110902","DOIUrl":"10.1016/j.cclet.2025.110902","url":null,"abstract":"<div><div>Pyridazine has garnered increasing attention as a privileged scaffold and bioisosterism in drug discovery due to its unique structural characteristics. It can serve as a hydrogen bond acceptor when interacting with receptors due to its two adjacent nitrogen atoms. Upon conversion to pyridazinone, it exhibits the ability to act as both a hydrogen bond acceptor and donor, showcasing its versatility. This inherent flexibility has prompted extensive research exploring its bioactivity in pesticides and pharmaceuticals. In order to promote the development of pyridazine-based pesticides, this review provides a comprehensive summary of advancements for pyridazine-based pesticides on herbicidal (36.9 %), insecticidal (26.2 %), antifungal and antibacterial (24.6 %), plant growth regulatory (10.8 %), and antiviral activities (1.5 %) from 2000 to 2024. It serves as an invaluable reference and source of inspiration for agricultural scientists conducting future research.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 8","pages":"Article 110902"},"PeriodicalIF":9.4,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144195759","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}
Chunshi He , Linqing Li , Yuanrong Sun , Xuefang Wang , Jie Ren , Jianbo Li
{"title":"Enhanced durability of a novel thiol-epoxy network thermosets with excellent hygrothermal and chemical resistance","authors":"Chunshi He , Linqing Li , Yuanrong Sun , Xuefang Wang , Jie Ren , Jianbo Li","doi":"10.1016/j.cclet.2025.110905","DOIUrl":"10.1016/j.cclet.2025.110905","url":null,"abstract":"<div><div>Epoxy resin is widely used in electronic packaging due to its exceptional performance, particularly the low-temperature curable thiol/epoxy system, which effectively minimizes thermal damage to sensitive electronic components. However, the majority of commercial thiol curing agents contain hydrolysable ester bonds and lack rigid structures, which induces most of thiol/epoxy systems still suffering from unsatisfactory heat resistance and hygrothermal resistance, significantly hindering their application in electronic packaging. In this study, we synthesized a tetrafunctional thiol compound, bis[3-(3-sulfanylpropyl)-4-(3-sulfanylpropoxy)phenyl]sulfone (TMBPS) with rigid and ester-free structures to replace traditional commercial thiol curing agents, pentaerythritol tetra(3-mercaptopropionate) (PETMP). Compared to the PETMP/epoxy system, the TMBPS/epoxy system exhibited superior comprehensive properties. The rigid structures of bisphenol S-type tetrathiol enhanced the heat resistance and mechanical properties of TMBPS/epoxy resin cured products, outperforming those of PETMP/epoxy resin cured products. Notably, the glass transition temperature of TMBPS/epoxy resin cured products was 74.2 °C which was 11.8 °C higher than that of PETMP cured products. Moreover, the ester-free structure in TMBPS contributed to its enhanced resistance to chemicals and hygrothermal conditions. After undergoing 1000 h of high-temperature and high-humidity aging, the tensile strength and adhesion strength of TMBPS-cured products were 73.33 MPa and 3.39 MPa, respectively exceeding 100% and 40% of their initial values, while PETMP-cured products exhibited a complete loss of both tensile strength and adhesion strength. This study provides a strategy for obtaining thermosetting polymers that can be cured at low temperatures and exhibit excellent comprehensive properties.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 6","pages":"Article 110905"},"PeriodicalIF":9.4,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143704151","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}
Ji-Jia Zhou , Li-Gao Liu , Zhen-Tao Zhang , Hao-Xuan Dong , Xin Lu , Zhou Xu , Xin-Qi Zhu , Bo Zhou , Long-Wu Ye
{"title":"Copper-catalyzed asymmetric cascade diyne cyclization/Meinwald rearrangement","authors":"Ji-Jia Zhou , Li-Gao Liu , Zhen-Tao Zhang , Hao-Xuan Dong , Xin Lu , Zhou Xu , Xin-Qi Zhu , Bo Zhou , Long-Wu Ye","doi":"10.1016/j.cclet.2025.110870","DOIUrl":"10.1016/j.cclet.2025.110870","url":null,"abstract":"<div><div>The Meinwald rearrangement has proven to be one of the most useful tools in organic synthesis. However, examples of asymmetric Meinwald rearrangements are quite scarce, and these reactions have so far been limited to the use of chiral Brønsted acids as catalysts. Here, we report a copper-catalyzed asymmetric cascade cyclization/Meinwald rearrangement reaction, allowing the practical and atom-economic synthesis of a range of chiral tricyclic pyrroles bearing a chiral oxa-quaternary carbon stereocenter in high yields and enantioselectivities. Thus, this protocol not only represents the first transition-metal-catalyzed enantioselective Meinwald rearrangement, but also constitutes the first example of asymmetric formal monocarbon insertion into C–O bond of ester. Moreover, theoretical calculations provide further evidence for this multiple cascade cyclization and elucidate the origin of enantioselectivity.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 9","pages":"Article 110870"},"PeriodicalIF":9.4,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144480601","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}
Hanghang Zhao , Wenbo Qi , Xin Tan , Xing Xu , Fengmin Song , Xianzhao Shao
{"title":"Metal single-atom catalysts derived from silicon-based materials for advanced oxidation applications","authors":"Hanghang Zhao , Wenbo Qi , Xin Tan , Xing Xu , Fengmin Song , Xianzhao Shao","doi":"10.1016/j.cclet.2025.110898","DOIUrl":"10.1016/j.cclet.2025.110898","url":null,"abstract":"<div><div>Enhancing the corrosion resistance of carriers within Fenton-like systems and inhibiting the migration and aggregation of single atoms in reaction environments are essential for maintaining both high activity and stability at catalytic sites, thus meeting fundamental requirements for practical application. The Fenton-like process of activating various strong oxidants by silicon-based single atom catalysts (SACs) prepared based on silicon-based materials (mesoporous silica, silicon-based minerals, and organosilicon materials) has unique advantages such as structural stability (especially important under strong oxidation conditions) and environmental protection. In this paper, the preparation strategies for the silicon-based SACs were assessed first, and the structural characteristics of various silicon-based SACs are systematically discussed, their application process and mechanism in Fenton-like process to achieve water purification are investigated, and the progress of Fenton-like process in density functional theory (DFT) of silicon-based derived single atom catalysts is summarized. In this paper, the preparation strategies and applications of silicon-based derived SACs are analyzed in depth, and their oxidation activities and pathways to different pollutants in water are reviewed. In addition, this paper also summarizes the device design and application of silicon-based derived SACs, and prospects the future development of silicon-based SACs in Fenton-like applications.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 6","pages":"Article 110898"},"PeriodicalIF":9.4,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143830257","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}
Kailu Guo , Jinzhi Jia , Huijiao Wang , Ziyu Hao , Yinjian Chen , Ke Shi , Haixia Wu , Cailing Xu
{"title":"Structural tuning and reconstruction of CeO2-coupled nickel selenides for robust water oxidation","authors":"Kailu Guo , Jinzhi Jia , Huijiao Wang , Ziyu Hao , Yinjian Chen , Ke Shi , Haixia Wu , Cailing Xu","doi":"10.1016/j.cclet.2025.110888","DOIUrl":"10.1016/j.cclet.2025.110888","url":null,"abstract":"<div><div>Heterogeneous catalysts have attracted wide attention due to their remarkable oxygen evolution reaction (OER) capabilities. Herein, a one-step strategy involving the coupling of Ni<sub>x</sub>Se<sub>y</sub> with CeO<sub>2</sub> is proposed to concurrently construct heterogeneous interfaces, adjust phase structure, and regulate electronic configuration, thereby enhancing OER performance. Thanks to the role of CeO<sub>2</sub> coupling in reducing the activation-energy and accelerating the reaction kinetics, the heterogeneous Ni<sub>x</sub>Se<sub>y</sub>/CeO<sub>2</sub> catalyst exhibits a low overpotential of 218 mV at 10 mA/cm<sup>2</sup> and long-term stability (>400 h) in 1.0 mol/L KOH for OER. Moreover, the post-OER characterization reveals that the Ni<sub>x</sub>Se<sub>y</sub> matrix is reconstructed into NiOOH, while the incorporated CeO<sub>2</sub> nanocrystals self-assemble into larger polycrystalline particles. Theoretical analysis further demonstrates that the optimized electronic states at NiOOH/CeO<sub>2</sub> interfaces can modulate intermediate chemisorption toward favorable OER kinetics. This study offers fresh perspectives on the synthesis and structure-activity relationship of CeO<sub>2</sub>-coupled electrocatalysts.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 8","pages":"Article 110888"},"PeriodicalIF":9.4,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144280289","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}
{"title":"Iron-catalyzed CH activation: A sustainable approach to efficient organic synthesis","authors":"Qiao Song , Xue Peng , Zhouyu Wang , Leyong Wang","doi":"10.1016/j.cclet.2025.110869","DOIUrl":"10.1016/j.cclet.2025.110869","url":null,"abstract":"","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 5","pages":"Article 110869"},"PeriodicalIF":9.4,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143550233","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}
Miaosen Yang , Junyang Ding , Zhiwei Wang , Jingwen Zhang , Zimo Peng , Xijun Liu
{"title":"NiMo-based alloy and its sulfides for energy-saving hydrogen production via sulfion oxidation assisted alkaline seawater splitting","authors":"Miaosen Yang , Junyang Ding , Zhiwei Wang , Jingwen Zhang , Zimo Peng , Xijun Liu","doi":"10.1016/j.cclet.2025.110861","DOIUrl":"10.1016/j.cclet.2025.110861","url":null,"abstract":"<div><div>Establishing an energy-saving and affordable hydrogen production route from infinite seawater presents a promising strategy for achieving carbon neutrality and low-carbon development. Compared with the kinetically sluggish oxygen evolution reaction (OER), the thermodynamically advantageous sulfion oxidation reaction (SOR) enables the S<sup>2-</sup> pollutants recovery while reducing the energy input of water electrolysis. Here, a nanoporous NiMo alloy ligament (np-NiMo) with AlNi<sub>3</sub>/Al<sub>5</sub>Mo heterostructure was prepared for hydrogen evolution reaction (HER, -0.134 V <em>versus</em> reversible hydrogen electrode (<em>vs</em>. RHE) at 50 mA/cm<sup>2</sup>), which needs an Al<sub>89</sub>Ni<sub>10</sub>Mo<sub>1</sub> as a precursor and dealloying operation. Further, the np-NiMo alloy was thermal-treated with S powder to generate Mo-doped NiS<sub>2</sub> (np-NiMo-S) for OER (1.544 V <em>vs.</em> RHE at 50 mA/cm<sup>2</sup>) and SOR (0.364 V <em>vs</em>. RHE at 50 mA/cm<sup>2</sup>), while still maintaining the nanostructuring advantages. Moreover, for a two-electrode electrolyzer system with np-NiMo cathode (1 M KOH + seawater) coupling np-NiMo-S anode (1 mol/L KOH + seawater + 1 mol/L Na<sub>2</sub>S), a remarkably ultra-low cell potential of 0.532 V is acquired at 50 mA/cm<sup>2</sup>, which is about 1.015 V below that of normal alkaline seawater splitting. The theory calculations confirmed that the AlNi<sub>3</sub>/Al<sub>5</sub>Mo heterostructure within np-NiMo promotes H<sub>2</sub>O dissociation for excellent HER, while the Mo-dopant of np-NiMo-S lowers energy barriers for the rate-determining step from *S<sub>4</sub> to *S<sub>8</sub>. This work develops two kinds of NiMo alloy with tremendous prominence for achieving energy-efficient hydrogen production from alkaline seawater and sulfur recycling from sulfion-rich sewage.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 9","pages":"Article 110861"},"PeriodicalIF":9.4,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144587495","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}